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Prog.EnergyCombust.Sci.Vol.22. pp.

267-306~1996

Pergamon

Copyright 1996ElsevierScienceLtd
Printedin Great Britain.All rightsreserved
0360-1285/96$29.00

PII: S0360-1285(96)00008-1

LASER-BASED TECHNIQUES FOR PARTICLE-SIZE MEASUREMENT:


A REVIEW OF SIZING METHODS A N D THEIR INDUSTRIAL
APPLICATIONS
David Lee Black,* Mardson Queiroz McQuay,t and Michel P. Bonin:~
*Department of Mechanical Engineering, Brigham Young University, 242 CB, Provo, Utah, 84602, U.S.A.
tDepartment of Mechanical Engineering, Brigham Young University, 242 CB, Provo, Utah 84602, U.S.A.
~Research and Development, lnsitec Measurement Systems, San Ramon. California, 94583, U.S.A.
Abstract--Laser-based techniques for particle-size measurement have become increasingly important in
combustion research and many other disciplines. Instruments are continually being developed and
improved to meet the demanding geometric, accuracy and other requirements associated with current
research and industrial applications. This paper reviews some of the many techniques now used, including
those marketed as commercial instruments and those ideas still in the research stage. Two distinct classes of
methods are identified: amplitude dependent and amplitude independent. The operating principles of
particle-size instrumentation using laser-based techniques, as well as difficulties associated with applying
these methods, are discussed. Applications of some techniques in research and industrial situations are also
reviewed. The paper provides a comprehensive review for those who are beginning studies in, or starting to
apply, any particle-sizing method based on laser illumination. Copyright 1996 Elsevier Science Ltd.
Keywords: particle, size, measurement, combustion, laser, applications, review.

CONTENTS
I. Introduction
1.1. Purpose and Description
1.2. Literature Overview
1.3. Importance of Particle-size Measurements
1.4. Extent of paper
1.4.1. Excluded techniques
1.4.2. Included techniques
2. Important Elements in Particle-size Measurement
2.1. Description of Particle Diameter and Shape
2.2. Particle Size Distribution Functions
2.3. The Gaussian Nature of Laser Beams
2.4. Spherical Versus Nonspherical Particles
2.5. Nonintrusive Versus Intrusive Methods
2.6. Other Optical Particle Sizing Concerns
2.6.1. Refractive index
2.6.2. Velocity measurements
2.6.3. Particle number density
2.6.4. Window access
3. Theories Used in Laser-based Particle Sizing
3.1. Lorenz-Mie
3.2. Generalized Lorenz-Mie
3.3. Fraunhofer Diffraction
3.4. Geometrical Optics
4. Single-Particle Counters (SPC)
4.1. Overview
4.2. Amplitude-dependent Methods
4.2.1. Absolute intensity
4.2.2. Intensity-ratio technique
4.2.3. Dual-beam sizing systems
4.2.4. Top-hat beam technique
4.3. Amplitude-independent Methods
4.3.1. Phase-Doppler analyzers
4.3,2. Projected grids
4.3.3. Displacement
4.3.4. Visibility
4.3.5. Miscellaneous particle analyzers
5. Ensemble Methods of Size Analysis
5.1. Fraunhofer Diffraction Based
5.2. Transmission Based
5.3. Comparisons Between Different Size Analyzers
267

268
268
269
270
270
271
272
273
273
275
276
276
277
277
278
278
279
279
280
280
281
281
282
283
283
283
284
285
286
287
288
288
291
292
292
294
296
296
297
298

268

D.L. Black et al.


6. Applications of Laser-Based Systems
6.1. Industrial Uses
6.1.1. Manufacturing processes
6.1.2. On-line process control
6.2. Research
7. Conclusions
Acknowledgements
References
NOMENCLATURE

Roman
b
d
dlo
d20
d21
d30
d31
d32
d43
dd
da
ds
dst
dF
dM
Dr
e
f
f(d)
fa
fd
F
I
I(0)
I0
I(s)
/max
Imin

JI
m
m'
n
N
N
r
R
R

Letters
measure of spread in particle sizes
equivalent spherical particle diameter
arithmetic mean diameter
surface mean diameter
surface diameter
volume mean diameter
volume diameter
Sauter mean diameter
weight mean diameter
drag diameter
projected area diameter
sieve diameter
Stokes' diameter
Feret's diameter
Martin's diameter
radial distance of the particle in the focal
plane from the optical axis
base of the natural log
focal length of the receiving lens
particle size distribution function
aniosotropic scatter frequency
LDA scatter frequency
function used in PDPA response to describe
system geometry
intensity of the scattered light
scattering intensity at a zero angle
laser beam intensity at a reference point
laser beam intensity at a distance s from a
reference point
maximum scatter intensity
minimum scatter intensity
first-order spherical Bessel function
refractive index of the particle
refractive index of the medium
characteristic of the particle material
relative refractive index (m/m')
number of particles in a sample
particle radius
percentage undersized
radial distance in focal plane
1. INTRODUCTION
1.1. Purpose and Description

Laser-based techniques for particle-size measurement are important in a variety of industries and to
researchers in many different fields. Examples include
combustion of pulverized coal and liquid fuels, spray
characterizations, analysis and control of particulate

299
299
300
300
301
301
301
301
s
distance along the path of the laser
S(d)
separation of refracted and reflected pulses
vp
particle velocity
vg
gas phase velocity
V
particle visibility
We
Weber number
x, y, z Cartesian coordinates
X
dimensionless radius used in Fraunhofer
diffrraction scattering
Greek letters
i5
fringe spacing of crossed LDV beams
0
half angle between the two cylindrical waves
00
beam convergence/divergence angle
Oi
incident angle
Ot
transmitted angle
~
optical thickness or opacity
laser wavelength
#
mean particle size
Ps
gas phase density
~r
standard deviation of size distribution
%
surface tension of a droplet
rR
refraction angle
rL
reflection angle

off axis angle of the receiver


~
phase difference between detectors
X
size parameter (dimensionless)
w
beam waist
Abbreviations
CFD
Computational Fluid Dynamics
DCW Dual Cylindrical Wave
DLS
Dynamic Light Scattering
EPCS Ensemble Particle Counter and Sizer
GLMT Generalized Lorenz-Mie Theory
GVG Grating Velocimeter-Granulometer
LDA Laser Doppler Anemometry
LDV Laser Doppler Velocimetry
Photon Correlation Spectroscopy
PCS
PDA
Phase Doppler Anemometry
PDPA Phase Doppler Particle Analyzer
PCSV Particle Counter Sizer Velocimeter
Polarization Intensity Ratio
PIR
SPC
Single Particle Counter
TESS Transform Extinction-Scattering
emissions, industrial process control, manufacture of
metallic powders and the production of pharmaceuticals. In response to different situations encountered
in sizing particles, many techniques have been and are
being proposed and developed to size particles
accurately. Often these techniques are capable of
measuring particle velocity as well. Use of the laser
has become increasingly popular in particle-sizing
applications. This has occurred because the laser's

Laser-based techniques for particle-size measurement


distinctive properties of nearly planar waves, monochromatic nature, coherence, and high spectral power
makes it an extremely useful tool for particle sizing.
This paper provides an introduction to a wide
range of topics related to areas of particle sizing that
use laser-based instrumentation. The text is oriented
toward those new to the field of optical particle sizing.
These would include students, industrial employees,
and others who are beginning studies in or needing
information on fields related to or involving particlesize analysis. With this in mind, the subject matter
of the paper assumes that the reader does not have
an extensive knowledge of light scattering and optics.
In addressing this audience, this review provides a
starting point for continued studies of various laserbased instruments commonly used for particle-size
analysis; it also introduces the reader to a large body
of related literature composed primarily of journal
articles.
The introduction provides an overview of literature
on particle-size analysis in general and articles that
review some of the techniques now in common use.
The specific techniques discussed in this paper are
also outlined in the introduction. Important issues
involved in the use of laser-based instruments for
particle-size analysis are then discussed in Section
2. These include definitions of particle size and
distribution functions, the Gaussian intensity of
TEM00 lasers, the issue of spherical vs. nonspherical
particles, particle velocity measurements, geometric
concerns relating to the instrumentation and the
optical access required by the instrumentation. This
section is followed by discussions of the various theories
important to laser-based, particle-size analysis. The
theories mentioned include Lorenz-Mie, generalized
Lorenz-Mie, Fraunhofer diffraction and geometrical
optics. Section 4 of the review describes various laserbased, single-particle counters, including those methods dependent on, or independent of, the amplitude of
the scattered signal. Section 5 discusses ensemble
methods of size analysis by which the particle size
distribution of a group of particles is determined
simultaneously. Section 6 is devoted to the application of laser-based particle-sizing methods in both
the industrial and research-and-development communities. General conclusions, including a brief
summary of the characteristics of instrumentation
reviewed in this paper, are presented in Section 7.
1.2. Literature Overview
Several texts discuss the significance of particle size
and the application of laser-based sizing systems,
specifically with an orientation toward combustion.
Instrumentation for Flows with Combustion, ~65 edited
by Taylor, is devoted to measurements in reacting
systems, including optical measurements of size and
velocity. Combustion Measurements, 34 edited by Chigier, addresses similar subjects related to measurements
in reaching flows. Atomization and Sprays, 116 by

269

Lefebvre, specifically focuses on spray formation,


description and combustion, including a discussion
of instruments suitable for spray measurements.
In addition to texts focused on combustion, other
texts provide an introduction to particle sizing in
general and discuss some of the laser-based techniques mentioned in this paper, as well as methods not
discussed in this review. These references provide
detailed discussions of distribution types, definitions
of particle size, sampling of powders and the theory of
classical optical and nonoptical particle measurement
techniques. These references include Particle Size
Measurement, by Allen, 5 Modern Methods o f Particle
Size Analysis, edited by Barth 18 and Particle Size
Analysis, by Jelinek. I8 A recent book by Washington, TM
written on an introductory level, presents essential
details of particle-size analysis and the instruments
available for this purpose. In addition to the texts
previously mentioned, other reference books discuss
the details of particle-size analysis. The two-part
series edited by Provder, 139'14 another edited by
Eddow 48'49 and one by Stockham and Fochtman 161
are compilations of papers by many different authors
on the basic elements of size analysis, distributions
and measuring techniques as used by people in a wide
variety of fields.
Several researchers have presented past reviews of
particle-sizing methods, most notably those of Azzopardi 7 in 1979, Hirleman 82 in 1980, Tayali and Bates 164
in 1990 and Barth and Sun 19 in 1993. Azzopardi 7
surveyed optical and nonoptical methods of size
measurement specifically suited to the measurement
of liquid drops. Hirleman 82 reviewed general laserbased sizing techniques under development or available
at that time, while Tayali and Bates ~64 compiled a
comprehensive review of both optical and nonoptical
methods of size analysis. This work describes the
operation of optical techniques that had been presented
in the literature, but does not mention any applications
of those methods in research or industry. Barth and
Sun 19 briefly review optical and nonoptical techniques
suitable for particle-size analysis. They also mention a
number of applications of these techniques, specifically those related to the field of chemistry. Another
excellent source of information on particle-size analysis
is the 20 November 1991 issue of Applied Optics. 84 This
issue is entirely devoted to subjects related to optical
particle sizing (some of the articles presented in the
1991 issue are referenced in this paper).
Several volumes of conference proceedings 36'6'16
contain many papers on aspects of particle sizing.
Many short reviews of particle-sizing techniques
have also appeared in the literature, such as those
by Houser, j4 Gouesbet, Maheu, and Gr~han 62 and
Dur~o and Heitor. 45 These are chapters or sections of
books and papers on larger subjects, such as spray
combustion or combustion measurements, devoted to
several specific methods of optical particle sizing.
These sections focus on using different sizing methods
in a particular area of application or research rather

270

D.L. Black et al.


Table 1. Applications of particle-sizing technology
Uses of particle-size analysis

Applications in area

Combustion
Sprays
Medicine/pharmaceuticals
Paints
Metallic powders
Agriculture
Pollution control
Foods and consumer products

Size and velocity measurements


Characterizations and descriptions of nozzles
Control of manufacturing processes
Control of pigment size distribution
Control of manufacturing processes
Control of pesticide application
Monitoring and analysis of emissions
Control of taste and texture

than on the development and evaluation of particlesizing instrumentation.


1.3. Importance o f Particle-size Measurements

Particle-size measurements are important to researchers, scientists and engineers in both the research-anddevelopment and industrial communities working in
a broad range of disciplines. Table 1 describes some
of the many fields in which particle-size analysis is
essential and lists some of the primary uses of particlesizing methods in these areas. For example, particle
size and number density are critical parameters in
two-phase combustion experiments and modelling,
since the particles or droplets represent the energy
source in reacting two-phase flows. Thus, knowledge
of the particle size distribution is a key parameter
in modelling radiative heat transfer, as well as in
characterizing other properties, such as droplet
evaporation rates and total droplet/particle burnout.
The particles and the associated heat release also have
a large impact on the flow field in the combustion
region. Smoot and Hill 154list particle dynamics as one
of nine critical areas in fundamental combustion
research and consider it one of the most critical areas
needing research. Holve et al) present an overview
of measurement techniques suitable for particle-size
measurements in fossil fuel systems and discuss the
requirements of optical sizing methods for application
in high temperature environments. Specific issues
discussed by the authors as they apply to sizing
systems suitable for use in reacting environments
include number density requirements, size range, shape
insensitivity, velocity and refractive index effects.
Chigier, 3s in Combustion Measurements, discusses
recent advances in particle-sizing instrumentation and
the importance of particle size and velocity measurements. Issues addressed in this book include the
interactions of particles with the flow field, measurements in large-scale combustion environments, and
detailed characterizations of single or groups of
reacting particles. In a recent paper, Bachalo l reviews
several techniques suitable for measurements in
multiphase flows. This paper specifically addresses
the measurement of the turbulence parameters in
two phase flows and discusses several types of
instrumentation suitable for work with these types
of environments. Bachalo II has also addressed the
topic of the combustion of liquid fuels and reviews

briefly the experimental work and measurement


developments applicable specifically to the subject of
droplet combustion.
Besides those involved in combustion, researchers
in areas such as meteorology, medicine TM and chemistry
apply and develop various methods of particle-size
measurement. Laboratory work with laser-based
sizing instrumentation includes work on the characterization of all types of two-phase flows, measurements of droplet size distributions in clouds, quality
control of injection fluids for medical use and studies
of respiratory illness caused by particle inhalation.
Laser-based methods of particle-size analysis are used
extensively in spray characterization and have
seen industrial applications in such diverse fields
as pulverized coal combustion, spray combustion,
powder metallurgy, pharmaceuticals manufacturing,
agriculture, powder and liquid paint production and
pollution monitoring. Techniques used by workers
in these fields are the same as, or similar to, those
that have found applications in areas of combustion
research. Since particle-size analysis is a broad topic,
it is necessary to consider work in fields other than
combustion to understand the techniques capable
of measuring particle size. Once the fundamental
principles of the various techniques are understood,
they can be applied to flows that require analysis
through particle size and concentration measurements.
Although optical techniques have been used
extensively to research numerous types of two-phase
flows, industrial applications of laser-based methods
have been limited to off-line, laboratory-based instruments that are typically based on the ensemble
diffraction technique. However, this is changing as
other laser-based sizing techniques are moved out of
the laboratory and integrated into the production
line. These new on-line techniques can provide realtime analysis of particle size and concentration,
enhancing process control and quality assurance of
the product stream. The large number of laser-based
systems, suitable for laboratory use, both in-situ and
off-line, as well as industrial, on-line instrumentation
provide many options for particle-size analysis in a
wide variety of environments.
1.4. Extent o f Paper

Figure 1 shows a diagram outlining several broad


methods of particle-size analysis, including those

Laser-based techniques for particle-size measurement

271

ill

I m'n l

I
SPC

I
Sieving
Sedimentation
lmpactors
Electrical

Photography
Microscopy
Holography
PIV

Absolute Intensity
Intensity Ratio

Diffraction

Dual Beam

PCS
Transmission

Visibility
Phase Doppler

DLS

DCW
Projected Grids
Shadow Doppler
Pulse Displacement
Polarization

Fig. 1. Various methods of particle-size analysis.


based on optical techniques and those mechanical in
nature. Many specific techniques are also listed under
their respective categories, although the list is not
all inclusive. Due to the large number of methods
available for sizing particles in many different fields,
the information in this paper has been restricted to
methods using laser light to determine particle size.
Because of the demanding nature of the environment
(high temperature and sometimes pressure), special
attention has been given to those methods that can
be applied to combustion systems to determine
the characteristics of the condensed phase before,
during, or after combustion. Instruments discussed
in this review include both commercially available
systems and research-type instrumentation. Commercial instruments are referred to by the manufacturer's
designation for the particular technique, where appropriate. This was done to show which types of
instruments are available commercially and which
must be constructed in the laboratory. By discussing
the instrumentation in this manner, no commercial
endorsement of any particular technique is intended.
The authors' intent is to inform the reader of
commercial instrumentation available for industrial
or research use and to describe the various strengths
and limitations of these instruments.
Because of the nature of the laser, it is particularly
useful for determining particle size information based
on properties of scattered light. Properties that
make the laser a useful tool include nearly planar
wave front, its monochromatic nature, coherence and
spectral power. Spectral power describes the intensity
per unit bandwidth or wavelength band of the laser.
For most lasers the range of wavelengths is small,
making the laser nearly monochromatic. This means
that large amounts of power can be concentrated in
narrow wavelength bands. For combustion systems

this property is particularly useful. Since combusting


flows typically have high light backgrounds, incorporating optical band pass filters in the collection
optics permits rejection of all but the laser wavelength, or the laser light scattered by the particle of
interest in the flow. Using this approach, measurements can be made in combustion environments
where broadband light sources would be useless. Due
to the above-mentioned properties, laser-based techniques are characterized by their own set of issues that
must be addressed, such as light scattering by single
or groups of particles, focused beam effects, sample
volume size and light-intensity profiles. These issues
and others, are discussed in Section 2 of this review.
Another constraint imposed on the information
presented in this paper is to discuss methods of analysis
suitable for sizing particles only in the submicron to
micron size range and above. Those techniques
suitable for sizing particles only in the submicron
region, such as Dynamic Light Scattering (DLS)
and Photon Correlation Spectroscopy (PCS), are
excluded. Emphasis on references discussed in this
paper is on articles published since Tayali and
Bates' review. 164 However, many earlier references
are included, especially for techniques that are now
commercially available or well established in their
reliability and applicability in various areas. References to earlier papers are limited primarily to those
that were instrumental in defining the various sizing
methods discussed in this work. More detailed reviews
of particle sizing and analysis done in the seventies
and early eighties can be found in past review articles,
such as those by Hirleman 82 and Tayali and Bates. 164

1.4.1. Excluded techniques


Methods not based on lasers, including sieving,

D.L. Black et al.

272

Table 2. Discussed methods of particle-size measurement


Amplitude dependent

Amplitude independent

Absolute intensity
Intensity ratio
Top-hat
Dual beam

Phase-Doppler
Projected grids
Pulse displacement
Visibility
Dual-cylindrical wave

and ensemble methods. Ensemble methods measure


the distribution of a group of particles, while SPC
systems size particles individually. SPC systems can
further be divided into two groups. The first group
consists of those techniques dependent on measuring
the amplitude of the scattered light. The second
consists of amplitude-independent methods in which
the size information is obtained from characteristics

Table 3. Summary of nonamplitude based instruments

USED
Industrial
Lab
Developmental
PARTICLE
Opaque
Transparent
Nonspherical
Reacting
FEATURES
Velocity
Accuracy
Size range
Concentration
Refractive
index
dependent

PhaseDoppler

DCW

Some
Yes
No

No
No
Yes

Yes
Yes
No
Yes
Yes
High
Large
High
Yes-trans.
No-opaque

Pulse
displacement

Projected
grids

Visibility

GVG

No
No
Yes

No
Yes
Yes

No
Yes
No

No
No
Yes

Yes
Yes
No
Yes

No
Yes
No
Yes

Yes
No
Yes
Yes

Yes
Yes
Yes
Yes

Yes
Yes
No
Yes

Yes
Unknown
Large
High
Yes

Yes
Moderate
Large
Moderate
Yes

Yes
Low
Moderate
Low
No

Yes
Moderate
Moderate
Low
No

Yes
Unknown
Small
High
Yes

sedimentation, impaction, photographic methods of


image analysis and methods using microscopes, have
been excluded from the material presented in this
review. Many of these methods are used extensively,
with developments and improvements continuing
to take place among these techniques, for example,
computer-controlled microscopy and high-speed photography. A large amount of literature published on
these methods discusses both their principles of
operation and experimental work done. Many
fundamental papers concerning these methods can
be found in the general review articles previously
mentioned.7,19,s2A64
The measurement techniques using white light as
an illumination source have also been excluded from
this paper due to the previously described problems
associated with broadband detection of a white light
source in a combustion environment. However, in
many applications, white light is a viable illumination
source that can be used in particle size and velocity
measurements. Researchers such as Sachweh 144 and
Hofeldt and Hanson 89 have proposed techniques using
white light. These methods, in many ways similar to
those using laser-light as an illumination source, are
outside the scope of this paper.
1.4.2. Included techniques
The sizing methods discussed in this paper fall into
two primary categories: single particle counters (SPC)

of the light-scattering signal besides its amplitude.


For example, phase-Doppler systems use the phase
difference between the light-scattering signals at
different spatial locations to calculate the particle
diameter. These methods depend on intensity only in
that the intensity of the scattered light must be large
enough to be properly measured. The specific sizing
methods considered in this paper are listed in Table 2.
Particle-sizing systems dependent on measuring the
amplitude of the scattered light discussed in this paper
include systems based on correlating particle size
directly to the measured amplitude of the lightscattering signal, the intensity-ratio approach and
methods using modified or multiple beams, such as
top-hat and dual-beam techniques. Other methods
are independent of the magnitude of the lightscattering signal. These include the phase-Doppler,
dual-cylindrical wave, pulse displacement techniques,
projected grids and the visibility method.
Tables 3 and 4 provide a subjective listing of the
various types of instrumentation discussed in this
paper. These tables attempt to rate the capabilities of
different techniques on the basis of where they are
typically used, what types of particle they can measure
and several specific features of interest of particlesizing systems. Instruments are classified according to
where they are used with the designations industrial,
laboratory and developmental. The term developmental is used to describe those instruments where
no significant work beyond the original, formulating

Laser-based techniques for particle-size measurement

273

Table 4. Summary of amplitude and ensemble based instruments

USED
Industrial
Lab
Developmental
PARTICLE
Opaque
Transparent
Nonspherical
Reacting
FEATURES
Velocity
Accuracy
Size range
Concentration
Refractive
index
dependent

Absolute
intensity

Intensity
ratio

Top-hat

Dual b e a m

Diffraction

Transmission

Yes

No
Yes
Yes

No
Yes
Yes

No
Yes
No

Yes
Yes
No

Yes
Yes
Yes

Yes

Yes
Yes
Yes
Yes

Yes
Yes
Yes
Yes

Yes
Yes
Yes
Yes

Yes
Yes
Yes
Yes

Yes
No
Yes
Yes

Yes
Moderate
Moderate
High
Yes

No
Moderate
Moderate
High
Yes

Yes
Moderate
Moderate
Moderate
Yes

Yes
Moderate
Moderate
Moderate
Yes

No
High
Large
High
No

No
Low
Large
High
No

Yes
Yes
'Yes
Yes
Yes

Table 5. Definitions of terms used in summary Tables 3 and 4

High
Low
Large
Small
Moderate

Accuracy

Size range (#m)

Concentration (#/cc)

better than 5%
less than 15%
NA
NA
5-15 %

NA
NA
0.5- I0 000
0.5-100
0.5-1000

greater than 106


less than 10 3
NA

research into the method, has been done. Features


listed include whether velocity measurements are
possible (although no distinction is made between
speed and velocity), the accuracy of the method, the
size range, concentration limits and refractive index
sensitivity. The meanings and approximate numerical
significance of the terms large, small, high, low and
moderate used in the summary tables are given in
Table 5 for the various categories in which they are
used. Since these summary tables are general in
classifying various types ,of instrumentation discussed
in this review, the features listed may not apply to
some specific types of instruments. The summaries are
intended to be general guidelines designated to point
readers in the direction of instrumentation that is
applicable to their specific circumstances. Table 3
lists information on nonamplitude-based techniques,
while Table 4 lists information on amplitude-based
and ensemble methods.

2. IMPORTANT ELEMENTS IN PARTICLE-SIZE


MEASUREMENT

Laser-based methods of particle-size analysis have


several common elements that must be addressed and
understood before a method can accurately be used
for particle-size analysis. A knowledge of particle-sizing
terminology and particle size distribution functions is
essential to understand the measurements from the

NA

103-106

Table 6. Particle shape terminology


Acicular
Angular
Crystalline
Dentritic
Fibrous
Flake-like
Granular
Irregular
Modular
Spherical

needle-shaped
sharp-edged
freely developed geometric shape
a branched crystalline shape
thread-like
plate-like
equidimensional irregular shape
lacking any symmetry
rounded, irregular shape
global in shape

various systems. Issues to resolve when applying


a technique include that of a Gaussian intensity
profile across the laser beam diameter, the scattering
characteristics of the particle, and the measurement
environment. Problems related to the Gaussian beam
profile must be resolved for all types of laser-based
systems. Some applications of laser diagnostics may
require the ability to make nonintrusive measurements in a flow field. This can lead to problems of
optical access to the flow, especially in high pressure
or temperature environments. These issues, among
others, are discussed in the following sections.

2.1. Description of Particle Diameter and Shape


A number of terms have specific meanings related
to the description of the shape and size of the
particles. Table 6 lists some of the more common

D. L. Black et al.

274

Table 7. Definitions of individual particle diameters


Symbol

Name

Definition

dd

Drag diameter

dst

Stoke's diameter

da

Projected area

dF

Feret's diameter

dM
ds

Martin's diameter
Sieve diameter

Diameter of a sphere with the same viscous drag as the


particle in the fluid with the same velocity
Diameter of a sphere of similar density having the same freefall velocity as the particle
Diameter of a circle having the same area as the projection of
the particle
The mean value of the distance between pairs of parallel
tangents to the projected outline of the particle
The mean chord length of the projected outline of the particle
The width of the minimum square aperture through which the
particle will pass

Table 8. Definitions and descriptions of mean particle diameters


Symbol

j.k.

Name

dl0

1,0

d20

2,0

d3o

3,0

d21

2,1

Arithmetic mean
diameter
Surfacemean
diameter
Volume mean
diameter
Surfacediameter

d31

3,1

Volume diameter

d32

3,2

d43

4,3

Sauter mean
diameter
Weight mean

Description
Normal average particle diameter of the size distribution
Diameter of a sphere with the average surface area of
the particles in the size distribution
Diameter of a sphere with the average volume of the
particles in the size distribution
Diameter of a sphere having the surface area of
the average particle size in the distribution
Diameter of a sphere having the volume of the average
particle size in the distribution
Diameter of a sphere with the equivalent surface to
volume ratio as all the particles in the size distribution
Diameter of a sphere having the average weight of all
the particles in the size distribution

terms related to aspects of particle shape, among with


their associated meanings.5 There are also many types
of particle diameters used to specify particle size. These
arise due to the variety of situations encountered by
those using particle-size measurement systems. For
different processes, different parameters of the size
distribution are important. For example, researchers
studying combustion phenomena are often concerned
with the volume and surface area of the particles since
this determines the area over which reactions can
occur and how long the particle will burn.
Most descriptions of the particle diameter involve
relating some aspect of the particle to a particle
having an equivalent spherical diameter. If the particle
under consideration is spherical, then all diameters
become equal. The wide variation in particle shape
leads to terms such as the volume diameter (where the
diameter is that of a sphere having the same volume as
the actual particle), the surface diameter (where the
diameter is that of a sphere having the same surface
area as the actual particle) and others, as defined in
Table 7. Each of these diameter definitions stems
from application of one or more methods of size
analysis. Diameter definitions, such as the projected
area diameter, Martin's diameter and Feret's diameter,
come from analyses using microscopy where these

diameters are easily measured. Others, such as the


drag diameter, come from sedimentation methods
of particle-size analysis. All laser-based methods of
particle sizing measure an equivalent spherical diameter.
However, the relationship between the actual particle
shape and the diameter measured is often complicated
and not as easily defined as it is for the nonoptical
techniques.
Laser-based particle analyzers generally determine
the distribution (discussed in detail in the following
section) of the equivalent spherical particle sizes. The
mean particle size of the distribution can then be
defined in different ways. Some of the most common
are the arithmetic mean (dlo), the surface mean (d20),
the volume mean (d30) and the Sauter mean (d~2).
Each mean diameter is defined to be the most useful
or convenient measure to use given the phenomena
under investigation. For example, d32 is used in
combustion related fields, d43 is used in the field of
chemical kinetics and d30 is common, since diffractionbased instrumentation typically report this parameter.
J(d~) is the value of the particle size distribution function
(discussed in detail in the following section) at the
discrete values of the particle size, represented by dr
in Eq. (1). The subscripts on the variables represent
the js and ks in the following expression used for the

Laser-based techniques for particle-sizemeasurement

275

Table 9. Common size distributions and their associated parameters


Distribution function

mean diameter

standard deviation

Normal
(d-ju)2
f ( d ) = -~2 exp[- - ~ - -

#=~S'

0.2

Log-normal
f(d) = J
41nd-lnu)"l
~2T~exp[21-Zi~----.J

#=X

if2

Rosin-Rammler
R = 100exp(-bd")
b
d
f(d)
n

1
l +
~ = zTgP(~

measureof the spread in the particle sizes.


particle diameter.
distribution function.
characteristicof the particle material.

= ~(dl-u)
N-I

1)

N number of samples.
R percentage undersized,
# mean of the distribution.
o- standard deviation of the distribution.

calculation of the various diameters:


dj f(di)
n

(djk)/-k -- ,.-,~d~ f ( d i ) "

'~(d,-u) 2

(1)

Table 8 summarizes the commonly used mean particle


diameters, the associated subscripts used in their
calculations and the physical meaning of the diameter
definition. The arithmetic mean is found from the
standard mathematical calculation of the mean particle
size, the area mean is the diameter of a particle having
the average area of the particles in the size distribution, the volume mean has a definition similar to that
of the area mean and the Sauter mean is the diameter
of a particle having the same mean surface area to
volume ratio as the sizes in the distribution.
2.2. Particle Size Distribution Functions
Particle size distribution functions are mathematical
expressions that relate some aspect of the particulates
in the flow, such as the volume or concentration, with
the particle diameter. These distributions functions,
given the symbol rid), are a simple mathematical
method of characterizing particulates without the need
for detailed plotting of the experimental distribution.
They allow communication of detailed information
about the particles in a concise manner. The use of
size distribution functions also provides a way to
extrapolate information about particle sizes outside
the measured range of values, makes calculation
of relevant information simple (such as the average
particle diameters and parameters describing the
distribution shape), and provides insight into the
processes involving the particles. 116
Distribution functions of particles and droplets can
be of several types, depending on the nature of the
particles and the environment in which they are used.
Some of the most common distribution functions
for powders and sprays are the normal, log-normal
and Rosin-Rammler distributions, The mathematical
formulas of the normal, log-normal and RosinRammler distributions along with the equations for
the mean and standard deviation for each distribution

are shown in Table 9. An excellent discussion of


these distributions and the calculations associated
with determining their statistics are given by Allen in
Particle-Size Measurement. s
The normal distribution is rare, usually applicable
only when the range of particle sizes is narrow. Most
distributions of powders in manufacturing processes,
pulverized coal, fly ash 58 and any powders produced
by grinding processes 174 fit a log-normal distribution.
The log-normal distribution is similar to the normal
distribution and is given by letting z = ln(d). Fine
powders and sprays can be described in terms of the
Rosin-Rammler distribution, written in terms of the
percentage undersized R; and the particle diameter d.
The variables b and n are a measure of the spread in the
particle size and a characteristic of the particle
material, respectively. For coarser sprays, the
Nukiyama-Tanasawa TM distribution function is
commonly used. Several additional distribution functions have been proposed to describe the distribution
shapes found in sprays, although these are less well
known than the Rosin-Rammler and NukiyamaTanasawa distribution functions. Details of the abovementioned functions as well as other formulations
can be found in texts by Lefebvre ~16 and Kuo. 113
In addition to having a distribution frequency with
size as described by the functions discussed above,
the distribution obtained from a particle-sizing
instrument can be further classified as temporal or
spatial. Temporal distributions result when particles
are sampled at a particular location in space over
some time period. Single Particle Counters (SPC)
return these types of measurements. Since they sample
a single particle at a time, the size distribution is
assembled from a series of scattering events occurring
over a defined time interval. The result is a distribution
that accounts for the velocity of the particles and is
representative of the actual particle-size distribution
in the flow. The particle velocity is important in
determining various statistics related to the flow field
being measured (such as concentration and turbulence information), since various size classes might
have differing velocities, as is the case for strongly
recirculating or high velocity flows.

276

D.L. Black et al.

Spatial distributions result from collecting scattering


information from a group of particles in a defined
sample volume at some instant in time, or in a way
that is independent of velocity. The distribution of
the entire group of particles in the sample volume is
then determined. Ensemble sizing systems measure
this type of distribution. If all the particles in a sample
are moving with the same velocity, then the two
types of distributions are the same. Otherwise, the
measured distribution is biased by the velocity of
the particles and does not represent the actual size
distribution in the flow. The difference in velocities
between the particle sizes cause the distribution to be
weighted toward the smaller particles as compared to
the temporal distribution, since more of the slow
moving particles will be measured.
To convert between the different types, the velocity
of the individual particles in the temporal distribution
must be known. By accounting for the differing
velocities of the particles in the temporal distribution
and assuming that all points in the region of interest
have the same temporal distribution, a temporal
distribution can be converted to a spatial one.
However, the reverse is generally not true. A spatial
distribution cannot be converted to a temporal
distribution unless the size resolved velocity information can be determined from the information contained
in the spatial measurement.

2.3. The Gaussian Nature of Laser Beams


One of the fundamental issues to address in sizing
particles using laser light is the Gaussian distribution
of light intensity across the diameter of the beam.
Lasers operated in the standard TEM00 mode are
characterized by a beam of Gaussian intensity profile
that produces a single spot of light when focused.
Detailed information on various lasers and their
modes of operation can be found in many books, such
as the text by Milonni and Eberly. 12 Particles in the
flow field generally pass through the beam, where
scattered light information is collected for particlesize analysis. Lock and Hovenac it7 describe the
scattering of light by a Gaussian beam and show
how the diffraction pattern from a single particle
varies across the diameter of the beam.
The problem the Gaussian beam creates for
particle-size measurement is that the light scattered
by a particular particle size passing through different
locations in the beam cross-section can scatter different
amounts of light. Thus a large particle passing through
the edge of the beam and a small particle passing
through the center of the beam can scatter the same
amount of light. This creates a dependence of particle
size on its trajectory through the sample volume.
The effect of trajectory must be accounted for by
instruments which rely on the measurement of the
scattering signal amplitude to determine particle size.
Various procedures have been proposed to account

for or eliminate this effect, such as the use of a top-hat


beam intensity profile, intensity deconvolution algorithms and nested beams.
The Gaussian distribution of intensity also creates
difficulties in defining the sample volume imaged by the
collection optics. At the radial edge of the sample
volume, large particles scatter detectable amounts of
light, while small particles are undetectable. This
effectively creates a different sample volume size for
different particle sizes. This problem, encountered by
all SPC systems, is usually removed by statistically
correcting the particle count distribution based on the
detectability of the scattered signal.

2.4. Spherical Versus Nonspherical Particles


Mathematical predictions of scattering intensity
used in particle-size measurement usually assume
spherical particles. A fundamental issue that determines the applicability of a sizing technique is its
sensitivity to particle shape. Some insensitivity to
particle shape can be achieved by using diffractive
scattering to determine particle size. By collecting the
signal in the near-forward direction, the sensitivity of
the signal to particle shape is minimized and particles
with aspect ratios up to two-to-one can be measured, ss
Diffracted light is collected in front of the particle
by a suitable collection system. For single particle
counters, small off-axis collection angles are also used
to limit the size of the sample volume, reducing
the problem of coincidence in particle flows of high
number densities, as discussed in detail in Section 4.
Orfanoudakis and Taylor m studied the effect of
particle shape on the optical parameters of collection
angle, lens aperture, and the diameter of the spatial
filter. Particles were represented by pulverized coal,
glass beads, and calibration pinholes. They quantitatively demonstrated that the response curves for the
particles studied approached those of the calibration
pinholes as the off-axis location of the receiver
decreased. The recommended off-axis collection
angle for minimum insensitivity to particle shape
was approximately 1.4. Umhauer and Bottlinger 166
have also analyzed the effect of particle shape and
structure on particle light-scattering patterns by
suspending a single particle in an electrical field.
They developed a method to mathematically correct
the loss in size distribution resolution due to irregularities in particle shape by analyzing the change in the
light-scattering patterns from a single particle in
different orientations. The method they developed is
applicable to particles having diameters between 15
and 100/zm.
Techniques using large detection angles to measure
light-scattering amplitude or other methods, such as
determining the phase shift between two signals from
the same particle, rely on the sphericity of the particles
and cannot measure nonspherical particles. Particular
details of the abilities of the various types of

Laser-based techniques for particle-size measurement


particle-sizing methods with respect to measuring
nonspherical particles are discussed in the section of
the paper corresponding to each particular method.

2.5 Nonintrusive versus Intrusive Methods


Many techniques, including current and past
methods, used for determining particle size are
intrusive in nature. Although the intrusive effects
can be minimized through probe miniaturization and
iso-kinetic sampling, an intrusive element in the flow
field remains that can cause unknown variations in
the flow field at, or downstream of, the sampling
point. Bonin 24 has demonstrated the potential impact
of intrusive sampling during a study of particle size
and velocity in an 80cm diameter, laboratory-scale
furnace using a laser-based probe. He first measured
gas-phase velocities with a hot film anemometer which,
due to its small size compared to the furnace, was not
expected to alter the velocity in the furnace as much as
the larger laser probe. He then measured the velocities
again with the hot wire anemometer installed in the
flow window of the 3.75 inch diameter cooling jacket
(the same size as the cooling jacket for the optical
system). His study showed that differences between
the two velocities ranged from 20 to 40%, depending
on location in the furnace. The experiments were
conducted under both swirling and nonswirling
conditions. Swirl was shown to increase the intrusive
effect of the large cooling jacket on the flow field.
Nonintrusive techniques are desirable in that no
probe must be inserted into the flow field to sample
the particles, eliminating potential problems of probeintrusion effects on the flow field. The nature of
the flow field can also be demanding, making the
insertion of optical probes difficult. For example, in a
reacting environment, the high temperatures make
cooling necessary, adding complexity to an already
intricate optical measurement system. Pressures above
atmospheric could further complicate inserting probes,
making the procedure potentially dangerous. In these
situations, nonintrusive instrumentation allows these
difficulties to be overcome.
Nonintrusive measurements are not without challenges. The application of these methods can be nearly
impossible or impractical. Examples include particle
measurements in large-scale systems such as utility
boilers, cross-diameter emissions monitoring in stacks,
and two-phase flow measurements in high pressure
facilities. For these applications, the physical dimensions and optical access may make nonintrusive
techniques impractical. For particle-size measurements
in large systems where the volume occupied by the
probe is insignificant relative to the size of the flow
chamber, probe insertion causes little disturbance and
they can be used without difficulty. In these situations,
probes offer a straightforward approach for assessing
the particle laden flow. This issue is illustrated by
the measurements taken by Bonin and Queiroz, 24'26

277

who used a laser-based probe in a laboratory-scale,


coal-fired furnace and on a large-scale utility boiler.
The flow field in the large-scale boiler was not
influenced by the presence of the probe, while the
same probe created large perturbations in the flow
field of the 80cm diameter laboratory furnace, as
discussed in the preceding paragraph.
Another possible difficulty encountered in applying
nonintrusive techniques lies in the need for optical
access to the measurement environment. Optical access
problems can range from straightforward for unenclosed geometries, to difficult in some enclosures, such
as high-pressure combustion chambers. Keeping the
windows clean in these situations can prove difficult.
This usually requires the addition of purge air, which
raises the possibility of undesired and unknown flow
perturbations in the measurement volume. Changes
in the optical configuration due to windows (as
discussed in Section 2.6.4.) must also be considered.
The effect of these issues on a laser-based measurement
system must be evaluated and if severe enough,
corrected for, to ensure accurate collection of particlesize information.
To summarize, problems involving access to the flow,
window interfaces, and the flow chamber geometry
must be successfully resolved in the implementation
of either method. Issues related to designing probes
with sensitive optical components to withstand high
temperatures, and corrosive and abrasive environments for the desired service life of the instrument,
must be resolved before probes can be successfully
used. Nonintrusive methods require optical access to
the particle-laden flow which may be difficult or
impractical to implement. Both techniques are widely
used, and instruments in both configurations have
been developed for application in a large variety of
situations.

2.6. Other Optical Particle Sizing Concerns


An issue that often becomes important when using
any of the instruments discussed in this paper is the
accuracy and consistency of the size measurement.
When applying a technique in a new situation, the
particle sizes, velocities and concentrations are often
unknown. In combusting flows, the particle type
itself can change, due to changes in the temperature
and chemical structure of the condensed phase. In
addition, the specific flow conditions near the
measurement location may change or be unknown.
To help overcome these difficulties, many instruments
have various types' of checks and redundancy measurements to assist in eliminating errors in the final result.
It is also important that the operator know how the
instrument behaves under different flow conditions
and understand the limitations and operation of the
particle analyzer. A few additional issues that are
often important when using laser-based techniques
are given in the following sections.

278

D.L. Black et al.

Beam
Laser

SpLtter

/f

X~,Co~r

Sig~
Processing

Jln/terference ~
(samplevolume)
Fringes
Fig. 2. General optical arrangement for generating interference fringes in a small sample volume using
crossed laser beams.
2.6.1. Refractive index

2.6.2. Velocity measurements

In addition to the problems arising from the Gaussian


nature of the laser beam, geometrical difficulties faced
in applying the optical configuration, and questions of
nonintrusive vs. intrusive measurements, the refractive
index of the particle or droplet measured is also a
concern. Most of the sizing techniques discussed in
this paper have some dependence on the particle's
refractive index. Roth, Anders and Frohn 143 address
the problem of an unknown refractive index or one
that varies with temperature such that the value is
not known. They incorporate a measurement of the
refractive index into the particle measurement by
determining the position of the first 'rainbow', which
is directly related to the refractive index of the
particle. The rainbow angle is the angle at which
the refracted and reflected rays combine to produce
a peak in the backscattered light. However, in many
environments, the change of the refractive index is
not great and the added complexity of determining
the refractive index in this way and incorporating
it into the measurement is not warranted. Bonin
and Queiroz 26 address the problem of the particle's
refractive index as it applies to the amplitude-based
sizing instruments described in Section 4.2.1. They
seek to minimize the effect of refractive index by
locating the collection optics in the near-forward
direction to collect primarily diffracted light, which is
independent of the particle refractive index. Zhang
and Xu 179 discuss the effect of varying refractive index
on systems dependent on the amplitude of the lightscattering signal. They calculated the effect of varying
the refractive index ofthe particle (m) between 1. I and
2.5 with 1.5 being the correct value. For the particle
sizes they considered, the effect of refractive index on
the Sauter mean diameter was generally less than 10%.

Detailed particle velocity information can be used


to characterize turbulence parameters, such as turbulent kinetic energy and Reynolds stresses, as well as
the correlations and cross-correlations between the
velocity and particle sizes. Velocity information can
also be used to determine boundary conditions for the
structure being analyzed for model validation. Since
SPC instruments are often used in-situ in a flow field,
knowledge of the particle velocity is particularly
important to determine the flow structure and particle
statistics. For example, information about particle
velocity is essential to determine the correct number
density or particle concentration.
Particle velocity information measured by the
sizing systems discussed here range from nonexistent
to detailed, particle-by-particle data, typical of that
measured using the LDA (Laser Doppler Anemometry)
technique. The essential optical configuration of the
LDA, shown in Fig. 2, is important for particle sizing,
since it is incorporated into several different sizing
systems to measure particle velocity. The optics are
characterized by two crossed laser beams which create
an interference pattern in the sample volume defined
by the lie 2 contour line. This line is defined by the
points where the illumination intensity falls to l/e 2
(13.5%) of the peak intensity. The particle velocity is
directly related to the frequency in the light-scattering
signal as the particle traverses the sample volume.
Velocity information is valuable only for those systems
designed for making particle-size measurements on a
research or industrial flow facility. For off-line systems,
such as laboratory bench top instrumentation, there
is little value in the velocity information, providing
it is properly incorporated in the size distribution
measurement.

Laser-based techniques for particle-size measurement


2.6.3. Particle number density
Particle number density, or concentration, is an
important parameter to determine for many two-phase
flow systems. This is particularly true for combustion
systems, since the condensed phase represents the
energy source. In addition to number density, mass
or volume flux measurements are often needed to
determine particle burning characteristics or to do a
mass balance on a system. When mass or volume flux
measurements are needed, careful attention must be
given to the accuracy of the number density of the
largest particles in the flow, as this is where most of
the volume is generally located.
The instruments discussed in this review generally
have some limitation on the maximum particle number
density that can be measured. This is primarily a
function of the sample volume size of the instrument,
SPC instruments usually have small sample volumes
so that high number density flows can be measured
without violating the single particle requirement of
the instrument. Typical sample volume cross-sections
(defined here as the cross-sectional area of the laser
beam in the sample volume perpendicular to the axis
of the beams) range from about 0.001 to 0.0001 cm 2,
which result in maximum measurable number
densities of 105-106 particles per cm 3. The drawback
of decreasing the size of the sample volume is that it
also decreases maximum measurable particle size,
specially for amplitude-based systems.
Basic ensemble methods are generally restricted to
extinctions in laser power of less than 50%, to avoid
complications due to multiple scattering effects. Each
scattering effect is defined to be the interaction of a
light ray with a particle. At extinctions above 50%,
there is a statistically significant possibility that a light
ray scattered by a particle will undergo secondary or
ternary interactions with additional particles before
reaching the detector. Therefore, the light-scattering
pattern is no longer a true representation of the sum
of the individual scattering events in the measurement
volume, since some collected rays will have effectively
been scattered more than once. Procedures have been
developed to correct for multiple scattering and are
incorporated into the signal processing for the various
diffraction-based instruments manufactured for size
analysis; these are discussed in more detail in Section
5 relative to the ensemble methods of particle-size
analysis.
In characterizing particle-laden flows, Bouguer's
law (or Beer's law as it is sometimes called), is often
useful as it describes the exponential decay in the
intensity of the laser as it travels along a path, due to
absorption and scattering by particles. A simple form
of Bouguer's law for a uniform medium can be
written as

1(s) = I~ e x p ( - ~ s )

(2)

where I(s) is the intensity of the laser beam a distance s


from the reference position and ~ is the optical opacity
JPECS 22:3-D

279

of the layer of thickness S. 153 The optical opacity can


be related to the overall concentration of particulates in the flow if the particle size distribution is
known.
2.6.4. Window access
The placement of windows in the path of the laser
beams in a particle sizing system can be a source of
potential measurement problems and errors. Windows
can change the alignment of laser-based systems so that
adjustment is needed whenever flow access windows
are used. For instruments where the scattered light
is collected in the forward direction, the need for
additional access for the receiving optics can create
more difficulties. The capability to monitor the optical
alignment of a laser-based particle sizing system is
essential in quantifying and resolving potential
difficulties related to windows used for optical access.
The windows that allow access to the particulates
is a significant factor in the design and application
of optical instrumentation. Nearly all types of laser
diagnostic instrumentation require a window interface,
integral to either an optical probe or an experimental
facility. Issues to resolve in designing an appropriate
window interface are the pathlength that can be
accommodated between the transmitter and collector
optics and the pathlength that can be tolerated
before light transmission through the particle flow
falls below an acceptable value. Long pathlengths
may require large lenses and focal lengths. These
optics can be expensive and their use requires large
windows in the flow chamber. In many systems, it is
not feasible to apply a nonintrusive instrument, since
the laser beam and or light-scattering signal cannot
pass through the flow field. The type and thickness of
the window must also be considered, with attention
to the necessary optical quality of the windows and
beam steering effects caused by the glass. Curved
or thick windows cause the most severe difficulties.
Curved windows make translation of nonintrusive
instrumentation difficult, because the curvature of the
window acts as an additional lens in the optical path.
Thick windows also cause problems because of their
potential effect on the focal lengths of the optics in
the system.
Another issue that must be resolved for laser-based
systems is the possibility of window fouling. For
amplitude-dependent systems, the magnitude of the
light-scattering signal, which depends on the intensity
of the illumination laser signal, determines the particle
size. Therefore, the absolute laser power reaching the
detector at the time of measurement must be
incorporated into the signal analysis. This is usually
done by ratioing the reference beam power level to
the measured level at the time of the measurement to
quantify the reduction in the light-scattering signal
from the particles. Nonamplitude-based methods
can also be influenced by window fouling due to the
possibility of beam interference from deposits on

280

D.L. Black et al.


R

Fig. 3. Diagram of the beam waist and divergence angle.

I0 -,t.

plane wav.~.
~.Top-hat
. / ~ ] J(",,,b,~,

L0 -~l

I. t

~010 -'~.
0

J-

I0 -l*.

beam

7i:

I~ Gausllian

beam

10 -is.
,

. . . . . .

10

Particle

100

diameter

0zm)

Fig. 4. Effect of beam shape on the collected intensity. Solid line: plane wave, stars: top-hat beam, dashed
line: Gaussian beam.59
the window where the laser beam passes through.
This could have a significant impact on the optical
configuration at the sample volume, disturbing the
measurement at that location. It is essential in systems
sensitive to the intensity of the illuminating laser to
use stable detectors and lasers. Instability from this
source could have a significant impact on the measured
results.
3. THEORIES USED IN LASER-BASED PARTICLE SIZING

Several theories are widely used as the basis for


laser-based instrumentation for particle-size analysis.
Theories discussed include Lorenz-Mie theory, generalized Lorenz-Mie theory, Fraunhofer diffraction
and geometrical optics. These theories characterize
the interaction of light with particles and provide a
physical basis and explanation for the operation of
the various methods of particle-size analysis. The
following sections describe these theories and their
applications with respect to particle sizing using
lasers.
3.1. L o r e n z - M i e

The classical theory relating particle scattering to


diameter is called Mie, or more properly Lorenz-Mie

theory. This theory is derived by solving Maxwell's


equations describing electromagnetic radiation for
the light scattered by a homogeneous sphere under
uniform illumination. Lorenz-Mie theory forms the
basis for the measurements of optical, particle-sizing
instruments based on measuring scattered light
intensity. Major assumptions involved in developing
the theory include plane light waves and spherical
particles. This theory was developed by several
individuals, primarily Lorenz and Mie. (The historical
development of Lorenz-Mie theory is briefly
discussed by Kerker. ll) Although computations
involving Lorenz-Mie theory are complex, several
codes are available for general use, including one listed
in the text by Borhen and Huffman. 28 Lorenz-Mie
theory incorporates the dimensionless size parameter
X as the fundamental parameter for light scattering
computations. The parameter X is defined as

x=

~rmd

(3)

where d is the particle diameter, )~ is the laser


wavelength and m is the refractive index of the
particle.
The mathematical formulation of Lorenz-Mie
theory is discussed extensively by van de Hulst, 16
Kerker, u and Borhen and Huffman. 2s Barber and
Hill 17 present computational algorithms and the source

Laser-based techniques for particle-size measurement


code for several scattering theories, including LorenzMie theory. Work is still being done on the theories
of electromagnetic scattering, a s Cho's 37 recent book
illustrates.
3.2. Generalized L o r e n z - M i e Theory
When the particle size is on the same order as
the beam cross-section at the sample volume, the
assumption of uniform illumination is no longer valid
and errors associated with particle size determination
using Lorenz-Mie theory will begin to increase. To
account for the effects of an arbitrary beam intensity
profile on the scattered light, recent improvements
have been incorporated into the original Lorenz-Mie
theory. This expanded theory, called the Generalized
Lorenz-Mie Theory (GLMT), was developed by
Gouesbet, Grrhan and Maheu. 6t'64 It accounts for an
arbitrary beam intensity profile, unlike the Lorenz-Mie
theory, which assumes plane light waves and uniform
illumination. A comprehensive recent summary of the
theory and the literature associated with it was
authored by Gouesbet. 59
The ability to account for a changing intensity
distribution across the laser beam is potentially
important, since many optical counters use laser
beams focused to small beam waists to preserve singleparticle scattering in high number-density flows. The
beam waist, ~, is defined as the diameter of the
focused beam, where the intensity falls to l/e 2 (13.5%)
of the peak intensity in the radial direction, where e is
the base of the natural logarithm. An illustration of a
focused laser beam showing the beam waist and the
convergence/divergence angle, 0o is shown in Fig. 3.
This figure illustrates the basic geometry around the
focal point of a typical laser beam used in particlesizing instrumentation. When the measured particles
begin to approach the diameter of the focused beam
waist, the assumption of plane waves is no longer
valid and the Lorenz-Mie theory cannot be applied
to describe the light-scattering phenomenon. This
effect of the plane wave assumption begins to manifest
itself when the particle is about 10% of the beam
waist and becomes steadily larger as the particle size
increases, as shown in Fig. 4. Figure 4 illustrates the
impact of the plane wave assumption on the scattered
light intensity as the particle size becomes large.
This graph shows the differences between the
scattering intensity from plane light waves (LorenzMie theory, solid lines), and a Gaussian profile
(GLMT, dashed line), as the particle diameter
approaches and then exceeds the 100#m waist
diameter of the beam. Points on Fig. 4 are values
of scattering intensity tbr a top-hat beam profile
discussed in Section 4.2.4.
Use of the more general theory, such as GLMT,
can potentially result in the measurement of larger
particles with a given beam waist or allow the beam
to be more tightly focused while still providing the
same measurement range possible with Lorenz-Mie

281

theory. The roll-off of the scattered light intensity


caused by the varying intensity profile of the beam
affects amplitude-based sizing systems most, however,
all laser-based instruments must account for the
effects of the varying intensity profile on the sample
volume of the instrument. GLMT has the potential to
account for the roll-off in the light scattered intensity
caused by the intensity distribution of the laser and
allow more accurate measurements of particle size
until the diameter is nearly equal to the beam waist.
The disadvantage of this approach is the time
consuming nature of the calculations using current
computer technology.
A number of publications present the mathematics
of GLMT, as well as experimental validation and
comparison of GLMT to the classical Lorenz-Mie
theory. Guilloteau, Grrhan and Gouesbet 67 compared
the near-forward scattering diagrams of optically
levitated 20 #m single particles with those calculated
using GLMT and Lorenz-Mie theory. They found
good agreement between GLMT and the experimental data for particles both smaller and somewhat
larger than the beam waist. They also showed significant
differences between results from GLMT and LorenzMie theory for particles larger than the beam waist.
Chevaillier et al. 33 also conducted a comparison
between Fraunhofer diffraction theory (discussed in
the following section), GLMT and experimental
results. They showed good agreement among the
three and concluded that diffraction theory was
accurate enough for scattering predictions in most
situations, although GLMT involved fewer assumptions. Another paper by Grrhan et al. 65 describes
the comparison between GLMT, classical LorenzMie theory and geometrical optics (described in
Section 3.4.) analysis of a simulated Dual Cylindrical
Wave (DCW) sizing system. This study indicates
good agreement between the DCW system and
GLMT. Geometrical optics and Lorenz-Mie theory
tend to be unreliable for large particles at small offaxis angles because a standard geometrical optics
analysis (as defined in Section 3.4.) neglects the
diffracted light component and the use of LorenzMie theory involves the assumption of plane light
waves.
3.3. Fraunhofer Diffraction
Fraunhofer diffraction theory represents the large
particle limit of the Lorenz-Mie theory for light
scattered in the near forward direction. The scattering
pattern produced by a single spherical particle consists
of a series of light and dark concentric bands that
decrease in intensity with increasing radial position.
The equation describing this distribution of intensity,
I, is called the Airy function and is given by

z(o)

(4)

where Ji is the first-order spherical Bessel function

282

D.L. Black et al.


I

0.8

0.6

0.4-

0.2"

A ~ ~ A A A A A A A A a A - - A A ~
0

0.00

2.00

~ ~

4.00

6.00

. . . . . . . .

8.00

10.00

Fig. 5. Fraunhofer diffraction intensity distribution with radial location.


Focal Plane
R
Fourier

Lens
I

Laser

t
~X

|l

Single Particle

Difl~efion t
Pa~rn

Fig. 6. Single particle diffracted light scattering pattern in the


focal plane of the receiving lens.
I(0) is the scattered intensity on the optical axis, and X
is a dimensionless parameter given by the following
expression, wherefis the focal length of the receiving
lens and R is the radial distance in the focal plane as
measured from the optical axis:
~rdR

X = -~7-.

(5)

A typical example of the intensity distribution as a


function of the dimensionless diameter ,V is shown in
Fig. 5. The diffraction pattern is independent of the
optical properties of the material and is a unique
function of particle size for a single particle, or the size
distribution for a group or ensemble of particles.
Information on the particle size distribution can be
found by measuring the scattered light intensity at
various radial locations to characterize the series of
annular rings from the particles' diffraction patterns
extending radially outward in the focal plane. Figure
6 illustrates this geometry and shows the shape of the
diffraction pattern generated by a single particle. In
particle sizing, usually only the location of the first

zero in the Bessel function for the desired range in


particle sizes needs to be characterized. This determines the geometry of instrumentation based on
diffraction theory by specifying the range of angles
that needs to be measured in the focal plane of the
receiving optics. Because only diffracted light is
considered, the particles can be thought of as a set
of opaque disks. In the case of very small particles,
or particles where the complex part of the index of
refraction is near zero, there is a possibility of significant
scattering due to the transmitted, or refracted, component of the laser light passing through the particle.
The particle complex index of refraction (m) consists
or a real part that describes the refracted light and
a complex part that describes the absorption. The
presence of transmitted light, known as anomalous
scattering and its effect on the diffraction pattern
are a function of the complex index of refraction
of the particle and the medium it is suspended in.
When anomalous scattering might have a significant
impact on the results, knowledge of the index of
refraction for the particle and the medium allow it
to be accounted for in measurements done using
Fraunhofer diffraction. Generally, this is a significant
issue only when sizing very small particles.
3.4. Geometrical Optics
Geometrical optics is the oldest theory of light
scattering useful for characterizing light interaction
with a sphere or other particles where the shape can be
specified. It is an approximation of the more exact
scattering theories, such as Lorenz-Mie. Essentially,
geometrical optics is a ray-tracing technique and can
be shown to be the large-particle limit of Lorenz-Mie
theory. Light waves are considered to be simple rays
of light and the laws of reflection and refraction are
applied to determine the behaviour of the light ray as

Laser-based techniques for particle-size measurement

283

l Reflected
,~0~/

OJ

DirectlyTransmitted
(Refracted,

Internal
Reflection
Fig. 7. Ray-tracing diagram for a single light ray interacting with a spherical particle.

it interacts with a spherical particle. The scattered


light is divided into reflected, transmitted (refracted)
and transmitted-after-internal-reflections components.
An example of a ray-trace diagram drawn using this
approach is shown in Fig. 7 for a single ray interacting
with a spherical particle. The possible outcomes of
a ray being reflected, transmitted (refracted) and
refracted after one internal reflection are shown,
along with the directions of the light ray leaving the
particle. The parameters Ot and Oi are related to the
relative refractive index N, defined as the refractive
index of the particle (m) divided by the refractive
index of the continuous phase (m'), by the following
expression

primary advantages in using geometrical optics is


its simplicity. This enables development and analysis
of instrumentation to be completed more easily
and simplifies the calculations needed to determine
particle size from the light-scattering information.
Geometrical optics is often used together with
Fraunhofer diffraction to provide a complete and
fairly simple representation of the reflected, refracted
and diffracted light scattered by a particle.

sin Ot = N.
sin Ot

Single-Particle Counters (SPC) are a broad classification of particle-sizing methods. These methods
typically incorporate small sample volumes into
the instrumentation to measure one particle at a
time. The sample volume size determines the largest
measurable particle size and number density of the
technique. Methods that fall in the SPC category can
be divided into two types: amplitude dependent and
amplitude independent.

(6)

Geometrical optics is the theory for light scattering


first presented in fundamental physics texts, such as
the text by Halliday and Resnick 68 and it is discussed
in more detail in advanced texts on light scattering,
such as Bohren and Huffman. 2s Unlike Lorenz-Mie
and GLMT, the technique is applicable to nonspherieal particles if the particle shape is known and can be
characterized in detail. The simplification implied in
the geometrical-optics approach work well, especially
for larger particles. Ungut, Grrhan and Gouesbet 168
compared calculations of classical Lorenz-Mie theory
with geometrical optics theory, Their calculations
show that geometrical optics is essentially as good as
the Lorenz-Mie theory when the particles are greater
than 10#m and when there is less than 5% deviation
from particle sphericity. Under these conditions, the
difference between rigorous Lorenz-Mie theory and
simplified geometrical optics is less than 10%. The

4. SINGLE-PARTICLECOUNTERS(SPC)

4.1. Overview

4.2. Amplitude-dependent Methods


Amplitude-dependent techniques measure the
absolute intensity of the light scattered by a particle
in the sample volume. All the techniques mentioned
here are SPC systems and are limited by the number
density of the flows that can be measured, usually on
the order of 105-107 particles per cm 3, as discussed in
Section 2.5. A major concern for methods using
this approach, as well as nonamplitude methods, is

284

D.L. Black et al.


Beam

Measurement Volume

Block

Fiber Optic Cable


to Signal Processor

Fiber Optic Coupler

Fig. 8. Light-scattering geometry employed by the PCSV instruments.

ambiguity in the measurements due to the particle's


trajectory through the Gaussian beam. This aspect of
particle sizing is discussed in Section 2.1. Researchers
have dealt with the problem of trajectory ambiguity in
a variety of ways, including methods such as intensity
deconvolution and co-incident trigger beams. Holve
and Self 94'95 and later, Holve and Davis, 97 have
developed a method for the analysis of the sample
volume characteristics for SPC systems to characterize the intensity distribution in the sample volume.
This theory mathematically describes the sample
volume intensity distribution as a function of particle
scattering properties and the geometric parameters
of the optical system. This intensity deconvolution
approach as well as several additional methods for
removing the particle size dependence on trajectory
are described in more detail in the following discussions
of the various techniques used.
4.2.1. Absolute intensity
Lorenz-Mie theory is the underlying principle that
explains the operation of nearly all instruments that
operate by measuring the absolute magnitude of the
scattered light. Essentially, Lorenz-Mie theory shows
that large particles, greater than 20/zm, scatter light
in proportion to the square of the diameter. The
relationship between the diameter and the power of
the scattered light increases dramatically as the
particles become smaller. For particles in the 0.10.2#m range, scattering intensity increases as the
sixth power of size. Early work on particle sizing
relied on either measuring the amplitude of the
scattered fight or the concept of visibility (discussed
later) to measure size. This was usually done using an
LDA systems, shown in Fig. 2, to provide the velocity
information and the light source. Measuring particle
size from the peak amplitude of the LDA signal was
first done on combustion flows by Yule, Ungut and
coworkers. 167'177 A later paper by Mizutani et al. 121
discussed the errors associated with this method and
proposed procedures to correct for them. Types of
errors discussed in this paper include the possibility
of two or more particles entering the sample volume
at the same time: a particle only partly in the control
volume, which would be represented as a smaller

particle; the dependence of the light-scattering signal


magnitude on the particle's location in the sample
volume; and the dependence of the sample volume
size on the particle diameter, since larger particles
have a larger effective sample volume due to the
Gaussian intensity distribution of the laser beam.
An instrument correlating scatter intensity with the
particle diameter was introduced by Holve and coworkers.94'95'97 In this instrument, a single heliumneon laser beam is used to illuminate particles and
the scattered light is measured in the near forward
direction. This creates some degree of insensitivity to
particle shape for particles with aspect ratios less than
two, as discussed in Section 2.2. Holve et al.94'95 also
developed an intensity deeonvolution algorithm that
statistically corrects the particle size distribution for
the intensity profile of the sample volume based on
the assumption that the trajectories of the particles
through the sample volumes are random. This method
is further explained in papers by Holve9 and Holve
and Annen. 96 Information on the speed of the particle
is found by measuring the time of flight of each
individual particle through the sample volume, as
described by Holve.91 Because of the intensity deconvolution algorithm needed, this technique is not capable
of measuring size-resolved particle and velocities.
However, it is capable of measuring both spherical
and nonspherical, solid and transparent particles with
aspect ratios smaller than 2:1 in a large variety of flow
conditions with number densities as high as 105-106
particles per era3. The optical configuration of this
method is shown in Fig. 8.
Equipment operating on this principle is manufactured by Insitec Inc. The PCSV-E (Particle Counter
Sizer Velocimeter) is a nonintrusive U-shaped instrument, where the transmitter and receiver are mounted
on opposite arms of the tube, instrument for laboratory
work. The PCSV-P is a probe version designated for
insertion into the flow field. Both instruments are
suitable for measurements in nonreacting and reacting
flows, with a particle size accuracy of 5-10%,
depending on the environment. A concise summary
of the PCSV instruments, the theory on which they
operate and their capabilities is given by Holve and
Meyer9s in Combustion Measurements, edited by
Chigier.

Laser-based techniques for particle-size measurement

285

I00(~
0
a.

U
III
~
t_

1C~)

0.01

0.0001
.00

10.00

100.00

1000.00

nd

-XFig. 9. Response functions for absorbing and nonabsorbing particles.


In the absolute intensity approach, the particle size
is determined from the maximum amplitude of the
light-scattering signal as the particles pass through the
sample volume of the instrument by using a response
function that is based on the scattered-light intensity
calculated using Lorenz-Mie theory. A separate
response function for light-absorbing and nonabsorbing particles is used to allow the instrument to
measure both types of particles. For systems based
on the absolute intensity of the scattered light,
instruments must be calibrated by the use of a
suitable reference before accurate measurements can
be made. Typical response functions for absorbing
and transparent particles, and their variation with the
complex part of the index of refraction are shown in
Fig. 9. These response functions are calculated using
Lorenz-Mie theory and the optical configuration of
the PCSV instruments. Essentially there is a monotonic relationship between particle size and intensity,
although several non-monotonic regions exist in the
response function. Because these regions where two
particle sizes result in the same value in the response
function occur over small size ranges, the overall
measured result is not adversely affected. Beam power
measurements are made before each measurement to
account for variations :in scattered intensity due to
duct window fouling or attenuation by other particles
in the beam path. In the PCSV instruments, two
beams with different beam waists was used to increase
the dynamic size range of the instrument. A small
beam measures particles with diameters in the range
of 0.5-2 #m, while the large beam measures particles
from three to several hundred microns, depending on
the optical configuration of the instrument. Measurements on the two beams are made sequentially, and
then concatenated to determine the total measured
distribution.
Several studies have been conducted with these
types of instruments, in addition to those done

by Holve and coworkers. Bonin 2a and Bonin and


Queiroz 25'26'27 have published several papers on
work done with a PCSV instrument in large-scale,
pulverized-coal boilers, as well as in controlled
atomization experiments. In a laboratory setting,
Baxter 21 has used the PCSV technique to study
char fragmentation and fly ash formation during
pulverized coal combustion. Baxter and Habib, 22 as
well as Dunn-Rankin et al. 44 have also used this
method in the study of coal-water slurries.
4.2.2. Intensity-ratio technique
The intensity-ratio method measures scattered light
intensity at two different collection angles, as determined by the size range of particles to be measured.
The technique can be applied to particles in the
0.1-10#m size range. The method was described by
Hodkinson, 87 who showed that is was possible to
obtain size information by measuring the scattered
light intensity at separate locations in the main lobe
of the particle's Fraunhofer diffraction pattern.
Hodkinson 87 also noted that the forward scattering
lobe described by Lorenz-Mie theory is very similar
to that given by the Fraunhofer diffraction equation.
Thus the technique can be applied to particles as small
as several times the laser wavelength where LorenzMie theory must be used. In a later study, Boron and
Waldie29 quantified the errors associated with this
assumption and showed that the error associated with
finding the particle size using this technique increased
with an increase in the relative refractive index, as
defined earlier. The increasing error is caused by
oscillatory factors in the particle extinction coefficient
(extinction efficiency). The particle extinction coefficient in this case is defined as the amount of light
removed from the incident beam by the particle
(scattered and absorbed) divided by the projected
area of the particle. These oscillating errors can be as

286

D.L. Black et al.


Beam

Laser

Dispersion MirrorExpander
Prism
Beam
Expander^

Polarization!
Rotator

Focusing
Lens^

Sample
Volume

PMT
Fig. 10. Optical configuration of the PIR technique.6

x~/~~mple
\

Volume
~R~eFocalPlane

SizingBeam
Fig. 11. Optical setup of the sample volume using a two-color method.
high as 40% for latex particles in air and approach
20% for latex in water. Due to the possibility of large
errors and the need to measure the intensity at two
separate locations, this method is not widely used for
particle analysis.
In a related method, called the Polarized Intensity
Ratio (PIR) technique, the ratio of the polarized light
intensity scattered from two different coaxial beams
illuminating a particle is measured and used to
determine the particle size. Azzazy and Hess 6 used
two coaxial beams of different wavelengths, polarized
in different directions. The measured light-scattering
signal of the two beams at 30 degrees from the
forward axis contained the information necessary to
determine the particle size. This is possible since
Lorenz-Mie theory contains information on both the
parallel and perpendicular polarization states of the
scattered light. The ratio of these two parameters
gives a unique curve that is only a function of particle
size. A schematic showing the implementation of this
optical system using an argon-ion laser is shown in
Fig. 10. Azzazy and Hess 6 compared measurements
taken using this technique with data from a pointerbeam instrument similar to one discussed in the
following section. From their data, they concluded
that the same type of oscillatory error is present in
the PIR technique as in the standard intensity-ratio
implementation previously discussed. They also found

ambiguities associated with the method which limits


the measurement range. This occurs because the
response is not monotonic with size. In general,
intensity-ratio techniques depend on the amplitude of
the light scattered in the forward direction and are
therefore sensitive to the complex index of refraction.
These techniques can also be used for nonspberical
particles provided the optics of the system are set up
to collect the scattered light in the near-forward
direction, which provides some insensitivity to
particle shape as discussed in Section 4.2.1.
4.2.3. Dual-beam sizing systems
Dual-beam, two-color systems, or pointer-beam
methods are all similar methods of particle-size
measurement characterized by the use of two
nested or coincident/coaxial laser beams at different
wavelengths. One beam has a relatively broad
diameter, while the second is focused to a smaller
waist coaxially within the larger beam. This configuration is shown in Fig. 1 I, where an LDA system is
positioned inside the size measurement beam for
velocity measurements. The light-scattering signal
from the smaller beam is used as a trigger (or pointer)
for the intensity measurement from the larger beam.
Particle size is then calculated from the lightscattering signal obtained from the larger beam.

Laser-based techniques for particle-size measurement


A

SizingBeam
Particle

287

~ / L
DopplerSignal
A

)V Beams
Scatter Sianal
Sizing Beam

From

Fig. 12. Top-hat beam sample volume cross-section and light scattering signals. 63

Triggering the signal in this manner assures that the


measured particle is passing through locations at, or
near, the center of the sizing beam. This minimizes
trajectory errors associated with the scatteringamplitude dependence caused by the Gaussian
intensity profile of a standard laser by assuring that
particles measured pass through the central, nearconstant intensity region of the larger beam. Systems
based on triggering beams have been used to size
particles in reacting, two-phase flows and in droplet
and spray characterizations.
Hess 77 describes such an arrangement in which an
LDV system for velocity measurement is positioned
inside a larger sizing beam, as shown in Fig. 11. The
optical geometry shown in Fig. 11 is typical of that
used in the various instruments designed using the
dual-beam approach. By requiting coincidence between
the signal from the sizing beam and the LDV beams,
the LDV signal can be used to trigger the sizing
measurement while simultaneously providing the
particle velocity information. Fincke et al. 56 developed
a system similar to that of Hess, but they also
performed two-color pyrometry on the particle at
the same time to obtain simultaneous size, velocity
and temperature. Wang: and Hencken describe the
application of such a system for measuring particle
size in the 10-200#m range. Their system used an
argon-ion beam for particle sizing and a concentric,
smaller helium-neon beam for the triggering signal.
Particle velocities were measured using the transit
time method described by Holve. 91 The complexities
of dual-beam systems involve the optical afignment of
the two coaxial beams needed for sizing and triggering
and the additional signal processing requirements
needed to process and compare the signals from the
two laser beams.
4.2.4. Top-hat beam technique
As previously discussed, one of the difficulties
involved in sizing particles using a standard TEM00
laser is the dependence of particle size brought about
by the Gaussian distribution of intensity. The top-hat

technique eliminates this problem by creating a beam


with a constant intensity distribution over most of the
beam width. However, the actual intensity profile of
the top-hat beam is not uniform over the entire beam
diameter but is characterized by a constant intensity
region in the center, with tails similar to a Gaussian
distribution appearing toward the edges of the beam.
With this method a trigger or pointer beam is not
needed, since the entire profile of the laser beam at the
sample volume is essentially at a constant intensity
out to the l/e 2 diameter of the original, unmodified
laser beam. The scattering amplitude dependence on
the particle trajectory is therefore minimized. Figure 4
illustrates the relationship between the scattered
intensity and the particle size for a top-hat beam
compared to the Gaussian beam and plane light
waves. The scattered intensity increases monotonically with size up to the l/e 2 diameter of the original
beam (100 #m), after which it falls off dramatically.
Although the top-hat beam minimizes the impact of
the intensity distribution of the beam cross-section,
the effect is still present to some degree in the
instrument response functions, due to the tails outside
the 1/e2 diameter of the original beam. Another
disadvantage of the top-hat beam technique is the
loss of laser power associated with the Gaussian filter
needed to create the constant intensity profile.
Allano and co-workers4 and Grrhan and Gouesbet 63
discuss implementation of this method. They describe
various methods of creating a top-hat beam profile,
the preferred approach being to use a filter with
Gaussian characteristics to create the necessary profile.
As the authors of the above papers demonstrate, a
standard LDV system can be focused inside the
top-hat sizing beam to yield simultaneous size and
velocity data, as is often done with the dual-beam
systems previously described. The configuration of
the probe volume and a typical representation of the
LDV and top-hat beam particle-scattering signals
obtained from this combined system are shown in
Fig. 12. The authors also present data from monodispersed droplet streams and compare them with
computations and holography measurements. Good

D.L. Black et al.

288

Measurement Volume
!

Transmitter
,

Laser Beam

Beaia S p l i t t e r

~ e c e i v e r

Deteetors ..... - - ' ' ' ~


Fig. 13. Simplified schematic diagram of a typical phase-Doppler optical system.

DIET 1
4;

OET2

DET @

^ ^.A.AA .AA
vvVVVVV
AAAAAAA,,^
- vvv_VVV
,
fi A A A A A

"vVVVVv

Fig. 14. High-pass filtered Doppler burst signals illustrating


the phase shift between detectors. 12
agreement was found, indicating satisfactory performance of the system. However, due to the disadvantages listed earlier and the development of techniques
to account for the intensity distribution in the sample
volume. The top-hat beam method is not widely used.
4.3. Amplitude-independent Methods
Some techniques for determining particle size are
not dependent on measuring the intensity of the
scattered light. Other features of the light scattered by
particles are used to determine size information, and
in some cases, the velocity of the particle as well.
These techniques generally suffer from fewer complications than the amplitude-based methods previously
discussed, however, they are usually more sensitive to
particle shape. Many of these types of instruments
have been used extensively in the study of two-phase
flows where liquid droplets or other spherical particles
are present. The following subsections discuss several
methods, listed in Table 2, that are insensitive to the
scattered light intensity. The advantage and disadvantage of the techniques are also discussed in each
section.
4.3.1. Phase-Doppler analyzers
The phase-Doppler technique is a well established
and widely used technique for measurement of droplet

size and velocity in sprays and solid-spherical


particles in two-phase flows. Commercial instruments operating on the phase-Doppler principle are
produced by Aerometrics, TSI, Dantec and Invent.
Many papers discuss in detail the method and its
supporting theory. The method was first described
by several researchers, including Bachalo, 8 Bachalo
and Houser 12 and Durst and Zar6. 46
Several summaries of the phase-Doppler technique
are available in the literature. Some of the most recent
are those given by Bachalo, 9 Bachalo and Sankar 13
and Sankar and BachaloJ 46 Other past reviews of
this methods include an overview by Bachalo, de
la Rosa and Sankar, 15 one by Bauckhage 2 and
another by Durst and Naqwi. 47 These papers provide
an overview of the phase-Doppler method and
discuss the advantages and disadvantages of various
implementations of the technique. Numerous references to the papers instrumental in the development of
the method are also provided, as well as some of the
recent experimental work done using phase-Doppler
instrumentation.
Figure 13 shows a diagram of the primary
components of a general PDA system. The phaseDoppler Particle Analyzers (PDPA or PDA) systems
are best described as LDA systems, discussed previously in Section 2.6, with particle-sizing capabilities.
Particle sizing relies on the measurement of the phase
difference in the light-scattering signal at two or more
spatial locations. The typical configuration for the
receiving optics is 30 from the forward axis. For
particles that do not scatter a refracted component, a
backscatter collection geometry of 150 can be used.
The forward scatter geometry is preferable, since
backscatter measurements introduce difficulties in the
instrument response function and limit the dynamic
size range of the method, as shown by Hardalupas
and Liu. 7~ Signal amplitudes in the backscatter
configuration are also lower than in the forward
direction, making data collection more difficult.
However, a PDPA system is insensitive to the index
of refraction of the particles in a flow in a backscatter
configuration, since only the reflected component is
measured. Although Fig. 13 illustrates only one set
of beams, additional crossed beam pairs forming

Laser-based techniques for particle-size measurement

289

3;50300"
250"
200'
I
a.

150
100'
50
0
d min

d max

Diameter (d)

Fig. 15. Representative response function for a PDPA system using three detectors.
interference patterns in other directions in the sample
volume can be established using different wavelengths.
This configuration allows particle-sizing systems that
measure one, two, or three velocity components.
Regardless of the velocity components measured,
only a single set of crossed beams is needed for
particle sizing.
To size particles, the PDA relies on the measurement of the spatial frequency of the interference
fringe pattern produced by the scattered light from
the particle. The interference fringe pattern produced
by the reflected and refracted rays from the particle is
a function of the optical parameters of the system, the
refractive index of the particle and the particle
diameter. The far-field interference pattern from the
light scattered from the particle at any particular
angle can be characterized by an amplitude and a
phase. In practice, the phase difference between the
light-scattering signal at two or more spatial locations
in the receiving optics is determined by finding the
time difference between the zero-crossings in the
Doppler signal between two detectors and dividing by
the measured Doppler period. The measured phase
difference, illustrated in Fig. 14, of the light-scattering
signal between the detectors can be linearly related to
the particle diameter based on geometrical optics.
Using this approach, the response function of a
PDPA instrument can be given by the following linear
relationship. 2
d = A__~__~
2zrF "

(7)

In the equation, A is the laser wavelength, ~ is the


phase shift between any two detectors and F is a
function of the optical configuration of the system
and the relative refractive index (N) between the
particle and the medium.
Figure 15 shows the instrument response function
for a typical PDPA system using three detectors. As

the diagram of the response function shows, the three


detectors provide a redundant size measurement that
can be used to check for sizing accuracy, since particle
size can be determined from the phase difference
between any two detectors. Additionally, the measurement range of the instrument is expanded. The
overall range of particle size that can be determined is
restricted by particles producing phase differences
between 0 and 360 degrees. Beyond this, larger particles
would be indistinguishable from smaller ones. The
particular measurable size range of a given instrument
is determined by the choice of optics comprising the
phase-Doppler system being used.
Phase-Doppler systems are capable of measuring
particles as small as 0.5#m to particles as large as
several millimeters in diameter. The maximum upper
sizing limit is governed by the Weber number, defined
as the ratio of the dynamic to the surface-tension
force acting on a drop.
W e = dpglVP - v~{z
ap

(8)

When W e << 20, then the droplets are spherical. As


the Weber number approaches 20, the droplets begin
to deform and eventually break up. it3 In this region,
the PDPA would no long give accurate results. Sizing
fine particles (< 10#m) has also been a cause of
concern, due to oscillations in the instrument response
function. Houser and Bachalo 15 and later Sankar
et al. 148 have shown that with careful selection of the
optical components of the system, the oscillations can
be minimized and particles as small as 0.5/~m can be
accurately measured. The phase-Doppler technique
has many advantages, such as providing timeresolved data, detailed velocity information, and
diameter and velocity cross-correlations. However,
its use is restricted to spherical particles. This occurs
because light scattered by refraction and reflection is
used to determine the phase shift in the light-scattering

290

D.L. Black et al.

signal that is a measure of the local radius of


curvature of the particle. Since for nonspherical
particles the local radius of curvature can vary by
large amounts, the calculated diameter based on the
measured curvature can result in large errors in
the particle size. Alexander e t al. 3 studying the error
associated with sizing nonspherical droplets, found
that the PDPA system overestimated size by 4 5 0 for
particles with an aspect ratio of 0.71 and underestimated size by 1 4 0 for particles with an aspect
ratio of 1.39. Under ideal conditions, velocities can be
measured to within 1% and particle size to within 4%,
although in actual measurements these errors increase
to some degree.
Several variations of the basic PDA systems are
also described in the literature. Naqwi e t al. 128'129
describe an extended phase-Doppler system for
measuring particle-size, refractive index and velocity.
This instrument incorporates four detectors in the
receiving optics. Two phase shifts are determined
from the four Doppler signals measured. The ratio
between the phase shifts depends on the particle
refractive index and is shown to be independent of
particle velocity and diameter. Naqwi e t al. 13
describe an extension of the phase-Doppler principle
to submicron particles by redefining the response
function of the system in terms of Rayleigh scattering
instead of geometrical optics. Von Benzon and
Bauchhavve, 169 who also discuss the application of
the phase-Doppler technique for sizing small particles, conclude that it can be done by modifying
the instrument response function, since the phasediameter relationship is not linear for submicron
particles. Using fibre optics, Domnick et al. 43 have
developed a miniature PDA system consisting of a
transmitter that uses a laser diode and a receiver
measuring 30 by 123 ran. Sankar and Bachalo 147 have
recently presented a description and theoretical
comparison between many of the variations on
the phase-Doppler method found in the literature.
They describe the various configurations used in
implementing the phase-Doppler technique and
show simulated results based on geometrical optics
theory of the signals obtained using the various
instruments. They conclude that many of the configurations proposed do not offer any real measurement
advantages over a properly configured standard
phase-Doppler system with advanced signal processing systems.
In the years since their development, a large
number of studies have been conducted using
phase-Doppler instruments. The papers mentioned
here and in other sections of this review are only a
sampling of the more recent and fundamental of the
many articles available in the literature. These serve as
a representative sampling of current phase-Doppler
work that can then be used as sources for any number
of similar studies or measurements done in the past.
Phase-Doppler instrumentation is particularly suited
to spray measurements and is a valuable tool in nozzle

characterization. Many studies of nozzles have been


completed, such as the work by Hardalupas and
Whitelaw. 72 McDoneU et al. ll9 recently conducted an
interlaboratory comparison of spray measurements
taken with several different instruments to establish a
'standard' spray for the evaluation of instruments
and operator performance.
The phase-Doppler technique has been and continues to be an important tool in the study of turbulent
two-phase flows. At a recent study on turbulence
properties in a confined swirling spray completed by
Brefia de la Rosa et al. 31 illustrates the capabilities
of this technique to measure turbulence parameters in
complex flow configurations. Phase-Doppler instruments have also been used to characterize the droplet
dynamics in a gas turbine combustor in two recent
publications by Wang e t al. 172'173 Other recent papers
illustrating the broad applicability of the phaseDoppler technique include those of Bachalo e t al.16 on
the interaction of droplets with large-scale eddies and
a characterization of fuel oil sprays from a y-jet
atomizer by Sayre et al.15 In addition to the extensive
experimental work done on sprays and droplets using
the PDPA technique, some work has also been done
using solid particles, such as glass beads. Sommerfeld
and Qiu 155A56A57 have conducted an extensive characterization of two-phase, swirling flows using a PDA
instrument for size and velocity measurements. The
detailed three-dimensional gas and particle velocity
information presented by these researchers provides a
useful data set for particle dispersion model evaluation and development is swirling, two-phase flows,
such as those found in many pulverized-coal fired
furnaces.
In addition to the experimental work, many
researchers have studied the performance and limitations of the phase-Doppler technique from a theoretical
perspective. A recent study by Albrecht et al. 2 provides
a theoretical analysis of the phase-Doppler system, in
addition to that given by Sankar and Bachalo. 145
Naqwi and Durst 126 also present a detailed model for
the simulation of phase-Doppler signals in the form
of a generalized treatment of light scattering from a
dual-wave system described in the following section.
Sankar et al. z49describe a theoretical treatment of the
light scattered from the sample volume by multiple
particles using a number of signal processing schemes.
They show that with Fourier transform signal
processing the size and velocity of two simultaneous
particles can be measured accurately. However, when
more than two particles are present in the sample
volume, the signal processing requirements become
extremely complex, and accurate measurements are
not feasible. Schaub et al. is1 studied the effect of
particle trajectory through the sample volume on the
performance of the phase-Doppler system. They
present a generalized theoretical model that incorporates the effects of finite beam diameter and arbitrary
particle location in the beam cross-section on the
phase-Doppler system. The study also compares

Laser-based techniques for particle-size measurement

291

Laser Sheet

[~

i S(d)

X-.~-

)J

Reflected Ray

Refracted Ray
Fig. 16. Particle scattering refracted and reflected light in an angle O.s

the results of this generalized theoretical model with


corresponding predictions from classical Lorenz-Mie
theory. Their work shows that Lorenz-Mie theory is
an accurate predictor for particles passing through
the center of the beams and that trajectory effects
tend to broaden the measured size distributions. This
occurs because it is possible for slightly different-sized
particles to have the same phase shift, depending
on the particle trajectory. Grrhan et al. 66 have also
investigated the effect of trajectory ambiguities for
a phase-Doppler system in both a backscatter
and forward scatter geometry. They use G L M T to
determine the light scattering variations due to the
particle trajectory and conclude that errors due to
trajectory can be specially significant when the particle
diameter is near the beam waist diameter.
Additional information on the limitations of the
phase-Doppler method is given by Edwards and
Marx 5 and Bachalo and Sankar. 13 Particular issues
addressed by these authors include the capability and
restrictions involved with using the phase-Doppler
method to measure concentration information, errors
involving the particle trajectory through the sample
volume caused by the intensity distribution across the
laser beam discussed in the preceding paragraph and
Weber number considerations as related to particle
sphericity. The primary motivation for these more
advanced theoretical descriptions of the PDPA
technique has been ~.o explain the oscillations that
are present in the response function, especially for
small particles; quantify the sensitivity of the response
to variations in refractive index; deal with the
problem of trajectory ambiguity; and to illustrate
the sensitivity of the system to nonspherical particles.

4.3.2. Projected grids


Particle-size measurement using projected grids is
accomplished by placing a grating in the receiving
optics in front of the detector and recording the lightscattering signal from the particle as the particle
passes through the sample volume. Size is determined
by analyzing the signal as the particle is seen through
different-sized gratings. The particle size corresponds
to the grating size where the scattering signal no
longer shows a plateau of intensity. An alternative
method is to vary the frequency of the grid and find
the frequency that causes a null point in the lightscattering signal as was done by Wang and Tichenor. 17 This frequency can then be related to the
particle size.
A similar approach was used by Semiat and
Dukler. 152 However, they also determined the particle
velocity by measuring the frequency of the lightscattering signal as the particle passed through the
fringe pattern generated by the gratings. A laser is
often used to illuminate the particles, although other
light sources are sometimes employed, For incandescent particles, no illumination is required and the
resulting signals are stronger than for an externally
illuminated particle. Errors involved using this
technique can be high, typically on the order of
10-20%.
A related imaging technique has recently been
proposed by Morikita et al. 122 and Hishida et al. 86
In this technique, a conventional LDA transmitting
system (as shown in Fig. 2) is used to define the
sample volume of the system and to obtain the
particle velocity information. In the shadow Doppler

292

D.L. Black et al.

d?
I '~
ii I ~1
$1 ,s ~S

Laser Diodes

Lens 1

Mask

'0

,~,

Detector

iI

01

,.,,-~ o2

Lens 2

%
Fig. 17. Diagram of the LMFV optical configuration.TM
method, the LDA laser beams pass through the
receiving optics where they are not blocked, but are
imaged with a photo diode array placed in the focal
plane of the collection optics. Size information is
found by analyzing the temporal signal of the diode
array to define the shadow of the particle passing
through the sample volume and therefore its shape.
This technique is useful for sizing nonspherical
particles and is insensitive to complications from the
index of refraction. The accuracy of the shadow
Doppler technique has been addressed by Hardalupas
et al. 73 They show that the sizing accuracy for both
transparent and opaque particles between 30 and
140#m is better than 10% of the measured particle
size for particles passing through the focal plane of
the transmitting lens. Additional error is encountered
from particles being imaged that are passing outside
the focal plane of the sample volume. This technique
has also been applied to a pulverized coal, laboratoryscale furnace to measure simultaneous size and
velocity information by Maeda et aL 11s.
4.3.3. Displacement
The pulse displacement technique uses a laser sheet
to measure particle size and velocity. The method is
capable of measuring particles from as small as a few
microns to as large as several millimeters in diameter.
The details of the technique were first described in
papers by Hess and Wood ys and Lading and Hansen. m
Additional details are given in two subsequent papers
by Hess and Wood. 79's Particle size is determined by
measuring the time between the reflected and refracted
rays scattered by the particle as it passes through a
laser sheet. With this information and knowledge of
the particle velocity, found by either traditional LDV
techniques or by measuring the transit time of the
particle, the separation distance between the refracted
and reflected pulses, S(d), can be calculated. S(d) is
then related to the particle diameter by
d =

2S(d)
cos rR + cos r L

(9)

where rR and rt are the refraction and reflection

angles, respectively. A schematic of the light scattering based on geometrical optics for sizing a sphere
using the pulse displacement technique is shown in
Fig. 16. This method of particle analysis depends on
the measurement of the correct particle speed to
determine the correct separation between the pulses.
For particles with unknown or varying trajectories,
this presents a problem in that particles not moving
perpendicular to the laser sheet will be inaccurately
sized. The change in the particle's refractive index
also represents a potential source of error, since the
method depends on measuring the refracted and
reflected light from the particle. The sizing limits
for this technique range from 0.2 to 1.5 times the
thickness of the laser sheet up to several hundred
times the sheet thickness, depending on the specific
optical configuration used to implement the technique.
In a technique that can also be described in terms of
displacements. Nakatani et a1.124 developed what they
call a laser three-focus velocimeter. A schematic of
this device is shown in Fig. 17. This device uses an
array of three laser diodes focused at the same
location to measure the particle size and velocity.
This is done by focusing the parallel beams to a set of
three parallel focal points. Since the spacing of the
focal points is known, the particle velocity can be
calculated from the time between the light-scattering
pulses measured as the particle passes through these
points. With this information, the particle size is
found by using two detectors and measuring the
refracted light from the particle. The delay time
between these two detectors can then be related to
particle size. This method has the same potential
problems with particle trajectories and refractive
index as the technique previously discussed.
4.3.4. Visibility
The concept of visibility, given the symbol V, as
related to particle sizing was theoretically established
by Farmer 51 in 1972 and later verified experimentally
by Farmer s2 and Hong and Jones. 13 By determining
the maximum and minimum scattered intensity from
a particle in the fringe pattern of an LDA system, the

Laser-based techniques for particle-size measurement


I

293

A_

0.6

0 . 4 . ~

0.2

0
0.00

'

'

'

I '
2.00

4.00

6.00

8.00

I0.00

nd
-'b-

Fig. 18. Fringe visibility vs. particle size for a sphere.

Slotted Mirror
Laser

Cell

Smnple Volume

t
~

Forward-Scatter
CollectionLenses

Slit

iI
I

mm~.mm

Slit

Fig. 19. Optical system for back and forward-scatter visibility measurements) 42

size of a spherical or nonspherical particle can be


determined from the visibility of the particle defined
by
V --- (/max - [min)
(/max + Imin)

(10)

where/max and Imin are the maximum and minimum


intensities in the pattern of light scattered by the
particle. In this method the visibility relates unambiguously to the particle size, provided it is larger than
0.15, as is shown by the plot of visibility vs. a nondimensional particle diameter shown in Fig. 18 for
spherical particles. In the expression for non-dimensional size, 6 represents the fringe spacing in the
sample volume and d is the particle diameter. For
the sphere, at visibilities below 0.15 the relationship
between visibility and particle diameter is no longer
monotonic and particle size cannot be uniquely

determined. The configuration of this method using


a standard LDV optical system is illustrated in Fig.
19. The approach can be implemented in either
forward or backscatter collection geometries and
the optical components for both are shown in Fig.
19. Farmer 53 developed a model to predict signal
visibility from LDA systems and addressed the issue
of sizing particles larger than the fringe spacing in the
sample volume. The results show how the size range
can be varied by aperture adjustments at the receiver.
As originally described, the visibility of a particle
could be found in either forward or back-scatter
configurations. However, Roberds 142 concluded that
only forward scatter was useful by examining experimental data taken using both configurations. Adrian
and Orloff t later showed that back-scatter information was limited because the visibility function
showed strong sensitivity to the imaginary index of

294

D.L. Black et al.

D e t e c t o r 1'1

Laser

Rouchi
Grafinl

"" ~
.,
..........

I ~ X

D e t e c t o r 1'2

Fig. 20. Diagram of the GVG optical system. 32

refraction in the back-scatter configuration. This


leads to an oscillating visibility response function
and a very small size range in which the results were
unambiguous. Negus and Drain 133 solved the problems associated with back-scatter signals by using
circular polarization and a specially designed aperture.
Although back-scatter measurements are possible
using the visibility technique, the measurement is
much more difficult than the forward-scatter measurement, which is largely independent of beam
polarization and particle refractive index. With the
visibility approach, response curves can be defined
for various particle shapes, providing capability for
sizing nonspherical particles. The primary disadvantage of the method is due to the large sample volume
defined by the collection optics. Although narrow in
diameter, a typical visibility sample volume can be
very long, providing the capability to measure particle
size only in very dilute flows.
Kliafas et al. 1" who discuss the effects of turbidity
(the degree of opacity produced by the media between
transmission/collection optics and the measurement
volume) on the visibility of the signal, conclude
that turbidity generates a spread in the measured
visibilities that increases with increasing particle void
fraction. Son and Gie115s studied the uncertainties in
the visibility response function and quantified the
effect of receiver lens size, refractive index, fringe
period and measurement location. As Farmer shows, sa
independent, simultaneous size measurements can be
done by using signal visibility and the magnitude of
the scattered signal. This provides a check on the
accuracy and consistency of the sizing measurement,
which can be difficult to determine in many optical
sizing systems.
4.3.5. Miscellaneous particle analyzers
Some methods of particle-size analysis do not fit
into any of the above categories. In general, these
techniques have been used by a small number of
researchers, or are limited in their applications. These
techniques are often used to do fundamental research

on light scattering only, or to describe results that


are useful for the understanding of other methods of
size analysis. The following briefly describes several
of these methods.
Cartellier 32 describes the application and theory of
a system very similar to the phase-Doppler signal,
except for its applicability in high-number-density
flows and dense suspensions. In this method the
optical grid is generated by using a transmission
grating instead of the crossed beams of the phaseDoppler approach. Figure 20 shows the geometric
layout of the optical components of a Grating
Velocimeter-Granulometer (GVG). The GVG instrumentation is more compact than typical PDPA
systems, and the signals generated by the system
closely resemble Doppler bursts. Laali et al. ll4 further
describe the system and present data collected with it.
A study of Gaussian beam effects on the light
scattered from a single droplet by Hesselbacher,
Anders and Frohn s~ illustrates a method of finding
particle size by evaluating the fringe spacing of the
scattering pattern. This method is shown to be a
highly accurate approach to sizing monosized droplet
streams, and it is insensitive to the effects of Gaussian
beams. Measurement accuracy is better than,2%,
provided the laser beam is larger than the particle.
This approach is not suitable for evaluating large
numbers of droplets of different size as is found in a
spray, since the scattering pattern for each individual
particle must be analyzed to determine the size
information.
Several papers by Naqwi, Liu and Durst 127'131
describe a Doppler-based method that relies on the use
of cylindrical waves. The arrangement of the essential
optical components in a DCW system is shown in Fig.
21. Particles pass through a fan of fringes created by a
pair of interfering cylindrical waves. The scattered
light is collected by two detectors. The signal from
one detector positioned normal to the fringes gives a
standard Doppler signal whose frequency is a measure
of particle velocity. A second detector located at some
angle from the forward direction receives a signal
at the Doppler frequency fd, plus the aniosotropic

Laser-based techniques for particle-size measurement

Loser

Beom-Exponder
Beom-Splitter

Mirror

295

Cytindn~colLens

Beom-Merger
Mirror
MovingPortiele

Loser Beoms

Detector

C y h n d r i c ~

Fnnges
Monosize Portictes

Fig. 21. Optical layout for the experimental DCW system, TM


Particle
Field
[AlSer

Fourier
Transform

Beam

i
Light

,~

De~tors
in Focal
Plane

Fig. 22. Optical set-up for laser diffraction particle sizing.


frequency )ca, that is linearly related to the particle
diameter d. The equation for transparent particles
relating the particle diameter to the measured
frequencies is
fa
fd

m cos O
d
2X/2(1 +cos~b)[1 + m 2 - m v / 2 ( 1 +cos~b)] zz

(11)
where m is the index of refraction and 9, ~ and z
describe the physical geometry of the system, as
shown in Fig. 21. In the system described above, the
particle size in the dual-cylindrical wave method is

related only to the frequency of the Doppler signal.


This greatly simplifies the signal processing requirement for data acquisition, making it similar to signal
processing techniques used in LDV systems. However, the alignment and implementation of the optical
system is somewhat difficult. The detailed derivation
of the relationship between the signal frequency and
the particle diameter and velocity is presented in
papers by Naqwi et al.128'129 Naqwi125 also presents a
theoretical analysis of the technique and elaborates
on the design and operation of the DCW system. The
DCW technique has only been used as a research
method and no other work has been done with it

296

D.L. Black et al.

Traction
Volume

Fig. 23. Sample volune comparison between diffraction and SPC instruments. 39

other than the demonstration of the concept by the


developers.

5. ENSEMBLE METHODS OF SIZE ANALYSIS

Ensemble methods of particle sizing measure the


distribution of a group, or ensemble, of particles.
Most methods falling in this category use Fraunhofer
diffraction to describe the underlying physics on
which measurements are made. However, Zege 178
has suggested using a generalization of small-angle
scattering to determine the overall particle size
distribution of a group of particles. Methods that
incorporate Fraunhofer diffraction are well established and are used in a variety of fields. The following
references represent only a few of the many studies
completed using instruments such as the Malvern
particle analyzers, the Coulter LS series of instruments,
the Insitec EPCS (Ensemble Particle Concentration
and Size) instrument and the Leeds and Northrup
Microtrac analyzer. The majority of these instruments are designed for off-line instruments suitable
for work in the laboratory as bench-top units.
However, some instruments have been designed
specifically for on-line measurements in production
processes and other applications.
5.1. Fraunhofer Diffraction Based
Ensemble diffraction-based instruments are well
established for measurement of particle size distributions of both aerosols and powders in a wide number of
both research and industrial environments. A general
diagram of a diffraction-based sizing system is shown
in Fig. 22. Swithenbank et al. 163 present a general

review of the diffraction technique and theory in


Combustion Measurements, edited by Chigier. 34
Particle-size analyzers based on Fraunhofer diffraction are among the most well known methods of
size analysis currently in use. Diffraction-based
instrumentation for particle-size measurements was
first developed by Swithenbank e t al., 162 whose work
later became the basis for the Malvern particle-size
analyzers. Diffraction-based particle analyzers pass a
laser beam through a sample that is either dispersed
in a liquid or entrained in an air stream. The light
scattered from all particles in the sample volume is
collected with a Fourier transform lens and focused
onto a detector, or series of detectors, of suitable
geometry to characterize the angular separation of
the incoming scattered light. A Fourier transform lens
describes a standard lens used in such a manner that
the angle of the incident scattered light corresponds to
a particular annular position in the focal plane of
the lens, regardless of the position of the scattering
particle. Above the Rayleigh limit, small particles
scatter light at large angles, while large particles
scatter light near the optical axis of the incident
laser beam. From Fraunhofer diffraction theory, the
particle size distribution can be determined from
the angular distribution of scattered light across the
detectors. The sample volume for SPC systems and
the line-of-sight, diffraction-based instrument are very
different, as depicted in Fig. 23. This diagram graphically
illustrates the nature of the ensemble measurement.
With the ensemble technique, the distribution of the
entire group of particles in the sample volume is
determined. In contrast, SPC instruments collect
particle-size information restricted to a small region
of the illumination beam.
Diffraction instruments must incorporate some

Laser-based techniques for particle-size measurement

Fig. 24. Basic transmissometer optical set-up.


method to invert the relationship between the
scattered intensity pattern and the size distribution.
There are at least two ways to accomplishing this:
iterative numerical methods and analytical inversion
techniques. Traditional methods for accomplishing
this inversion are presented by Bayvel and Jones. 23 In
more recent work, an analytical method for evaluating the integrals involved in calculating the particle
size distribution from the forward scattering pattern
was formulated by Knight et al. 112 Their formulation
of the integral transform does not require that
the experimental data be numerically differentiated.
Comparison with results from a Malvern analyzer
showed that the analytical transform accurately predicts
the size distribution of the latex particles studied.
Diffraction-based particle analyzers are among the
most well-known and widely used of all laboratory
or off-line, laser-based sizing methods. They are
employed in a variety of applications and have been
studied in detail by a number of researchers. Hirleman
et al. s5 studied the effect of the sample volume and
receiving lens on the operation of a Malvern particle
sizer. They found that ideally, the instrument response
does not depend on the position of the particle in
the sample volume. However, due to nonidealities in
practical systems, such as finite lens aperture and
lens aberrations, variations of 15% in the response
function of the instrument can occur due to particle
position. They also present a theoretical model to
predict the instrument response as a function of
particle position to the sample volume.
An assumption generally incorporated in some
diffraction-based instruments is singular scattering
of incident light by particles in the flow field. In this
situation the light scattered at any radial location in
the focal plane of the receiving optics is the sum of all
the individual particle diffraction patterns in the
sample volume at that location. Multiple scattering
is characterized by the interaction of the collected
scattered light by more than one particle. Therefore,
the overall diffraction pattern in this case is not simply
the sum of the individual particle diffraction patterns,
but represents a more complex summation of
the scattered light. To measure size distributions in
high number-density flows where multiple scattering
effects are present, researchers have developed methods
to resolve this problem. Hamidi and Swithenbank 69
resolved the problem of multiple scattering by the

297

particles in the sample volume by use of the beam


extinction as a parameter in a set of correction
equations developed from earlier work by Felton
et al. 55 They also determined in their study that
multiple scattering effects become significant only at
extinction greater than 50%, where extinction is the
fraction of light scattered out of the beam path by
the particles. Therefore, since many measurements
are done at extinctions of less than 50%, multiple
scattering is not a significant problem and some
commercial instruments do not account for this effect.
When needed, multiple scattering can be accounted
for in determining the particle size distribution using
procedures explained in the literature.
Hirleman 83 also treats the problem of multiple
scattering theoretically by considering multiple scattering orders for the discrete annular detectors of the
sizing instrument. Multiple scattering orders are
defined by the number of scattering events undergone by a photon before it reaches the detectors.
Under the single particle scattering assumption, the
scattering order is one. Excellent agreement is shown
by Hirleman between this theory and experimental
data. Holve and Harvil199 have also worked on solving
the multiple scattering problem using the theory
outlined by Hirleman. They have developed a method
to solve the problem of accounting for multiple
scattering with an unknown size distribution. Experimental results indicate successful correction of the
scattering data down to light transmissions of 5%.
The problem of multiple scattering continues to be a
concern to researchers who are interested in measuring dense two-phase flows and is still a topic of
investigation, as evident in a more recent study by
Paloposki and Kankkunen 136 on the effects of multiple
scattering on the size distributions of glass spheres
measured by a diffraction-based sizing instrument.
5.2. Transmission B a s e d
Transmission measurements relate the drop in
transmission of a laser beam to the volume of particles
contained in the path of the beam. The simplest
instrument of this type is called a Transmissometer,
shown schematically in Fig. 24. In measurements
using this technique the pathlength of the beam is
made long enough inside the flow field that significant
extinction (10-20%) of the laser beam occurs. By
assuming a size distribution function for the particulates, the total volume of particles in the sample
volume (the entire pathlength of the laser) can be
determined. This is done by using Bougeur's law,
which was discussed in Section 2.7.2. This technique
is often used to estimate the concentration of soot
in flames, since there are no currently proven, readily
available in-situ measurements systems for sizing
submicron particles in flames.
Another system built by Insitec for monitoring of
particle concentration over time is the TESS (Transform method for Extinction-Scattering with Spatial

298

D.L. Black et aL

80-

+
Powder manufacturer supplied
---o----Insitec ensemble diffraction (EPCS)
=
Impactormeasurements
=

~ / rv~
/ / /~"

20-

0.1

10

I00

Particle Diameter ~ m )

Fig. 25. Comparison between several types of particle-sizing instrumentation on measurements of silicon
dioxide powder.

100

---0- I.AStER-DIFF'RAClION~
p~s~-ooPpt~ srs suo

SMD J

80

~eo
t

~,

40
2o

r,,,
hi

I--

-5

- 14

- t3

/2

-1

RADIAL DISTANCE FROM CENTERLINE (ore)

Fig. 26. Comparison of the D32 measured as a function of


radial location by Aerometrics phase-Doppler and Malvern
laser diffraction instruments. 4
resolution) instrument) 2 This system determines
particle concentration and the Sauter mean diameter
in the 1-100#m range based on measurements of
ratio between the scattered and transmitted laser light.
Outside this range the instrument must be calibrated
to accurately reflect particle concentrations. Since the
instrument is built as a probe with an approximately
10era long sample volume, spatial resolution is
provided by inserting the probe in the flow of interest
and measuring the average result in the probe's
sample volume at various locations throughout the
flow field.
5.3. Comparisons Between Different Size Analyzers
Several studies compare measurements done with
ensemble sizing systems to measurements done with
SPC systems or sieving results. Boyko et aL 3 compared

the results of the Insitec EPCS system with sieving


results and the single particle PCSV system also
developed by Insitec. Nathier-Dufour et a l l 32 compared the results of the Malvern Master Sizer with sieve
results. Dishman et al. 38 compared the results from a
Leeds-and-Northrup Microtrac analyzer and a sieve.
An example of comparison measurements on a silicon
dioxide powder by several types of instrumentation,
both SPC and ensemble, are shown in Fig. 25.
Agreement between the methods used in the various
studies discussed above was generally good; however,
under some circumstances, significant differences
were found.
The differences were blamed on the different
nature of the sizing techniques, the irregularity of
the particles, flow stratification and the differences in
the sample volume between the various methods.
Particle shape was the dominant factor in measurement differences because of the way the particles are
measured. This result is clearly illustrated by Kanerva
et al. 19 in a comparison of diffraction measurements
with a microscopic technique on three different
particles with widely varying aspect ratios. Their
results clearly show that reliability in the absolute
measurement done with optical instrumentation
decreases as the particles become nonspherical. This
result is supported by the authors of other comparison studies in which nonspherical particles were
measured.
Differences for nonspherical particles between
methods are especially prevalent between measurements completed with optical instruments and
mechanical sieves. Optical systems measure an
average spherical diameter for the particle, while
mechanical methods such as sieving measure the
smallest diameter of the particles. Due to this effect,
optical measurements of nonspherical particles will
always be larger than sieve measurements. However,

Laser-based techniques for particle-size measurement


Liae-at-~lht
Ring n~

t~

Fig. 27. Deconvolution ring and line-of-sight measurement


w:flume.7

trends in the size distributions were predicted


properly by all the methods used.
There have also been several comparison studies
between various instruments on droplets and sprays.
Comparisons made by Jackson and Samuelsen 17 on
a cold spray between the visibility, phase-Doppler
and a Malvern laser diffraction instrument show close
agreement among the three methods. Zurlo et al. is
studied the differences in the measurements of three
techniques (ensemble scattering, phase-Doppler and
intensity deconvolution) on a kerosene spray. The
methods used all gave slightly different results at
various locations in the kerosene spray. Differences
were attributed to the wide size distribution of
particles in the spray and in the limited dynamic
range of the instruments. Dodge and co-workers 39'40'42
have also published several papers comparing spray
measurements done with an Aerometrics PDPA and
a Malvern laser diffraction size analyzer: In addition
to comparisons between the PDPA and the Malvern
instruments, one of these references 39 reports measurements from four other types of instruments. These
studies show excellent agreement between mean
diameters measured by the two methods, as illustrated
in Fig. 26. Dodge and Schwalb 41 have shown good
agreement between phase-Doppler measurements, a
diffraction-based particle sizer and C F D (Computational Fluid Dynamics) simulations for a nonevaporating spray. A sample of the measured Sauter mean
diameter from these experiments is shown in Fig. 26.
Since the two instruments have very different sample
volumes, the measurements from the Malvern system

299

have been manipulated to provide a spatial resolution


similar to that measured using an SPC instrument.
Dodge e t al. 39'40'41'42 describe detailed procedures
to account for the temporal distribution measured
from the phase-Doppler particle analyzer and the
spatial distribution measured by the Malvern analyzer. To convert line-of-sight data obtained with the
Malvern system to equivalent point data, they used
the technique established by Hammond. 7 The need
for this procedure is illustrated by the comparison
between the SPC sample volume and the line of sight
measurement volume of the diffraction-based instruments shown in Fig. 23. Due to the different sample
volumes of the instruments, the data from one type
of instrument must be converted into an equivalent
form of data from the other comparisons between
measurements with different instruments can be made.
The procedure described by Hammond involves
dividing the measured region into a series of concentric
rings. Figure 27 illustrates how the rings are defined
for each measurement. A series of measurements is
then taken at the radius of each ring seen with the
line of-sight instrument. The mathematical procedure
presented in Hammond's paper 7 can then be used to
determine the size distribution and number density in
each ring by using the previously measured information from all the outer rings.

6. A P P L I C A T I O N S OF LASER-BASED SYSTEMS

Applicability of the techniques discussed in this


paper to industrial needs and problems is important
if laser-based methods of particle-size analysis are
to find wide acceptance in both the industrial and
research environments. Eventually, research into new
techniques and theories should result in instruments
and techniques that have applications in some practical
environment. To accomplish this goal, both fundamental research into new approaches as well as
development of instrumentation is needed. For this
type of development to continue, a demand for
the developed products needs to exist; whether in
a research setting, such as two-phase flow measurements for model validation, or in an industrial
application such as quality and process control.
6.1. Industrial Uses

Some laser-based methods, especially SPC methods


of particle-size analysis, are beginning to find additional
applications in industrial environments. In the past,
many laser-based SPC methods have been employed
primarily by researchers at universities and private or
government research facilities. Few of the techniques
described in Section 4 and 5 have developed into
commercial products and hence are not available
to industry. This is now changing as new price
competitive systems are being designed that withstand
the rigors of industrial environments. Instruments

300

D.L. Black et al.


350

'

'

'

'

'

'

'

'

'

'

'

'

'

'

'

'

Sieving medlam
particle diameter

300

---<>--Ensemble

scattering

angular light
median

250

a
,m

200

150

100

50

....

I ....

I * , * , l , , , , l l l l l l

J , , , I

....

Run number

Fig. 28. The volume distribution's mean particle diameter for sieving and ensemble angular light scattering
over eight test runs. 76
employing Fraunhofer diffraction, such as the
Microtrac, Coulter and Malvern particle analyzers,
have been used for some time in a large number of
industrial, lab-based environments. 123 These techniques have enjoyed wide acceptance for a number of
years because of their ability to measure powder and
droplet size distributions easily and consistently.
Traditional particle analyzers consisted primarily
of off-line instruments and have been used for quality
control and laboratory analysis. Through recent
development of SPC and ensemble diffraction
systems, laser-based instruments are also now
capable of providing real-rime, on-line information
suitable for process control in manufacturing processes. Wedd 175 illustrates the increasing focus
on particle measuring systems designed especially
for the industrial community. Poh1138 and Weiner and
Fairhurst 176 discuss the selection of instrumentation
suitable for use in a particular industrial application.
Issues such as size range, imaging vs. nonimaging
systems, diffraction vs. single-particle methods, informarion content of the measurement, time involved in
sampling and measuring, as well as use of nonoptical
techniques among other concerns, are discussed
specifically in relation to the application of sizing
instrumentation in industrial environments.
6.1.1. Manufacturing processes

A wide variety of industries depend on methods of


particles size measurement to monitor and control
product manufacturing processes and product quality. Examples of these include producers of metallic
powders, pharmaceuticals, toners, paint products,
foods, cosmetics, ceramics and other products. Particle
size plays a critical role in manufacturing consistently
high-quality products in these areas. For example, the
release of medicine in the body is a strong function

of the particle size distribution of pharmaceuticals.


Pigment size distribution is a critical parameter in
determining the hiding power of paint. Taste and
texture of many foods and consumer products are
strongly related to the size distributions of the
particles they are made from. Copier toner must be
sized carefully and consistently to ensure proper flow
and printing properties.
Heiskanen 75 examines some of the difficulties of
controlling particle size in a number of particulate
processes and discusses the need for controlling
particle size as an essential step in increasing the
performance of processes dealing with particulates.
This objective requires the use of on-line devices that
will incorporate into the control systems governing
the processes, as well as the use of laboratory-based
instruments for assuring product quality. Parsons 137
briefly discusses particle analyzers suitable for use in
the laboratory and for process control. This paper
specifically focuses on using instrumentation based on
laser diffraction for particle-size analysis in industrial
processes.
6.1.2. On-line process control
Equipment has been developed for on-line process
control in industries that use and produce powders.
Holve 92 discusses the implementation of various
diffraction-based methods of process control and
analysis, in addition to the considerations involved in
selecting instrumentation for a given application. One
instrument developed specifically for this purpose
is the EPCS (Ensemble-Particle-Concentration and
Size) instrument manufactured by Insitec Inc. Harvill
and Holve 74 discuss instrument performance and its
ability to provide continuous monitoring of particle
size and concentration during the manufacturing of
powders. In another paper relating specifically to the

Laser-based techniques for particle-size measurement


EPCS instrument, Holve 93 compares the results of
the diffraction-based instrument to sieve results on
measurements of salt crystals. These results are shown
in Fig. 28. Ensemble measurements were, on average,
33% larger than the results from the sieve. Differences
between each measurement type were primarily
attributed to the fact that sieves measure the smallest
dimension of a particle, while diffraction instruments
measure the potentially larger, average projected
diameter of the particle, Differences were also associated with the coarse size classes of the sieve compared
to the higher resolution of the diffraction instrument.
Although the initial cost of such monitoring
instrumentation can be high, the potential benefits
and increasing use of this type of technology in
industry will continue to make it more useful and
economical. Henein et al. 76 discuss the applicability
of on-line particle sizing in the atomization of zinc.
The authors indicate that although no on-line sensors
existed at that time to assess the size distribution
quantitatively, the laser-based, PCSV system discussed
earlier could be used as such. Sparks and Dobbs ~s9
discuss the performance of a Partec particle-size
analyzer on transparent and opaque particles. They
find that the instrument is suitable for implementation
in a process control system and provides accurate
results for opaque, reflective particles. However, large
errors occurred for all types of particles less than
about 5 #m in diameter and for transparent particles.
6.2. Research

Research needs in various disciplines requiring


the study of particle size distributions and velocities
continue to have a strong influence on the design
and development of optical sizing systems. Research
applications of particle-sizing techniques are usually
specialized in that the equipment is specifically adapted
or constructed for a particular application. This results
in more time, money and a higher level of operator
ability than are typical for industrial applications.
Abilities to measure nonspherical particles accurately,
obtain detailed velocity data, determine particlevelocity interactions, among others, continue to
advance the development of optical systems and the
signal processing capabilities to implement them.
Applications of laser-based particle-sizing techniques
to research include characterization and study of
turbulent, two-phase flows, analysis of condensed
phase in combustion systems and characterization
and study of solid particle dynamics. Many specific
references on these research orientated subjects are
discussed in the description of the individual sizing
techniques given in Sections 4 and 5. This is
particularly true in Sections 4.2.1., 4.3.1., 5.1. and
5.3., where well-developed instrumentation is discussed that is commercially available to the research
and industrial communities.
Alliances of industry with researchers have resulted
in several studies that have potential application

301

in industry. One example of this type of effort


include particle measurements on large-scale, industrial boilers such as those done by Bonin and
Queiroz 24'26'27and Giel et al. 57 Measurements such as
these are taken to provide information useful for
model development and to increase knowledge of
the complex phenomena involved in the large-scale
combustion processes. Another example is measurements done by Holve et al. 11 on hydrofluoric acid
aerosols. The motivation for this study was to
understand the effect of water spray mitigation on
the accidental release of hydrogen fluoride into the
atmosphere.

7. CONCLUSIONS

The laser-based methods of particle-size analysis


reviewed are divided into two broad categories. Single
Particle Counters (SPC) are characterized by small
sample volumes and are restricted to measuring a
single particle at a time. Single particle counters can
further be classified as amplitude independent or
amplitude dependent. Ensemble instruments, characterized by line-of-sight sample volumes, measure
the average size distribution of a group of particles.
The characteristics of the various techniques discussed in this review have been summarized in Tables
3-5. Tables 3 and 4 present overviews of the
nonamplitude-based and amplitude based instruments, respectively. Table 5 lists the terminology
and guidelines used in developing these summaries.
The unique nature of the laser allows the development of many different sizing schemes for application
in a wide variety of situations. Use of lasers allows
detailed in-situ measurements to be made in environments not accessible to other types of particle-sizing
systems, due to high temperatures, the hazardous
nature of the environment, or risk of contamination.
Many of the laser-based techniques discussed in this
paper for particle-size measurements will continue
to play an important and increasing role in many
fields, including droplet and particle measurements in
combustion science, nozzle characterizations, powder
manufacturing technologies, manufacturing of consumer products and industrial process control.
work was sponsored by the
Advanced Combustion Engineering Research Center
(ACERC) at Brigham Young University. The authors
would also like to thank Dr William Bachalo from
Aerometrics Inc. for his valuable comments and suggestions
regarding the text.

Acknowledgements--This

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