LongTransient Effects in Lasers with Inserted Liquid Samples

J. P. Gordon, R. C. C. Leite, R. S. Moore, S. P. S. Porto, and J. R. Whinnery

Citation: J. Appl. Phys. 36, 3 (1965); doi: 10.1063/1.1713919
View online: http://dx.doi.org/10.1063/1.1713919
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JOURNAL

OF

APPLIED

PHYSICS

VOLUME 36,

NUMBER

JANUARY

1965

Long-Transient Effects in Lasers with Inserted Liquid Samples

J.

P. GORDON,

R. C. C.

LEITE,*

R. S.

MOORE,

S. P. S.

PORTO, AND ].

R.

WHINNERyt

Bell Telephone Laboratories, Incorporated, Murray Hill, New Jersey

(Received 18 May 1964)

Buildup and decay transients were observed when polar or nonpolar liquid cells were placed within the
resonator of a helium-neon laser operating in the red at 6328 A. Similar but smaller effects were also observed with two solids. Time constants were the order of a few seconds for all materials, which suggests a
thermal phenOlnenon, but general heating effects were ruled out by the strong localization of the phenomenon. Transverse motion of the cell by about one beam width caused new transients similar to the initial ones.
It is believed that the effects are caused by absorption of the red light in the material, producing a local
heating in the vicinity of the beam and a lens effect arising from the transverse gradient of refractive index .
.-\bsorptions of 10-3 to 10-4 parts per centimeter are sufficient to produce the effects, and are believed to be
reasonable values for the materials studied. One of the most important applications may in fact be for the
measurement of small absorbancies.
The experiments are described, and analysis of the lens effect from absorption is given. Alternate explanations which were considered are stated briefly.

I. INTRODUCTION

actly, a small reflection remaining at each of the

surfaces.
Liquids included benzene, nitrobenzene, toluene,
carbon disulfide, chloroform, carbon tetrachloride,
pentane, hexadecane, ethylene glycol, and water.
Several different laser tubes were used, different mirrors
and different resonator lengths. A typical arrangement
utilized mirrors with curvature radii of 2 m, with about
1.8 m spacing. The laser beam was usually turned off
and on by a shutter in the position shown in Fig. 1.
Some of the most significant observations follow:

EVERAL interesting phenomena were observed

S
when cells containing polar or nonpolar liquids were
placed within the resonator of a helium-neon laser
operating at 6328 A. The effects induded buildup and
decay transients, mode changes, and relaxation oscillations, all with time constants of the order of seconds.
The observed phonomena are described in more
detail, with a simple analysis of the proposed explanation. It appears that the basic phenomenon is a lens
effect in the liquid cell produced by local heating along
the beam, with a corresponding change of index of
refraction in the vicinity of the beam. Absorption of
about 10-3 to 10-4 parts per centimeter would produce
the effects described. Absorptions of this order might be
explainable by the tail of the high ultra violet absorption
common to these materials, although other small loss
mechanisms are undoubtedly present. Smaller but
similar effects were observed in certain solids.
The phenomena are important to anticipate when
materials of this class are inserted in the feedback path
of a laser. It is believed that they may also provide a
very sensitive way of measuring small absorbancies of
materials. The method is currently being applied to the
study of such losses, with results to be published when
available.

1. In almost every case there was a buildup of power

from the initial va.lue to a maximum, followed by a
decay to a value lower than the initial value. Time
constants for both parts were the order of seconds. A
typical photograph is shown in Fig. 2. (Figure 3 shows
a case in which mode changes occurred during the
transient. )
2. In some cases the buildup transient was not
observed, but only the decay transient, apparently
depending upon how the resonator was tuned. However,
retuning did not bring the lower steady-state value up
to the maximum power of the transient.
3. If the laser was turned off by interrupting the
beam, it required a time comparable with that of the
"turn-on" transient (say 8 to 10 sec) for the liquid to
recover. That is, if the shutter was opened at a shorter
time than the above after the turn off, smaller transient
effects were observed.

II. EXPERIMENTS

The setup, designed for the study of Raman spectra

in liquids, is sketched in Fig. 1. A cell 1 cm long with
optical fiats on the sides contains the liquid, and is
placed between the tube containing the helium-neon
mixture, and one mirror of the laser. The cell is adjusted
by means of a mount to the approximate Brewster
angle, usually by maximizing the power of the laser. The
condition for zero reflection cannot be obtained ex-

PMl A

M"l 11

LC

__

12 M.. 2

Qiq--~stt-D +,-_L_T_fC--~-+Q
OSC

PMZD-OSC
PM =PHOTOMUlTIPliERS
A APERTURES
m = PARTIAl REFlECTION
MIRROR

* On leave of absence from the Instituto Tecnologico de Aeronautica, Brazil.

t On leave of absence from the University of California at

Berkeley.

M=MIRRORS
1 = IRIS
S=SHUTTER
LT = lASER TUBe
LC = liQUID CEll
MO=POWER MONITOR

FIG. 1. Schematic of the experimental arrangement.

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GORDON et at.

FIG. 2. Transients on the power density at the center of the beam

(upper trace) and total power output (lower trace). The similarity
bet~een the two. traces s~ggests tha! no mode change took place
durmg the traJ?-s~ent. !hls was obtamed .by manipulation of Iris
# 1 thus obtammg smgle mode operatIOn. (Time scale is 0.5
sec/div).

4. A movement of the cell in a direction perpendicular

to the beam after the laser had reached steady operation made the transient reappear just as if the shutter
had been opened again. The displacement required was
very small, of the order of one spot width (i.e., 1 mm).
5. Sometimes the transients described were followed
by oscillations in power; this was generally at very low
power outputs. Observation of the beam usually showed
mode changes associated with these transients with
. periods of fluctuation between 0.1 and 10 sec.
'
time
6. When the laser was oscillating near its threshold.
still other phenomena occurred. At times the oscillating
mode would shift among several forms at intervals of
the order of seconds. Under similar conditions the laser
apparently stopped oscillating periodically, starting
again after a few seconds. By suitably altering the
apertures after the laser was on, it was possible to either
turn it off so that it came back on after a few seconds
. on, but in such a state that if the beam was'
or remamed
interrupted, the laser remained off after the interruption
was removed. All of these effects indicate that the liquid
cell altered the properties of the laser resonator when
the beam was on.

FIG. 3. Transients on the power density at center of the beam

.(uPl?er trace) a!ld total power output (lower trace) for the system
In Fig. 1. Th~ difference between the two traces discloses the mode
changes dunJ?-g ~e transients. This was obtained by making
aperture A With diameter one tenth of beam width. (Time scale
is 1 sec/div).

. 7. Glass ~lates slanted at the Brewster angle were

mtroduced m the path at various points to eliminate
~ossible o~cillati.ons in the infrared region, and especIally the hIgh-gam 3.39-~ line. Aside from slight diminutions of power explainable by the slight reflection from
~he pla:es,. these changed nothing, so the effects arising
m the bqUId seem caused by the red line itself.
8. Observation of the diameter of the laser beam
showed that it was smaller at the mirror on the cell
side than on the opposite mirror. With the cell removed
the two beam spots were about the same. This sup~
ported the thought that the effect was a lens effect in
the cell. Utilizing resonator theory, it was estimated
from path lengths and spot sizes that the cell acted as a
diverging lens with focal length about equal to that of
the mirrors (i.e., 1 m).
9. A suggestion to apply a dc field of about the same
strength as the field at the light frequency was :first
t~ied with two wire electrodes within the cell. ApplicatIOn of the field provoked new transient effects and in
one cell with a large number of dust particle~, these
were strongly agitated by the application of the :field.
However, when the :field was applied by placing wires
or plates outside the cell, there was no noticeable effect
of the dc :field. Thus there was probably some charging
of the dust particles when the wires were within the
cell, an effect which has been observed with the inhomogeneous :fields used for separation of material particles.!
10. Careful observation of the drift of observable
particles through the beam, even with relatively dustfree samples, showed drift usually upward, independent
of the polarization direction of the beam. The rate of
movement was different for different liquids, but generally was about one beam width within :five seconds and
does indicate some slight convection. Repetition ~f the
experiment of cell displacement (4, above) with vertical
displacement of the cell showed essentially the same
effects as with horizontal displacement. In both cases the
beam appeared elongated in the direction of motion
somewhat more so in the case of vertical displacement~
Thus the convection appears to produce a slight modification, but not to be the essence of the matter.
11. Experiments were made with the entire cell
heated, and then allowed to cool. Temperatures were
mea~~red by a thermocouple in the top of the cell.
sensItive enough to show normal fluctuations in temperature which were around 0.1 C. It required temperature differences of 3 or 4C from the tuned state to
reduce power by amounts comparable to the transient
changes being studied. Temperature changes from the
laser beam itself (;QuId not be measured, so were less
than the normal fluctuations of about 0.1.
~2. Th~ effect was observed to a lesser degree in two
solIds, lucIte and a glass of unknown composition. Solids
with small absorption (judged by the strength of maser
I

H. A. Poh!, Sci. Am. 203, 107 (1960).

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LONG-TRANSIENT

EFFECTS

IN

LASERS

oscillation) yielded no such effect. Those with too large

absorptions prevented lasing.
III. EXPLANATION BASED UPON A LENS
EFFECT FROM HEATING

As stated in the introduction, we believe that a lens

effect is produced by a change in dielectric constant
near the beam, similar to that predicted for proposed
liquid lasers.2 It is also believed that the heating to
produce the required gradients comes from absorption
of the red light in the material within the cell. An
approximate model of this effect will be presented.
Imagine that the index of refraction changes with
radius about the beam center as sketched in Fig. 4.
The beam intensity is Gaussian in the dominant mode,
and one might expect the variation of n to be approximately of that form, especially in the early part of the
transient. However, for simplicity we consider here the
change as parabolic in radius, which matches the center
portion of the variation reasonably, as is shown. Thus
let
(1)
where Wo in the spot size, or spot radius, of the beam
(see Appendix A).
A ray entering parallel to the axis will follow a circular
path with radius of curvature3 given by
l/R= -aT' vln n= (l/n)dn/dr= -20r/wo2

(2)

The unit vector aT is in the outward radial direction.

Assuming the cell thickness to be small compared with
its focal length, the latter is found from Fig. 4 to be
F=r/O=rR/l= - (1/20)wNl.

(3)

The experiments of Sec. II gave an estimated focal

length of 1 meter. Thus with wo=O.l cm, l= 1 cm, the
fractional change in n from center to beam edge is
0= -wN2IF= - (0. 1)2j2 X lX (-100) =5X 10-5 , (4)

or with n= 1.5, the total on would be 7.5X 10-5 Thus

only a very small change in index of refraction need
be obtained to explain the effects observed.
Several mechanisms for changing the index of refraction are discussed in Sec. V, but let us consider here
that of simple heating by absorption of light energy.
Since the contribution to index of refraction from permanent dipole moments should be negligible at visible
frequencies, the temperature effect for both polar and
nonpolar liquids should be primarily that from the
change in density of molecules contributing to polarization. This yields a dn/dT of the order of (-10-3).
(For example, the value for carbon disulfide at 20C
is found 4 as -0.794Xl()-3.) Thus a change in index of
H. Winston and R. Gudmundsen, Appl. Opt. 3, 143 (1964).
3 M. Born and E. Wolf, Principles of Optics (Pergamon Press
Ltd., Oxford, England, 1959), p. 123.
4 Handbook
of Chemistry and Physics (Chemical Rubber
Publishing Company, Cleveland, Ohio, 1959), 41st ed., p. 2935.

~--1.--~
FIG. 4. Sketch for obtairung lens focal length.

refraction from beam center to beam edge of 7.5 X 10-5

requires a temperature change of only about 0.075.
As is seen, this may be explained by an absorption of
from 10--a to lQ-4 parts per centimeter.
Appendix A gives the temperature distribution as a
function of radius and time when the source of heat is a
Gaussian beam of characteristic radius Wo, established
at time zero. Figure 5 shows the plots versus ,-/wo for
different values of t/te, where te is a characteristic time
defined as
(5)
where D=k/pcp ; k=thermal conductivity, calories per
(cmsecoK); p=density, g/cm3 ; cp=specific heat,
calories/ (g. OK).
(6)
The dashed curve in Fig. 5 is the steady-state solution
for a bounded region with temperature constant at
r=a. The radius a of the cell is 0.5 cm, and Wo is estimated at about 0.5, mm, so a= l(}-dJo. The solid curves
for finite time are derived for the source in an infinite
medium. The finite boundary condition would not
change these curves perceptibly, however, since they
decrease to negligible values before the external radius
of 10 Wo is reached.

\
'\
PARABOLIC APPROXIMATION
'k----IN VICINITY OF AXIS

\\

\"

STEADY-STATE CURVE FOR

AT r =10

'("-- t.T=O
,

t/tc=',
24.5'\

' .......

....................
6

............
8

10

FIG. 5. Radial temperature distribution for a Gaussian beam in

infinite medium. Also steady-state distribution for finite boundary
condition. Parameters defined in the text.

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GORDON

The curves of Fig. 5 show several important points.

The first is that for all values of time, temperature drops
off very rapidly outside the beam. For small times, the
temperature distribution is essentially the Gaussian loss
distribution as expected, but even in the steady state
the temperature at 2wo is less than half that at the
center. Observation 4 of Sec. II is consistent with this
strong localization of excess temperature, and observation 11 is explainable by the localization and the small
temperature changes.
A second point shown by the curves is that a parabolic approximation holds fairly well up to r=wo. Since
87% of the light energy is concentrated within this
radius, the resulting lens should have little spherical
aberration, and Eq. (1) should give a good approximation to its focal length. For a temperature rise !::.T, the
corresponding index of refraction is
n(r,t)

no+ (dnj dT)!::'T(r,t) ;

thus using the parabolic approximation (A13) from

Appendix A,
dn)0.06bP
n(r,t)=no+ ( --dT
'Irk
(7)

Since dnjdT is small, the first term in the brackets

adds only a negligible part to the r-independent nand
can be dropped. Equation (7) is then of the form (1)
with
(j= -

0.12bP(dn) 8Dt
n ok7r dT wo2 +8Dt'

Foo [ 1+ 2t '

(9)

where
F co = k1rnowNO.24bPI(dnjdT).

(10)

Figure 6 shows a plot of focal length versus time, and

it is seen that it approaches the asymptote F in only
a few times
(i.e., in a few seconds) even though it
takes much longer for the temperature distributions of
Fig. 5 to approach the steady state. Thus an effect based
upon varying focal length is consistent with the buildup times of 2 to 8 sec observed.
The equation of Fco in (10) allows calculation of the
absorption b if F is known. With the following estimates, F=-l m, P=0.8 W, wo=0.05 em, dnjdT
=-10-3, no=1.5, 1=1 em,
and k=4X1Q-4,
b=7rnokwNO.24FPI (dn/dT) =2.5X lQ-4 em-I.
Considering the estimates, the expected range of
b would be 10-3 to lQ-4. In looking at absorption mecha-

te

-------~~==~------~
~~--~----~2----~3----~4----~5

FIG. 6. Focal length vs time curve.

nisms to explain this, the absorption accompanying

Raman scattering is estimated at 10-12 jcm, so is much
too low. Some absorption from impurities in the
liquids could be imagined, but tests were duplicated
over a fair range of impurity. The breaking of molecular
clusters 5,6 is a possibility, but values for this are not
known. Most likely is the tail of the strong ultraviolet
absorption which is about the same for all liquids tested
except water. Water has an ultraviolet absorption edge
at shorter wavelengths, and, consistent with this,
showed smaller transients.
It was most interesting that the time constants of the
observed transients vary so little for the different materials tested. This also may be understood from the
characteristic time defined by (5), which is the basic
parameter in heat buildup (Fig. 5) and the lens effect
(Fig. 6). Theoretical values for several materials are
shown on Table F and it is seen that they are remarkably grouped around 2 or 3 seconds.
IV. POWER CHANGES PRODUCED BY THE
LENS EFFECT

te]

0.24bPl(dn/dT) (8Dt)

6~-----------------------'

(8)

The focal length, from (3) is then

F(t)

et at.

<>0

The discussion has so far concentrated on the lens

effect from localized absorption and heating. Time constants and localization in space have seemed consistent
with the observations. It is clear in a general way how
a varying lens introduced in the oscillator path can
cause power changes, but this should be examined in
somewhat more detail.
Referring to Fig. 1, it appeared that the finallimitation in power was by the size of beam at aperture # 2,
which is the tube end, and is 4 mm in diameter. The
size of the spot on mirror # 2 was consistent with this.
The lens produced by the liquid cell and mirror # 1 can
roughly be considered together as a plane reflector. Thus
it is believed that the limiting power is that in which
the lens focal length just adjusts so that diffraction
losses at aperture # 2 equal the laser gain. This is of
5 J. Frenkel, Kinetic Theory of Liquids (Oxford University Press
'
Oxford, England, 1946), p. 302 et seq.
6 H. S. Green, The Molecular Theory of Fluids (North-Holland
Publishing Company, Amsterdam, 1952), p. 64 et seq
7 Ref. 4, p. 2439.
.

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LO~G-TRANSIENT

EFFECTS IN

TABLE I. Thermal constants and calculated values of te. (k = thermal conductivity, p=density, cp=specific heat, te=characteristic
time.)

Material

(Ref. 7)

cp

te (for
wQ=1 mm),
sec

chloroform
benzene
nitrobenzene
toluene
carbon tet.
pentane
hexadecane
ethylene glyc.
water
Lucite

2.9
3.8
3.9
3.8
2.5
3.2
3.2(?)
6.2
14
5

0.226
0.406
0.339
0.39
0.201
0.527
0.496
0.57 (?)
1
0.35

1.49
0.88
1.20
0.87
1.59
0.626
0.775
1.115
1
1.18

2.9
2.35
2.61
2.23
3.19
2.58
3.0
2.56
1.78
2.06

kX10 4

course complicated slightly by the different volume of

active material included as the path changes.

the heat generated per unit length will be proportional

to the square of this,
Q(r)=A exp(-2r2/wo2) cal/(cmsec).

APPENDIX A. HEATING AND FOCUSING EFFECT

OF GAUSSIAN LASER BEAM

If field of the laser beam has the Gaussian form of

the principal mode,9
E(r) = Eo exp( -r2/wo2)
8
9

Ref. 6, Chap. TV.

A. Yariv and']. P. Gordon, Proc. IEEE 51, 4 (1963).

(AI)

Carslaw and Jaeger lO give the temperature at radius

r and time t from a unit heat source at radius r', time
zero, in an infinite medium as
(A2)

where D is as in (6) of the text. Thus temperature distribution for the distributed source is
I::.T (r,t) =

1"'11

=~

V. OTHER PHENOMENA CONSIDERED

Until the extremely sensitive behavior of the laser

to thermal gradients was apparent, other mechanisms
were sought to explain the described experiments. In
one model the nonlinear effects tending to orient the
induced and permanent dipole moments were analyzed.
This effect is similar to that of the inverted pendulum.
Calculated time constants from this orienting force in
the presence of thermal effects were about the same as
the normal relaxation times (10-12 sec). The displacement of dipoles in the inhomogeneous optical fields was
also calculated. Transverse gradients appeared too small
to be effective, and longitudinal gradients arising from
the standing wave pattern would not be expected to
remain stable in position within one half wavelength
(0.3/-L).
In considering thermal effects, convection was considered together with conduction. A very crude model
was set up in which the calculated temperature change
was used to find the corresponding change in density.
This, with the gravitational constant, gave the upward
force on a small volume. The motion from this force
could be calculated either from the viscosity and
Stokes' law, or the mobility constant for the material,
which are of course related. 8 The velocities calculated
were about 0.03 em/sec, which is in the range observed.
It is thus believed that heating in the amounts calculated in Sec. III can explain the observed convection
motion; but that this plays only a secondary role. For
example, it may explain observation 10 of Sec. II concerning the slight difference between vertical and horizontal motion of the cel1.

LASERS

2k

27T"r'Q(r')G (r,r',t')dt' dr'

fl exp( -r2/4Dtl)dtll'" r'

t'

The second integral in (A3) may be evaluated by

Eq. 13.3 (1) of Watson,n
(A4)

This integral is valid for unrestricted complex a

and Iarg pi < 7T"/ 4. Thus in applying to (A3),

jr
a=-

2Dt"

f=

[ 2

1 ]
-+4Dt' .
U'o2

(AS)

This integral is simplified by the substitution

y= (wo2+8Dt' )-1

giving
(A6)

This form has solutions

in tegrals. 12

AW02{ (2r2)

111

terms of exponential

2r2)} .

I::.T(r,t)=-- Ei - - -Ei 8k
wo2
8Dt+wo2

(A7)

10 H. S. Carslaw and J. C. Jaeger, Operational JfethodsinApplied

Mathematics (Dover Publications, Inc., New York, 1963), p. 109.
11 G. N. Watson, Bessel Functions (The Macmillan Company,
New York, 1948), 2nd ed., p. 393.
12 E. Jahnke and F. Emde, Tables of Functions (Teubner,
Berlin, 1938), pp. 1-8.

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GORDON et at.

Curves from this equation are plotted in Fig. 5 vs

r/wo for various tlte, where te is defined by (5) and is
around 2 sec for the materials studied.
The infinite model has the weakness that !:J.T ~ 00
as t ~ 00. This is because the gradient approaches 1/r
in the steady state, and with !:J.T=O at r= 00, temperature integrates to infinity at all finite radii. Reference
10, Sec. 55, gives the corresponding Green's function
for a source in a medium of finite radius, but we were
not successful in carrying out the integrations of this
form. In view of the localization of temperature, it
does not seem very important, but it is useful to have
the steady-state curve for the finite cylinder. The
following equation will give the steady-state heat conduction at r from the sources within.
dt
- k21rr-=
dr

Jr 21rY'A exp(-2r'2)
- - dr',

timeter per second] and by b, the fractional dissipation

per centimeter.
Q(r)=0.Z4bw(r).
Total beam power is
P=

fa 21rrA ( -2r2)
a
- dr
fo 21rrw(r)dr = --exp
O.24b
wo

= 1I'A

W
02[1_exp(_ -2a2)J"",,~AWo2
wo2

O.48b

(AIO)

O.4Sb

or
(All)
This may be substituted in (A7) and (A9)
For small values of r, the following series12 is ~useful,
Ei( -x) =1njtx-x+ (x2/4) ...

wo

(AIZ)

'Y= 1.7S1.

Using the above in (A7) and substituting (All), we

have for temperature near the axis,
This may be integrated again [the second term
utilizing 31Z(5d) of Ref. 13J. The result, with boundary
condition !:J.T=O at r=a is

2
AW02[ Ei (Zr2)
rJ
!:J.T(r)=- - -Ei (za
--- )-21n-.
Sk

wo2

wo2

(A9)

0.06bP[ (
SDt)
16Dt r2 ]
In 1+. (A13)
2
k
wo
wo2+SDt wo2

tJ.T(r,t)~--

Similarly for the steady-state solution of the bounded

region,

O.06bP[

tJ.T(r)~--

The curve for this steady state is shown dashed in

Fig. 5.
The constant A may be related to total power and
the rate of dissipation. The heat density of (Al) is
the power density in watts per square centimeter multiplied by 0.24 [to convert to calories per square cen-

(z'Ya

2r2]
)
In -- .
wo2
wo2

(A14)

The last equation is plotted as a dotted curve in

Fig. 5, and is seen to be a good approximation up to
r/wo approaching unity.
13 W. Grobner and N. Hofreiter, Integraltafel (Springer-Verlag,
Berlin, 1949).

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