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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


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JOURNAL OF APPLIED PHYSICS VOLUME 36, NUMBER 1 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 ob-
served 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 phenome-
non. 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 explana-
tions which were considered are stated briefly.

I. INTRODUCTION actly, a small reflection remaining at each of the


EVERAL interesting phenomena were observed surfaces.
S when cells containing polar or nonpolar liquids were
placed within the resonator of a helium-neon laser
Liquids included benzene, nitrobenzene, toluene,
carbon disulfide, chloroform, carbon tetrachloride,
operating at 6328 A. The effects induded buildup and pentane, hexadecane, ethylene glycol, and water.
decay transients, mode changes, and relaxation oscil- Several different laser tubes were used, different mirrors
lations, all with time constants of the order of seconds. and different resonator lengths. A typical arrangement
The observed phonomena are described in more utilized mirrors with curvature radii of 2 m, with about
detail, with a simple analysis of the proposed explana- 1.8 m spacing. The laser beam was usually turned off
tion. It appears that the basic phenomenon is a lens and on by a shutter in the position shown in Fig. 1.
effect in the liquid cell produced by local heating along Some of the most significant observations follow:
the beam, with a corresponding change of index of 1. In almost every case there was a buildup of power
refraction in the vicinity of the beam. Absorption of from the initial va.lue to a maximum, followed by a
about 10-3 to 10-4 parts per centimeter would produce decay to a value lower than the initial value. Time
the effects described. Absorptions of this order might be constants for both parts were the order of seconds. A
explainable by the tail of the high ultra violet absorption typical photograph is shown in Fig. 2. (Figure 3 shows
common to these materials, although other small loss a case in which mode changes occurred during the
mechanisms are undoubtedly present. Smaller but transient. )
similar effects were observed in certain solids. 2. In some cases the buildup transient was not
The phenomena are important to anticipate when observed, but only the decay transient, apparently
materials of this class are inserted in the feedback path depending upon how the resonator was tuned. However,
of a laser. It is believed that they may also provide a retuning did not bring the lower steady-state value up
very sensitive way of measuring small absorbancies of to the maximum power of the transient.
materials. The method is currently being applied to the 3. If the laser was turned off by interrupting the
study of such losses, with results to be published when beam, it required a time comparable with that of the
available. "turn-on" transient (say 8 to 10 sec) for the liquid to
II. EXPERIMENTS recover. That is, if the shutter was opened at a shorter
time than the above after the turn off, smaller transient
The setup, designed for the study of Raman spectra effects were observed.
in liquids, is sketched in Fig. 1. A cell 1 cm long with
optical fiats on the sides contains the liquid, and is
__
PMl A M"l 11 LC 12 M.. 2

placed between the tube containing the helium-neon Qiq--~stt-D +,-_L_T_fC--~-+Q


mixture, and one mirror of the laser. The cell is adjusted OSC I
by means of a mount to the approximate Brewster I
M=MIRRORS
1 = IRIS
angle, usually by maximizing the power of the laser. The PMZD-OSC
S=SHUTTER
condition for zero reflection cannot be obtained ex- LT = lASER TUBe
PM =PHOTOMUlTIPliERS LC = liQUID CEll
* On leave of absence from the Instituto Tecnologico de Aero- =
A APERTURES MO=POWER MONITOR
nautica, Brazil. m = PARTIAl REFlECTION
MIRROR
t On leave of absence from the University of California at
Berkeley. FIG. 1. Schematic of the experimental arrangement.
3

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4 GORDON et at.

. 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 espec-
Ially the hIgh-gam 3.39-~ line. Aside from slight diminu-
tions 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
FIG. 2. Transients on the power density at the center of the beam the cell. Utilizing resonator theory, it was estimated
(upper trace) and total power output (lower trace). The similarity
bet~een the two. traces s~ggests tha! no mode change took place from path lengths and spot sizes that the cell acted as a
durmg the traJ?-s~ent. !hls was obtamed .by manipulation of Iris diverging lens with focal length about equal to that of
# 1 thus obtammg smgle mode operatIOn. (Time scale is 0.5 the mirrors (i.e., 1 m).
sec/div).
9. A suggestion to apply a dc field of about the same
strength as the field at the light frequency was :first
4. A movement of the cell in a direction perpendicular
t~ied with two wire electrodes within the cell. Applica-
to the beam after the laser had reached steady opera-
tIOn of the field provoked new transient effects and in
one cell with a large number of dust particle~, these
tion made the transient reappear just as if the shutter
had been opened again. The displacement required was
were strongly agitated by the application of the :field.
very small, of the order of one spot width (i.e., 1 mm).
However, when the :field was applied by placing wires
5. Sometimes the transients described were followed
or plates outside the cell, there was no noticeable effect
by oscillations in power; this was generally at very low
of the dc :field. Thus there was probably some charging
power outputs. Observation of the beam usually showed
of the dust particles when the wires were within the
mode changes associated with these transients with
. periods of fluctuation between 0.1 and 10 sec.
time ' cell, an effect which has been observed with the inhomo-
geneous :fields used for separation of material particles.!
6. When the laser was oscillating near its threshold.
10. Careful observation of the drift of observable
still other phenomena occurred. At times the oscillating
particles through the beam, even with relatively dust-
mode would shift among several forms at intervals of
free samples, showed drift usually upward, independent
the order of seconds. Under similar conditions the laser
of the polarization direction of the beam. The rate of
apparently stopped oscillating periodically, starting
movement was different for different liquids, but gener-
again after a few seconds. By suitably altering the
ally was about one beam width within :five seconds and
apertures after the laser was on, it was possible to either
does indicate some slight convection. Repetition ~f the
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
experiment of cell displacement (4, above) with vertical
displacement of the cell showed essentially the same
interrupted, the laser remained off after the interruption
effects as with horizontal displacement. In both cases the
was removed. All of these effects indicate that the liquid
beam appeared elongated in the direction of motion
cell altered the properties of the laser resonator when
somewhat more so in the case of vertical displacement~
the beam was on.
Thus the convection appears to produce a slight modifi-
cation, 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 tem-
perature which were around 0.1 C. It required tempera-
ture 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
FIG. 3. Transients on the power density at center of the beam solIds, lucIte and a glass of unknown composition. Solids
.(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 with small absorption (judged by the strength of maser
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). I H. A. Poh!, Sci. Am. 203, 107 (1960).

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LONG-TRANSIENT EFFECTS IN LASERS 5

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 ~--1.--~
radius about the beam center as sketched in Fig. 4.
The beam intensity is Gaussian in the dominant mode, FIG. 4. Sketch for obtairung lens focal length.
and one might expect the variation of n to be approxi-
mately of that form, especially in the early part of the refraction from beam center to beam edge of 7.5 X 10-5
transient. However, for simplicity we consider here the requires a temperature change of only about 0.075.
change as parabolic in radius, which matches the center As is seen, this may be explained by an absorption of
portion of the variation reasonably, as is shown. Thus from 10--a to lQ-4 parts per centimeter.
let Appendix A gives the temperature distribution as a
(1) function of radius and time when the source of heat is a
where Wo in the spot size, or spot radius, of the beam Gaussian beam of characteristic radius Wo, established
(see Appendix A). at time zero. Figure 5 shows the plots versus ,-/wo for
A ray entering parallel to the axis will follow a circular different values of t/te, where te is a characteristic time
path with radius of curvature3 given by defined as
(5)
l/R= -aT' vln n= (l/n)dn/dr= -20r/wo2 (2)
where D=k/pcp ; k=thermal conductivity, calories per
The unit vector aT is in the outward radial direction. (cmsecoK); p=density, g/cm3 ; cp=specific heat,
Assuming the cell thickness to be small compared with calories/ (g. OK). (6)
its focal length, the latter is found from Fig. 4 to be
The dashed curve in Fig. 5 is the steady-state solution
F=r/O=rR/l= - (1/20)wNl. (3) for a bounded region with temperature constant at
The experiments of Sec. II gave an estimated focal r=a. The radius a of the cell is 0.5 cm, and Wo is esti-
length of 1 meter. Thus with wo=O.l cm, l= 1 cm, the mated at about 0.5, mm, so a= l(}-dJo. The solid curves
fractional change in n from center to beam edge is for finite time are derived for the source in an infinite
medium. The finite boundary condition would not
0= -wN2IF= - (0. 1)2j2 X lX (-100) =5X 10-5 , (4) change these curves perceptibly, however, since they
decrease to negligible values before the external radius
or with n= 1.5, the total on would be 7.5X 10-5 Thus
of 10 Wo is reached.
only a very small change in index of refraction need
be obtained to explain the effects observed.
Several mechanisms for changing the index of re-
fraction are discussed in Sec. V, but let us consider here \
that of simple heating by absorption of light energy. ~ \
'\ PARABOLIC APPROXIMATION
Since the contribution to index of refraction from per- 'k----IN VICINITY OF AXIS

manent dipole moments should be negligible at visible \\


frequencies, the temperature effect for both polar and \" STEADY-STATE CURVE FOR
AT r =10 w
nonpolar liquids should be primarily that from the
change in density of molecules contributing to polar-
,
,
'("-- t.T=O
0

t/tc=',
ization. This yields a dn/dT of the order of (-10-3). 24.5'\ ' .......
(For example, the value for carbon disulfide at 20C \ ....................
is found 4 as -0.794Xl()-3.) Thus a change in index of
............
6 7 8 9 10

2H. 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. FIG. 5. Radial temperature distribution for a Gaussian beam in
4 Handbook of Chemistry and Physics (Chemical Rubber infinite medium. Also steady-state distribution for finite boundary
Publishing Company, Cleveland, Ohio, 1959), 41st ed., p. 2935. condition. Parameters defined in the text.

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6 GORDON et at.

6~-----------------------'
The curves of Fig. 5 show several important points.
The first is that for all values of time, temperature drops 5
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
2
strong localization of excess temperature, and observa-
tion 11 is explainable by the localization and the small -------~~==~------~
temperature changes.
A second point shown by the curves is that a para- ~~--~----~2----~3----~4----~5
bolic approximation holds fairly well up to r=wo. Since
87% of the light energy is concentrated within this
FIG. 6. Focal length vs time curve.
radius, the resulting lens should have little spherical
aberration, and Eq. (1) should give a good approxima-
tion to its focal length. For a temperature rise !::.T, the nisms to explain this, the absorption accompanying
corresponding index of refraction is Raman scattering is estimated at 10-12 jcm, so is much
too low. Some absorption from impurities in the
n(r,t) no+ (dnj dT)!::'T(r,t) ; liquids could be imagined, but tests were duplicated
over a fair range of impurity. The breaking of molecular
thus using the parabolic approximation (A13) from clusters 5,6 is a possibility, but values for this are not
Appendix A, known. Most likely is the tail of the strong ultraviolet
absorption which is about the same for all liquids tested
dn)0.06bP
n(r,t)=no+ ( - --- except water. Water has an ultraviolet absorption edge
dT 'Irk at shorter wavelengths, and, consistent with this,
showed smaller transients.
(7) It was most interesting that the time constants of the
observed transients vary so little for the different ma-
terials tested. This also may be understood from the
Since dnjdT is small, the first term in the brackets characteristic time defined by (5), which is the basic
adds only a negligible part to the r-independent nand parameter in heat buildup (Fig. 5) and the lens effect
can be dropped. Equation (7) is then of the form (1) (Fig. 6). Theoretical values for several materials are
with shown on Table F and it is seen that they are re-
0.12bP(dn) 8Dt markably grouped around 2 or 3 seconds.
(8)
(j= - n ok7r dT wo2 +8Dt'
IV. POWER CHANGES PRODUCED BY THE
LENS EFFECT
The focal length, from (3) is then
The discussion has so far concentrated on the lens
te] effect from localized absorption and heating. Time con-
F(t)
0.24bPl(dn/dT) (8Dt)
Foo [ 1+ 2t ' (9)
stants and localization in space have seemed consistent
where with the observations. It is clear in a general way how
a varying lens introduced in the oscillator path can
F co = k1rnowNO.24bPI(dnjdT). (10) cause power changes, but this should be examined in
Figure 6 shows a plot of focal length versus time, and somewhat more detail.
it is seen that it approaches the asymptote F in only <>0
Referring to Fig. 1, it appeared that the finallimita-
a few times te
(i.e., in a few seconds) even though it tion in power was by the size of beam at aperture # 2,
takes much longer for the temperature distributions of which is the tube end, and is 4 mm in diameter. The
Fig. 5 to approach the steady state. Thus an effect based size of the spot on mirror # 2 was consistent with this.
upon varying focal length is consistent with the build- The lens produced by the liquid cell and mirror # 1 can
up times of 2 to 8 sec observed. roughly be considered together as a plane reflector. Thus
The equation of Fco in (10) allows calculation of the it is believed that the limiting power is that in which
absorption b if F is known. With the following esti- the lens focal length just adjusts so that diffraction
mates, F=-l m, P=0.8 W, wo=0.05 em, dnjdT losses at aperture # 2 equal the laser gain. This is of
=-10-3, no=1.5, 1=1 em, and k=4X1Q-4, 5 J. Frenkel, Kinetic Theory of Liquids (Oxford University Press
b=7rnokwNO.24FPI (dn/dT) =2.5X lQ-4 em-I. Oxford, England, 1946), p. 302 et seq. '
6 H. S. Green, The Molecular Theory of Fluids (North-Holland
Considering the estimates, the expected range of Publishing Company, Amsterdam, 1952), p. 64 et seq
b would be 10-3 to lQ-4. In looking at absorption mecha- 7 Ref. 4, p. 2439. .

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LO~G-TRANSIENT EFFECTS IN LASERS 7

TABLE I. Thermal constants and calculated values of te. (k = ther- the heat generated per unit length will be proportional
mal conductivity, p=density, cp=specific heat, te=characteristic
time.) to the square of this,

te (for Q(r)=A exp(-2r2/wo2) cal/(cmsec). (AI)


kX10 4 wQ=1 mm),
Material (Ref. 7) cp p sec Carslaw and Jaeger lO give the temperature at radius
chloroform 2.9 0.226 1.49 2.9 r and time t from a unit heat source at radius r', time
benzene 3.8 0.406 0.88 2.35 zero, in an infinite medium as
nitrobenzene 3.9 0.339 1.20 2.61
toluene 3.8 0.39 0.87 2.23
carbon tet. 2.5 0.201 1.59 3.19 (A2)
pentane 3.2 0.527 0.626 2.58
hexadecane 3.2(?) 0.496 0.775 3.0
ethylene glyc. 6.2 0.57 (?) 1.115 2.56
water 14 1 1 1.78 where D is as in (6) of the text. Thus temperature dis-
Lucite 5 0.35 1.18 2.06 tribution for the distributed source is

course complicated slightly by the different volume of


active material included as the path changes.
I::.T (r,t) = 1"'11 27T"r'Q(r')G (r,r',t')dt' dr'

V. OTHER PHENOMENA CONSIDERED =~ fl exp( -r2/4Dtl)dtll'" r'


Until the extremely sensitive behavior of the laser 2k 0 t' 0
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. The second integral in (A3) may be evaluated by
Calculated time constants from this orienting force in Eq. 13.3 (1) of Watson,n
the presence of thermal effects were about the same as
the normal relaxation times (10-12 sec). The displace-
ment of dipoles in the inhomogeneous optical fields was (A4)
also calculated. Transverse gradients appeared too small
to be effective, and longitudinal gradients arising from This integral is valid for unrestricted complex a
the standing wave pattern would not be expected to and Iarg pi < 7T"/ 4. Thus in applying to (A3),
remain stable in position within one half wavelength
(0.3/-L). jr [ 2 1 ]
In considering thermal effects, convection was con- a=-
2Dt"
f= -+-
4Dt' .
U'o2
sidered 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.
(AS)
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 This integral is simplified by the substitution
Stokes' law, or the mobility constant for the material,
which are of course related. 8 The velocities calculated y= (wo2+8Dt' )-1
were about 0.03 em/sec, which is in the range observed. giving
It is thus believed that heating in the amounts calcu-
lated in Sec. III can explain the observed convection (A6)
motion; but that this plays only a secondary role. For
example, it may explain observation 10 of Sec. II con- This form has solutions 111 terms of exponential
cerning the slight difference between vertical and hori- in tegrals. 12
zontal motion of the cel1.
APPENDIX A. HEATING AND FOCUSING EFFECT AW02{ (2r2)
I::.T(r,t)=-- Ei - - -Ei - ( 2r2)} . (A7)
OF GAUSSIAN LASER BEAM 8k wo2 8Dt+wo2
If field of the laser beam has the Gaussian form of
the principal mode,9 10 H. S. Carslaw and J. C. Jaeger, Operational JfethodsinApplied
Mathematics (Dover Publications, Inc., New York, 1963), p. 109.
E(r) = Eo exp( -r2/wo2) , 11 G. N. Watson, Bessel Functions (The Macmillan Company,
New York, 1948), 2nd ed., p. 393.
8 Ref. 6, Chap. TV. 12 E. Jahnke and F. Emde, Tables of Functions (Teubner,
9 A. Yariv and']. P. Gordon, Proc. IEEE 51, 4 (1963). Berlin, 1938), pp. 1-8.

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8 GORDON et at.

Curves from this equation are plotted in Fig. 5 vs timeter per second] and by b, the fractional dissipation
r/wo for various tlte, where te is defined by (5) and is per centimeter.
around 2 sec for the materials studied. Q(r)=0.Z4bw(r).
The infinite model has the weakness that !:J.T ~ 00
Total beam power is
as t ~ 00. This is because the gradient approaches 1/r
in the steady state, and with !:J.T=O at r= 00, tempera-
a fa 21rrA ( -2r2)
ture integrates to infinity at all finite radii. Reference
10, Sec. 55, gives the corresponding Green's function
P= fo 21rrw(r)dr = --exp
O.24b
- dr
wo
0
2

for a source in a medium of finite radius, but we were


not successful in carrying out the integrations of this = 1I'A W
02[1_exp(_ -2a2)J"",,~AWo2 J (AIO)
form. In view of the localization of temperature, it O.48b wo2 O.4Sb
does not seem very important, but it is useful to have or
the steady-state curve for the finite cylinder. The (All)
following equation will give the steady-state heat con-
duction at r from the sources within. This may be substituted in (A7) and (A9)
For small values of r, the following series12 is ~useful,
dt
- k21rr-=
Jr 21rY'A exp(-2r'2)
- - dr',
2
Ei( -x) =1njtx-x+ (x2/4) ... (AIZ)
dr 0 wo '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 0.06bP[ ( SDt) 16Dt r2 ]
tJ.T(r,t)~-- In 1+- - . (A13)
2
utilizing 31Z(5d) of Ref. 13J. The result, with boundary k wo wo2+SDt wo2
condition !:J.T=O at r=a is
Similarly for the steady-state solution of the bounded
2 rJ
- - -Ei (za
region,
AW02[ Ei (Zr2) --- )-21n-.
!:J.T(r)=-
Sk wo2 wo2 a
(A9)
tJ.T(r)~--
O.06bP[
In -
(z'Ya
)
2
2r2]
-- . (A14)
k wo2 wo2
The curve for this steady state is shown dashed in
Fig. 5. The last equation is plotted as a dotted curve in
The constant A may be related to total power and Fig. 5, and is seen to be a good approximation up to
the rate of dissipation. The heat density of (Al) is r/wo approaching unity.
the power density in watts per square centimeter mul- 13 W. Grobner and N. Hofreiter, Integraltafel (Springer-Verlag,
tiplied by 0.24 [to convert to calories per square cen- Berlin, 1949).

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