METALLOGRAPHY

6, 93-101 (1973)

93

Particle Size Distribution by Area Analysis: Modifications and Extensions of the Saltykov Method *

HOMER D. LEWIS, KENNETH L. WALTERS, AND K. ALLAN JOHNSON

Los Alamos Scientific Laboratory, University of California, P.O. Box 1663, Los Alamos, New Mexico 87544

The stereological problem of estimating the size distribution of particles in a sample volume from area analysis of a planar slice is examined. Two approaches to the problem are considered. The first involves selection of size interval end points related by a constant multiplier, C. A computer algorithm is developed for calculating spherical intersection probabilities for any set of size intervals having end points related by any C. A table of coefficients for the estimation of the number of particles per unit volume in thirty size intervals whose end points are related by C=10 '1 (the Saltykov multiplier) is presented. A table based on C=10 '5, is also presented. The computing formula is shown to be independent of absolute end point values and a generator of an invariant set of probabilities for any particular value of C. The second approach provides an algorithm for computer solution of the general problem where the values of size interval end points need not be related, and where the particle shape, i.e. intersection probability function, may change from interval to interval. The practical implications of all computing methods are briefly discussed.

Introduction
One of the more difficult problems in applied stereology is the estimation of the size distribution and n u m b e r of particles per unit volume in a system of heterogeneously sized particles from measurements on a sample surface. Investigation of the utility of the Saltykov type procedure [1] is of interest for several reasons. T h e data generated by modern automatic image analysis devices, such as the Quantimet 720 [2], directly provides a sample distribution of intersected particle areas observed on a random test plane, the sample test probe being the plane of observation. T h e Saltykov method is directly applicable to analysis of this type of data without consideration of the problems which may be inherent * Work performed under auspices of United States Atomic Energy Commission. (~ American Elsevier Publishing Company, Inc., 1973

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Homer D. Lewis, Kenneth L. Walters, and K . Allan Johnson

in analysis of intercept data generated by multiple parallel interception of particles by the video scan test probe used in automated image analysis equipment. The use of instruments like the Quantimet 720 and CDC 7600 computers, allows major extensions of the Saltykov procedure. In addition to generating highly accurate sets of coefficients, algorithms have been devised for calculating coefficients for any defined set of intersection probabilities. This procedure allows for the calculation of coefficients for any particle shape for which appropriate intersection probabilities can be determined. It will be shown that under certain conditions, a single preselected set of size intervals can be used for any practical Saltykov type analysis where the maximum size particle falls within the domain of the set. A study of the definition of intersection probabilities for nonspherical shapes currently presents problems in implementation [3]. Thus the spherical case is usually extended to cases where the underlying assumptions [1] are not exactly met. The algorithms presented have only been applied to the spherical particle case, but are not limited to such restriction.

Classical Saltykov Method

The Saltykov equation for examining circular cross-sections [1], provides a simple, compact approach to the calculation of the number of particles per unit volume in the Kth interval, NvK. Nv~ D~ [1.6461 N Ax -- 0.4561 N ~ ( x - o -- 0.1162 N A(x-2) - - 0.0415 NA(x-a) -- 0.0173 NA(x-4) -- 0.0079 N~(x_5) - - 0.0038 NA(x-6) -- 0.0018 NA(x-7) -- 0.0010 N A ( K _ S ) - - 0.0003 NA(K-9) -- 0.0002 NA(x-lo) - - 0.0002 NA~X-11)].

(1)

Based on the intersection probabilities of a random test plane cutting a test sphere [3], Saltykov's coefficients theoretically correct the observed number of particle sections per unit area for the ith intersection size interval, NAi, for contributions from particles of larger spherical diameter [1, 3]. Using this "classical Saltykov" formula employing these particular coefficients, based on interval end points related by the multiplier 10.x, requires no sequential calculations, nor tables of coefficients, as do some other techniques [4]. The intersection probabilities are the key to the calculation of coefficients. Utilizing Saltykov's derivation [1], an alternate, more general form of the equation may be obtained,
NvK -- DI@I

[NAK --

P2Na(x-x) - - PaNt(x-a) . . . . .

pxN~a],

(2)

where P x is the intersection probability in the ith intersection size interval,

Extensions of the Saltykov Method

95

and Nsx = DxNvx. T h i s equation, implicit in Saltykov's o w n derivation, forms the heart of one of our c o m p u t e r algorithms and leads directly to highly accurate evaluations of the coefficients. T h e thirty coefficients s h o w n in T a b l e I were generated by setting all Nax values equal to one, t h e n calculating the K t h coefficients each corrected for contributions f r o m all larger size intervals. Alternatively, e q u a t i o n two m a y be expressed algebraically to indicate t h e c o n t r i b u t i o n of all intersection probabilities in the estimation of NvK. (See Table II) TABLE I Computer Generated Saltykov Coefficients Based on Size Intervals Related By the Constant Multiplier 10"1 1. 2. 3. 4. 5. 6. 7. 8. 9. 10. 11. 12. 13. 14. 15. 1.64612085334 0.456122645308 0.116190477752 0.41494511474 x 10 -x 0.17271104925 x 10 -z 0.7794637145 x 10 -~ 0.3683810805 x 10 -2 0.1789500627 x 10 -2 0.884056423 x 10 -~ 0.441358745 x 10 -3 0.221811628 / 10 -3 0.111946135 x 10 -3 0.56650647 x 10 -4 0.28717815 x 10 -4 0.14574049 x 10 -4 16. 17. 18. 19. 20. 21. 22. 23. 24. 25. 26. 27. 28. 29. 30. 0.7401493 x 10 -s 0.3760609 x 10 -s 0.1911286 / 10 -5 0.971575 x 10 -6 0.493947 x 10 -6 0.251141 x 10 -6 0.127696 x 10 -6 0.64931 x 10 -7 0.33017 x 10 -7 0.16789 x 10 -7 0.8537 x 10 -8 0.4341 x 10 -s 0.2207 x 10 -s 0.1122 x 10 -s 0.570 x 10 -6

Coefficients can be calculated using t h e equations in T a b l e I I b u t this m e t h o d clearly b e c o m e s awkward after v e r y few terms. A t t e m p t s to obtain a recursion f o r m u l a by e x t e n d i n g these equations w h i c h involve only values ofpx and NAnhave so far p r o v e d unfruitful.

A Generalized Modification of the Saltykov Method

Practical i m p l e m e n t a t i o n of a u t o m a t e d area analysis is based u p o n one of two m e t h o d s of selecting the end points defining the size intervals of o b s e r v e d intersected planar areas. T h e m o r e general m e t h o d , w h i c h will be discussed in a s u b s e q u e n t section, makes no a s s u m p t i o n concerning the relation a m o n g end p o i n t values. T h e o t h e r m e t h o d is based on selecting a set of size intervals w h o s e end points are related by a constant multiplier. T h e classical Saltykov, w h i c h is of this type, defines a set of intervals w h o s e end points are related by a m u l t i p l y i n g factor of 10 "1. T h e set of intersection probabilities, hence coefficients, can be

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Homer D. Lewis, Kenneth L. Walters, and K. Allan Johnson

TABLE II Algebraic Solution for NVK, K = 1, 2.... , 6

Nv~ = D~" t,--~[Na,],

1 1

1 I p, NV2=DT"2"Pll [1.ONA2 Pl N A,], NV3=D~'pl

.

~NA2--

--~f

AIJ'

1 1 [1.0 NA4 _ P2N

P~] -~-~f N~

{~1 NV5

2p2P3+ ~ } NAI]

1 1 P2 ~ P~} Ds Pl [1.0NA s --Pl NA4- P{~I --P~ NA3 _ {~ 2p2P3_. P~ N

--{~1 2p4P2 3p~pa p~

P~

1 1 P2N Pa~N NVS=~-6"~I [ 1 . 0 / A6--pl AS--~p3--pZ1J A4 ~f as

{~11 2p4p2 p~ p~+ 3p~p3] N A2 p~ p$ p~ -bY-J /)6 2p2PS 2p3P4 3p~P4 4p~p3
L p~ p~ + p~ p]

+ ~ _ _ __P~ NA 1~. ~_~j3p2P~ .4-

calculated for any set of intervals related by any constant multiplier. For example, Table III lists the coefficients for size intervals whose end points are related by the multiplier, 100.o5. Definition of interval end points by any constant multiplier results in a set of "sliding intersection probabilities" which are invariant for any set of sphere sizes if the largest sphere diameter of the set corresponds to one of the planar intersection diameter interval end points. In order to demonstrate this important point, and to facilitate subsequent discussion, notation will be introduced which is consistent with the original Saltykov development [1], the discussion by Underwood [5] and notation used in particle size analysis [6]. Figure 1 illustrates the notation. It will be important to keep in mind that sphere radii, planar intersection radii, and their respective size intervals are indexed such that the larger index represents the larger radii,

Extensions of the Saltykov Method

Computer TABLE Ill Generated Saltykov Coefficients Based on Size Intervals R e l a t e d B y t h e C o n s t a n t 10 '~ M u l t i p l i e r 0 . 5 2 3 2 0 2 6 5 3 x 1 0 -3 0 . 3 6 7 0 8 7 2 5 7 x 1 0 -3 0 . 2 5 8 1 7 3 6 6 9 10 -3 0 . 1 8 1 9 1 8 3 5 2 10 -z 0 . 1 2 8 3 7 7 8 9 0 10 -3 0 . 9 0 7 0 2 1 6 8 10 -4 0 . 6 4 1 4 3 4 4 3 10 -a 0 . 4 5 3 9 5 2 0 6 1 0 -4 0 . 3 2 1 4 5 8 1 1 10 -4 0 . 2 2 7 7 4 1 8 5 10 -~ 0 . 1 6 1 4 0 7 4 6 10 -~ 0 . 1 1 4 4 2 8 3 3 10 -a 0 . 8 1 1 4 2 1 3 10 -5 0 . 5 7 5 4 9 4 5 10 -5

97

1. 2. 3. 4. 5. 6. 7. 8. 9. 10. 11. 12. 13. 14. 15.

2.20502065610 0.748660468814 0.226080731345 0 . 9 8 3 3 9 7 9 7 7 6 1 10 - t 0 . 5 0 9 4 8 1 7 2 9 9 4 x 10 t 0 . 2 9 1 4 3 4 5 5 4 2 0 x 10 - t 0.17730418945 10 -t 0 . 1 1 2 3 6 8 1 8 1 6 2 10 -x 0 . 7 3 2 6 1 7 7 3 8 6 10 -2 0 . 4 8 7 4 5 6 3 6 4 9 10 -z 0 . 3 2 9 2 1 2 2 7 4 8 10 -2 0 . 2 2 4 8 3 6 0 3 3 3 1 0 -2 0 . 1 5 4 8 5 8 5 5 2 3 1 0 -2 0 . 1 0 7 3 5 5 9 4 9 8 10 -2 0 . 7 4 7 9 9 5 4 3 4 10 -3

16. 17. 18. 19. 20. 21. 22. 23. 24. 25. 26. 27. 28. 29.

60. 0 . 1 3 9 10 -~

SIZE INTERVAL
SPHERE SIZE ~1' SPHERE J PLANAR INTERSECTION T END POINT r{ q_, COMPUTATIONAL INTERVAL k=, INTERSECTION PROBABILITY

~\'

04

I-,

k:2

rj"

i :

k ~ ~ -

Pl(k]= Pal where ~>: = sphere rodiue Pnj

n= 1,2,3,....N

i=j= N= k - k + l

r;
rl~ re.

"
2
i

'
2
i

r;
r~
r~

K-I
K

l = 0,1,2.,3 ....j.., J

i =0,1,2,3,.,. I...I

i=j= K- k+ I " Max. sphere radius

/
f~ l ~\ | p .=pa(k) ./P~ nl . . . . Pn(j_l)= pn(k+ i ) r~=,=~=.;.~.~

.~" "",~q" riLI~ J

~'~/ / k , i J"~! n,l
i L_

isl computational Ist intersection prob

for s p h * ere. ~=j "

ri~
I-2

.'~.\\~" / / ~ / / / / ' / / r",~,\".,\\\~'~l -~/ "/ //i

camp. interval

For Size InJervals Related hy a Constant Multiplier

(~ ~- d ~
FIG. 1. ability.

and r;= d r~

Relations among notation for end point, sphere size, and intersection prob-

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Homer D. Lewis, Kenneth L. Walters, and K. Allan Johnson

while the larger index for intersection probability and computational interval for N v relate to smaller intersection radii and sphere radii. T h e invariance of intersection probabilities for section size intervals related by a constant multiplier can be shown as follows. Let a general set of size interval end points of the planar intersection radii be defined r~ for i = 0, 1, 2 . . . i . . . I. T h e total number of intervals in the set is then I. T h e set of sphere radii, r*, for j = 0, 1, 2 , . . . j . . . J can be defined for the same set of intervals such that i = j. I f the interval end points are specified such that r* = CJr* for C > 1, then r*=y = r~ = C Jr*. Define the nth intersection probability Pn, such that when n = 1 the probability Pl is that for obtaining planar intersections of radii between the sphere radius r* and the next planar intersection interval end point. Then, for any maximum sphere radius in the domain of the set of end points defined by r* < CJr~ < CJr~, the nth intersection probability, Pnj, for rmax = CJr* can be written,
1 '

which is seen to be equivalent to Eq. 5.8 of Ref. 5, p. 113. With simplification,

pn; = [(I -- C-2~) -- (I -- CZ-~")i], (3)

or,
Pnj = PnJ"

This indicates that for all sets of planar intersection intervals whose end points are related by the same constant multiplier, there exists an invariant set of intersection probabilities which can be considered a "sliding" set of probabilities relating the nth intersection probability for a sphere of radius r~=i to the size interval (i -- n + 1, i -- n). Approximation is necessary when using a Saltykov type of analysis dependent upon intersection probabilities determined by the method described above. Although it is not the intent of this discussion to provide a detailed error analysis, the following qualitative comments are offered to illustrate the practical utility of the method. For purposes of data comparisons among many samples, the selection of a standard set of size intervals is advantageous, especially if the comparisons are made among calculated sample distribution statistics such as mean, variance, and skewness. Definition of size interval end points resulting in the set of "sliding intersection probabilities" provides a convenient method of obtaining the particle size distribution based on a standard set of size intervals. In automated image analysis, using a device such as the Quantimet 720, the upper end point of the largest size interval can be set to a certain fraction of the live frame area, equivalent to the area, or diameter, of the largest particle expected in a set of measurements. Errors in the calculated particle size distribution would

Extensions of the Saltykov Method

99

then be dependent upon the accuracy to which the size discriminator settings on the analyser match the calculated end point values, and the accuracy of the match between the largest particle in the sample and the upper bound of one of the size intervals in the set. Errors resulting from significant-figure limitation in end point setting for a given analyser can be eliminated by use of the general method discussed in the next section. Error resulting in mismatch of the size of the largest detected area and an upper end point of the interval representing the first intersection probability might be no greater than the error, existing in the classically exact analysis, resulting from the relatively small probability of having sampled the largest particle. There are several advantages in the use of the above method in automatic image analysis. Definition of a standard set of size intervals permits direct comparisons of calculated particle size distributions. Intersection probabilities, hence the coefficients for calculating Nv(k) need not be calculated for each problem. The largest detected area need only fall in the domain of the set of size intervals.

The General Method

A general computational formula which can be applied to cases in which intersection size interval end points are not related by a constant multiplier and/ or where the particles need be the same shape only within a size interval can be written,
N,(k) D NA(k) -- n>~2[p,~(k -- n + 1) N~(k -- n + 1)] ,

(4)

where Na(k) = the number of planar intersections per unit area observed in the kth computational interval, Nz(k) = the number of observed intersection in the kth interval corrected for intersections from all larger spheres, N , ( k ) = D(k) Nv(k), N~ (h) = the number of spheres per unit volume of the kth computational size interval (recall that for k = 1 the sphere size interval is (if, J - 1) or the largest size interval), D(k) = the sphere diameter corresponding to the upper bound of the kth interval.

Pr,(k) "~- Pn(i=K--k+l) = ~

[(r72 --

r~2n) --

(r~ 2 -- r~-2n+l)]

For example this could be applied in a case where shape may be some function of size such as in fission gas bubbles in fast reactor oxide fuels. Of course, the intersection probabilities must be determined for each shape. Although a preselected set of size intervals can be used to facilitate automated image

100

Homer D. Lewis, Kenneth L. Waiters, and K. Allan Johnson

analysis, a new set of coefficients would necessarily be calculated for each maximum size defined in the domain of the end point set. A computer algorithm for solving Eq. (4) directly would be more convenient than solving for coefficients. For example, the first few terms would be N~(I) = p ~ Nn(2) = ~
1 1

[Na(1)],

Uv(1 ) -- X~(1)
1)0) '

[NA(2) -- p2(1)NB(1)], Nv(2 ) --

N~(2) D(Z) '

NB(3) = P~0) [Na(3) -- Pz(2)Na(2) -- P3(1)N~(i)]' Nv(3) = N~(3) D(3) ' NB(4) = ~ [NA(4) -- p~_(3)N~(3) -- p3(2)NB(2) -- p4(1)N,~(l)], Nv(4 ) = N.(4) 3(4) " The general solution can also be written in terms of the general sphere size interval as, 1 [ n=J-j+l 1 Nvj -- 2r*p. NAj -[Pn(a+n-1) NI~O~-n--1)] ,

n>~22~

(5)

where

Pn(J+l) z O.
Clearly there is somewhat more computational difficulty in application of the general solution which may limit its practicality to those with large, fast, central computor facilities.

Summary and Conclusions

The Saltykov procedure is particularly useful for computer augmented automatic image analysis. Using an algorithm developed on CDC 7600 computers highly accurate sets of coefficients have been calculated using both the classical Saltykov interval endpoint values and one other set of intervals related by a constant multiplier. In addition the algorithm may be used to generate the set of intersection probabilities and coefficients for determination of Nv(k ) for any particle shape for which the general intersection probability is defined, based on any set of size intervals whose endpoints are related by any constant multiplier. The coefficients thus generated can be used to practical advantage in automated image analysis utilizing a fixed set of size intervals. An algorithm was developed for a general solution to the planar intersection area analysis problem in which size interval endpoints need not be related in any particular manner and in which particle shapes may vary if a characteristic shape, i.e. general intersection probability, can be defined for each interval.

Extensions of the Saltykov Method

References

101

1. S. A. Saltykov, T h e determination of the size distribution of particles in an opaque material from a measurement of the size distribution of their sections, Stereology (H. Elias, Ed.) Proc. Second Int. Cong. for Stereology, Springer-Verlag, New York (1967) p. 163. 2. Quantimet 720 Instruction Manual, Imanco, New York (1971) p. 10.1. 3. E. E. Underwood, Particle size distribution, in Quantitative Microscopy, (R. T. DeHoff and F. N. Rhines, Ed.) McGraw-Hill, New York (1968). 4. Ibid. p. 118. 5. E. E. Underwood, Quantitative Stereology, Addison-Wesley, Menlo Park (1970). 6. H. D. Lewis, and A. S. Goldman, Los Alamos Scientific Laboratory Report LA-3656 (1967).

Accepted November 15, 1972