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4669
for the case where 17C was the dividing point for the
two curve segments. However, since the end point of
the upper experimental subset for this particular case
showed a deviation greater than 30', the degree of
confidence that one could attach to the existence of a
discontinuity at this point is very small. A deviation
of 30' corresponds approximately to a value of the
dielectric constant differing by 0.02 from the value
represented by the least-squares fit of the data. This
small deviation altered significantly the statistical
results and confirmed our initial statement regarding
Drost-Hansen's interpretation of Devoto's data.
15 DECEMBER 1966
NAUGLE,
t J. H. LUNSFORD,
AND
J. R.
SINGER
The volume viscosity in liquid argon has been calculated from ultrasonic attenuation measurements at
temperatures between 85 and 145K with pressures up to 157 kg/cm2 Measurements taken at densities
from 1.06 to 1.42 g/cm3 result in values of 2.3 to 0.8 for the ratio of volume to shear viscosity. These values
are compared with theoretical predictions of other investigators. It appears that the volume viscosity
increases with increasing density whereas the ratio of volume-to-shear viscosity decreases. The ultrasonic
attenuation rapidly increases as the temperature approaches the critical temperature. This increase in
attenuation is a consequence of the change in the density and compressibility of the medium. Thus no new
mechanism of dissipation is required within about 7K below the critical temperature.
INTRODUCTION
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4670
EXPERIMENTAL
The precision variable-path-Iength apparatus previously used in this laboratory2.3 could not be used for
the high pressures required to explore the properties of
liquid argon up to 145K. The pressure bomb and
ultrasonic cell which is described in the following
paragraphs was designed to meet the new requirements.
Nevertheless, the ultrasonic attenuation and velocity
t~ken with the new equipment was carefully compared
wIth the absolute values obtained by the reliable
variable-path-Iength equipment. The diameter of the
tube through which the ultrasonic waves move in the
new pressure equipment is only 0.75 in. compared to
2.5 in. in the older cell. While the small diameter in the
new ultrasonic test cell described here gave no difficulty
at 50 Me/sec because the sound beam was so very
narrow, the beam spread at 30 Mc/sec was large
enough to require a 12% correction to all attenuation
measurements at that frequency. Those readers not
interested in the details of the new high-pressure test
cell may turn directly to the results and discussion.
The apparatus employed in these measurements was
a single-transducer double-path-Iength8 pulsed system
(Fig. 1) enclosed by a high-pressure cell capable of
withstanding 160 kg/cm2 of pressure. The sample
chamber consists of two reflectors and three spacers
(A, B, and C). The reflectors are right circular cylinders
1.000 in. in diameter and 0.25 in. in length. The
reflecting surface was ground flat within 0.00002 in.
and optically polished. Spacers A and B are hollow
right circular cylinders 1.000 in. o.d., 0.750 in. Ld.
Spacer A is 0.348 in. in length, while Spacer B is 1.923
in. in length. These distances allowed return echoes to
be clearly separated on the scope trace. The difference
in the signal strength of the two echoes determined the
attenuation caused by the extra path length of one
over the other. The inner surface of Spacers A and B
is uniform and round within less than 0.1 % throughout
the length. Spacer C is 0.089 in. in length. The crystal
which was 0.50 in. in diameter, was mounted to one
face of Spacer C, and was held in place by a Teflon
ring fitting over the crystal edge. Both Spacer C and
the Teflon ring were tapered along their inside circumference. Three spring-loaded screws were used to
connect the Teflon ring and spacer, and also to ensure
uniform tension around the crystal edge. The ends of
all three spacers were ground normal to the cylinder
axis and parallel within 5 sec of arc. Both ends of each
spacer were ground flat within 0.00002 in. All components of the sample chamber were made from the
same piece of lnvar stock. Thus, path lengths did
not change significantly over the temperature range
employed in these experiments.
The sample chamber was assembled in a Teflon
sleeve, closed at the lower end. This was then placed in
8
(1956) .
SAMPLE CHAMBER
CELL
SUPPORT TLBE
FILLING TUBE
LOCK NUT
TOP
FERRULE
COMPRESSION CAP
COAXIAL CABLE
BNC CONNECTOR
Q-REFLECTOR
~SPACER
~TEFLON
A
RING
~ BRASS STRIP
TRANSDUCER
BODY
SPACER C
SAMPLE CHAMBER
BRASS JACKET
TEFLON SLEEVE
SPACER B
DEWAR
Q-REFLECTOR
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4671
7
6
50 kg/cm 2
A
<D '"
-o .,"
-;_VJ
~ Ie
'C;2.3
8=0~--~90~----ltOO~----lrI0------12~0----~13-0-----1+4-0-----15~0---
T(OK)
146K. The temperature was measured with a calibrated copper-constantan thermocouple imbedded in
the base of the high-pressure cell. Great care was
taken to allow the entire system to attain thermal
equilibrium at a constant pressure before ultrasonic
attenuation measurements were made.
The electronics were the same as described in Refs. 2
and 3. A quartz transducer with a fundamental frequency of 10 Mc/sec was driven at odd harmonics for
measurements of attenuation at 30 and SO Mc/sec.
Two Arenberg pulsed oscillators were used, one to
generate the ultrasonic signal and provide the triggering
signal and the other to generate a comparison pulse.
The signals were displayed on a Tektronix 585 oscilloscope. Attenuation measurements were made by adjusting the attenuation in the comparison network, so
that the comparison pulse amplitude was matched to
each echo amplitude after a change of pressure and/or
temperature.
RESULTS
The coefficient of attenuation in liquid argon was
measured at constant density with variable temperature and pressure, and also measurements were taken
at constant temperature with variable pressure. For
the constant-temperature measurements, the pressure
was varied from 1.5 to 107 kg/cm2 The pressures and
temperatures used for constant-density measurements
are shown in Table 1. The maximum pressure used
during constant-density measurements was 157 kg/cm2
The change in attenuation in the comparison attenuator
was recorded as a function of the change in pressure and
temperature. Fig. 2 shows the temperature dependence
of a/F. Attenuation became so great in the region of
the critical temperature, 151K, that return echoes
vanished. Indeed, only the 30-Mc/sec sound waves
could be measured above 130 0 K and with considerable
pressure.
(1)
1].
1].=
(2)
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4672
1. Data and results for calculation of the volume viscosity in liquid argon.
Cpb
(OK)
(g/cm3)
(kg/cm2 )
(cal/g
OK)
1.062
146.2
142.4
140.4
135.2
133.4
131.2
158
126
108
62
47
26
0.299
0.319
0.341
0.368
0.370
0.405
p.
l'
2.92
3.14
3.22
3.20
3.19
3.78
KXI0 40
(m/sec)
(cal/oK
seccm)
'1.X 103 d
(g/cm.
sec)
a/f2X101s
(cm-1 sec2)
'1vXIOS
(g/cm
sec)
560
547
536
514
505
485
1. 70
1. 70
1. 70
1. 70
1.69
1.68
0.73
0.72
0.71
0.71
0.71
0.73
4.49
4.77
5.02
5.88
6.38
7.29
1.66
1.60
1.60
1.81
1.94
1.84
'1'/'1'
2.28
2.22
2.26
2.55
2.74
2.52
Av 2.43
1.068
145.4
142.4
137.9
134.2
131.2
153
127
91
57
27
0.296
0.318
0.330
0.365
0.395
2.81
3.14
2.98
3.16
3.76
559
547
535
515
492
1.72
1. 70
1. 74
1.72
1. 70
0.73
0.72
0.72
0.72
0.74
4.07
4.50
4.90
5.80
7.27
1.36
1.40
1.57
1.80
1.95
1.86
1.95
2.18
2.50
2.64
Av 2.23
1.280
114.8
112.6
110.9
109.0
106.0
156
126
103
77
32
0.259
0.266
0.271
0.275
0.284
2.43
2.39
2.42
2.50
2.48
752
746
742
737
726
0.253
0.252
0.251
0.250
0.250
1.44
1.45
1.46
1.47
1.50
2.02
2.07
2.18
2.25
2.40
1.60
1.67
1.83
1.83
1.95
1.11
1.15
1.25
1.24
1.30
Av 1.21
1.287
113.7
112.3
110.8
110.4
108.9
108.0
105.5
157
136
119
119
91
79
40
0.259
0.263
0.268
0.267
0.272
0.275
0.282
2.43
2.46
2.50
2.50
2.41
2.46
2.47
760
756
754
754
748
748
738
0.255
0.254
0.254
0.255
0.253
0.253
0.252
1.48
1.49
1.50
1.50
1.50
1.51
1.53
1.65
1. 71
1.72
1.72
1. 73
1. 76
1.93
1.35
1.67
1.39
1.39
1.41
1.45
1.71
0.91
1.12
0.93
0.92
0.94
0.96
1.12
AvO.99
1.294
112.6
110.2
108.5
106.0
105.0
103.1
156
122
96
63
43
13
0.259
0.266
0.271
0.278
0.281
0.287
2.39
2.41
2.43
2.44
2.38
2.38
764
758
752
745
735
727
2.56
2.56
2.54
2.55
2.53
2.53
1.52
1.54
1.52
1.57
1.55
1.60
1.69
1.77
1.81
1.89
1.96
2.05
1.54
1.65
1.68
1. 72
1.80
1.82
1.01
1.07
1.11
1.09
1.16
1.14
Av 1.10
1.294
112.6
112.3
110.7
109.2
108.1
106.6
155
148
125
106
87
69
0.259
0.261
0.265
0.270
0.272
0.276
2.35
2.45
2.43
2.40
2.48
2.47
767
764
760
756
751
749
2.56
2.56
2.55
2.56
2.54
2.54
1.52
1.51
1.53
1.53
1.52
1.53
1.67
1. 70
1.71
1. 76
1.81
1.84
1.58
1.55
1.50
1.57
1.62
1.68
1.04
1.02
0.98
1.03
1.07
1.09
Av 1.04
1.402
90.5
89.2
88.7
87.7
86.7
99
64
58
35
19
0.257
0.259
0.260
0.261
0.262
2.06
2.06
2.05
2.07
2.11
873
865
864
860
861
3.06
3.03
3.02
3.00
3.00
2.36
2.40
2.43
2.46
2.56
1.57
1.62
1.64
1.66
1.66
2.13
2.13
2.17
2.10
1.96
0.90
0.89
0.89
0.85
0.76
AvO.86
1.408
91. 7
90.4
90.1
88.9
88.2
87.7
86.8
85.0
149
124
113
91
79
65
47
28
0.255
0.256
0.257
0.258
0.260
0.260
0.261
0.262
2.00
2.02
2.01
2.00
2.02
2.03
2.00
2.01
885
881
879
876
874
870
869
870
3.11
3.10
3.03
3.09
3.07
3.07
3.05
3.08
2.42
2.44
2.42
2.45
2.50
2.54
2.56
2.80
1.31
1.35
1.35
1.37
1.40
1.42
1.46
1.54
2.01
2.08
2.10
2.11
2.12
2.05
2.26
2.30
0.83
0.85
0.87
0.86
0.85
0.81
0.88
0.82
AvO.85
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4673
(g/eml )
1.410
T
(OK)
P
(kg/em2)
Cpb
(cal/gOK)
l'
C
(m/see)
KXIQ4
91.8
90.9
89.1
88.3
87.7
155
136
98
78
66
0.255
0.256
0.257
0.258
0.259
2.14
2.03
2.00
2.06
2.05
887
883
878
874
872
3.10
3.09
3.08
3.07
3.06
(calrKsec-em)
'1.X 1()3 d
(g/emsec)
(em-1 see2)
'1.Xl()3
(g/emsec)
2.41
2.41
2.45
2.48
2.54
1.34
1.38
1.41
1.46
1.48
2.13
2.34
2.33
2.40
2.39
a/rXlOl&
'1./"13
0.88
0.97
0.95
0.97
0.94
AvO.94
1.413
91.1
90.1
89.1
88.2
87.7
86.3
0.255
0.256
0.257
0.259
0.260
0.261
155
135
113
93
79
57
1.99
2.00
1.99
2.00
2.00
2.00
891
886
883
878
878
876
3.12
3.10
3.09
3.09
3.09
3.09
2.46
2.46
2.50
2.54
2.56
2.68
2.21
2.04
2.31
2.50
2.39
2.09
1.32
1.31
1.39
1.45
1.44
1.42
0.90
0.83
0.92
0.96
0.93
0.78
AvO.89
a Reference 10.
b Rl!ferences 9 and 10.
o L. D. Ikenberry and S. A. Rice, J. Chem. Phys. 39,1561 (1963); WADD
Tech. Rept. 60-56 "A Compendium of Properties of Materials at Low Tempera
tures (Phase I) ,n NBSCEL (1960).
-..
I f)
o.
0
0
RAY It RICE---+I
(REF.41
O~
1.0
-+____________+-__________
__________~____________~__________
1.1
1.2
1.3
1.4
I,e
FIG. 3. Density dependence of '1.: Range of values calculated for "Iv at constant density under variable temperature and pressure
(bars). Single data-point calculations or averages of several points at the same temperature and pressure'I[O, 50-Mc/sec. dll-tll-i AI
corrected 30-Me/sec data); D, results of Naugle (Ref. 3) J.
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4674
~TJs
o~------------~------------~--------------~------------~---------1.4
1.1
L3
La
1.2
p< g/cm3 )
FIG. 4. Density dependence of 11./11.: Averages of values at constant density under variable temperature and pressure (e, 50-Me/sec
data; A, corrected 30-Mc/sec data). Single data-point calculations or averages of several points at the same temperature and pressure
[( 0, 50-Me/sec data; 1':.., corrected 30-Mc/sec data); 0, results of Naugle (Ref. 3); . , results of Luks, Miller, and Davis (Ref. 7);
<>, results of Gray and Rice (Ref. 4)].
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4675
800
700
C(m"'c)
600
500
50kg/cm 2
400~----~--~~--~~--~----~-----+-----+-------
80
90
100
110
130
140
150
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4676
error of both values. The ratio of 71.111. is -i for a zerothorder rigid-sphere calculation,12l3 and very close to -i in
the small step diffusion theory of Rice and Kirkwood. l4
It appears that 71.171. decreases with increasing density.
Using a square-well potential and a pair correlation
function for hard spheres, Luks, Miller, and Davis7
have recently calculated the ratio of 71.1718 at the same
temperatures and pressures that were reported by
Naugle. s These calculated values, which are shown in
Fig. 4, are within the experimental error of our results;
however, they do not reflect that 71.1718 decreases with
increasing density.
Our values of 71. at constant density do not indicate
an increase of 71. with increasing temperature as the
theory of Gray and Rice4 predicts. Scatter in the
experimental data, however, is greater than the 10%
increase which they predict for a comparable temperature range. The data reported here suggest that
as density increases 71. also increases.
The increase in alP as the temperature approaches the
critical temperature is in agreement with the ultrasonic
attenuation work of Chynoweth and Schneider l5 on
liquid xenon. They have explained the increase in alP
in terms of structural relaxation processes; that is, a
high-density region formed by the acoustic wave does
not relax rapidly with respect to the time scale repre12 H. C. Longuet-Higgins and J. P. Valleau, Mol. Phys. I,
284 (1958).
13 H. C. Longuet-Higgins and J. A. Pople, J. Chern. Phys.
25,884 (1956).
14 S. A. Rice and J. G. Kirkwood, J. Chern. Phys. 31, 901
(1959).
16 A. G. Chynoweth and W. G. Schneider, J. Chern. Phys.
20, 1777 (1952).
J.
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