Diffusion Coefficients of Helium in Fused Quartz

D. E. Swets, R. W. Lee, and R. C. Frank

Citation: The Journal of Chemical Physics 34, 17 (1961); doi: 10.1063/1.1731562
View online: http://dx.doi.org/10.1063/1.1731562
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VOLUME 34, NUMBER 1

THE JOURNAL OF CHEMICAL PHYSICS

JANUARY, 1961

Diffusion Coefficients of Helium in Fused Quartz

D. E.

SWETS,

R. W.

LEE, AND

R. C.

FRANK

General Motors Research Laboratories, Warren, Michigan

(Received April 27, 1960)
The diffusion of helium through the walls of high-purity fused quartz hollow cylinders was studied using
a mass spectrometer as a detecting device. By surrounding the outside of the hollow cylinder with helium
and observing it diffuse through into the mass spectrometer, permeation rates and diffusion coefficients
were measured in the temperature range of 24 to 1034C. The diffusion process appeared to be relatively
simple with only small deviations from Fick's laws occurring. The activation energy was found to be different
in the temperature range of 24 to 300C than in the range of 300 to 1034C. In the low-temperature range
the diffusion coefficients are expressed by
cal/g atom) cm2/ sec,
D=304XI0-'

exp (558056RT
and in the high-temperature range they are expressed by
cal/g atom) cm2/sec.
D = 740X 10-' exp (_ 661340RT
The solubility was also determined by dividing the permeability by the diffusion coefficients. This was expressed by
cal/g atom) a t oms/ cm 3
S = 1.99X 1017 exp (_ -68060RT
in the temperature range of 24 to 300C and by
g atom)
17
S =128XI0

exp ( _ -1174120cal/
RT
atoms / cm 3
in the range 300 to 1034C.

INTRODUCTION

EXPERIMENTAL PROCEDURE

HE relatively good agreement between the many

investigators who have measured the permeability
of helium in fused quartz is very encouraging. 1- 5 Although there have been a number of good measurements
of the permeabilities there have apparently been only a
few attempts to determine the diffusion coefficients.
Barrer6 calculated diffusion coefficients by dividing
his permeabilities by the solubility values obtained by
Williams and Ferguson.7 Jones5 measured both the
permeabilities and solubilities and divided the first
by the second to get the diffusion coefficients. In the
present work the diffusion coefficients have been obtained directly by measuring the rate of change of
helium permeation through hollow fused quartz
cylinders with a mass spectrometer when helium was
suddenly introduced or removed from the outside
surface of the cylinder. The permeabilities were obtained from the steady state permeation and the solubilities were calculated by dividing the permeabilities
by the diffusion coefficients.

The fused quartz diffusion specimens used in these

tests were constructed as shown in Fig. 1. Two such
samples were used, one having a wall thickness of l.4S
0.06 mm, the other a wall thickness of O.90SO.OSS
mm. The quartz used in these samples were analyzed
spectrographically and found to have the following
impurities: Al 0.0040%, Mg O.OOlS%. Visual and microscopic inspection showed no gross defects although
some striations were present.
The diffusion specimen and associated equipment
are shown in Fig. 1. The inner volume was connected
directly to the ion source of a mass spectrometer. The
outer volume was attached to a vacuum and gas inlet
system. The entire sample system was enclosed in a
resistance oven which was large enough so that the
temperature along the length of the sample was uniform. A chromel-alumel thermocouple was mounted as is

1 L. S. Tsai and T. Hogness, J. Phys. Chern. 36, 2595 (1932).

E. O. Braaten and G. F. Clark, J. Am. Chern. Soc. 57, 2714
(1935) .
3 R. M. Barrer, J. Chern. Soc. 1934, 378.
4 Francis J. Norton, J. Am. Ceram. Soc. 36, 90 (1953).
5 W. M. Jones, J. Am. Chern. Soc. 75, 3093 (1953).
6 R. M. Barrer, Diffusion in and through Solids (Cambridge
University Press, New York, 1951), p. 141.
7 G. A. Williams and J. B. Ferguson, J. Am. Chern. Soc. 46,
635 (1924).
2

To Mass spectrometer

FIG. 1. Diagram of the diffusion specimen mounting and oven.

17
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18

SWETS, LEE, AND

o=

MATHEMATICS OF THE METHOD

Diffvdon CoeFficient

I = Woll Thicknesl
L = Effective Time lag
= Evolution Time Constant

'0

Helium Introduced Into

the

Fused Qvar'-

--1---

ll
---1

He I'IUfTI E
va ulion

FIG. 2. Typical mass spectrometer record for helium diffusion

through fused quartz.

FRANK

The mathematics of the method used for calculating

the diffusion coefficients has been discussed in earlier
papers,8-10 so only a brief discussion is needed here.
When gas is suddenly introduced into the outside of the
hollow cylindrical specimen, the mass spectrometer
reading on the gas can be shown to vary as10
h= (sA DCo/ F1l) [(k-1) / Ink]

X {1+2:E( -1)n exp( -rn2/P)Dtll, n= 1,2, "',

shown in Fig. 1 and used to read the sample temperature. The mass spectrometer was a modified General
Electric 60 deg sector field instrument.
The procedure carried out for each test was as
follows. The outer volume was evacuated to a pressure
of about 1 X 10-5 mm of Hg by an oil diffusion pump,
after which the valve to the pump was closed. Helium
gas from a lecture bottle was then quickly allowed into
the system through a liquid nitrogen cold-trap to remove impurities. The pressure was read with a mercury
manometer and held constant. As gas permeated the
wall of the inner quartz tube it was continually recorded by the mass spectrometer. After a constant
rate had been reached, establishing a value for the
steady-state permeation rate, the gas in the outer
chamber was evacuated. The mass spectrometer then
recorded the evolution of gas from the sample. Both the
input and the evolution data were used to obtain values
for the diffusion coefficient. See Fig. 2. Tests were made
at a number of temperatures chosen at random until the
range of 24C to 1034C had been covered. Fewer
tests were made at the lower temperatures because of
the long periods of time required to carry out the
tests.
Several tests were made in an attempt to establish
the relationship between the permeation rate and the
gas pressure on the outside of the specimen. Most of
these were carried out at temperatures above 300C
because at temperatures below this the time required
to reach steady state each time was rather long. In
each test the temperature was held constant and the
permeation rate was measured at various pressures.
The permeation rate was plotted against pressure on
logarithmic graph paper. It was found that the relationship between the permeation rate and pressure could
be expressed by
h=Kjf",

where h is the mass spectrometer reading, p is the pressure outside the specimen, and K is a constant of
prop?rtionality, x was found to be slightly less than 1,
varymg from about 0.93 to 0.97. The error of the method
was such that this value could not be established more
accurately without performing a large number of tests.

(1)

n=1

where A = the in temal surface area of the specimen j

s= the mass spectrometer sensitivity for the gas being
usedj F1=the conductance of the leak used to obtain
Sj Co=the concentration of the gas dissolved in the
outside surface of the specimen; l=the wall thickness of
the specimen; k=the ratio of the outside to the inside
diameter of the specimen. D=the diffusion coefficient;
and, t=time.
This equation is applicable only if the following conditions exist: (a) The diffusion coefficient D is a constant. (b) The thickness of the wall must be small
compared to the radius of the cylinder (1 <k< 1.5).
(c) The time constant for the pump-out rate of the ion
source of the mass spectrometer must be much smaller
than the time constant for the transient effect of the
diffusion process.
When steady state is reached the exponentials drop
out and the equation becomes

ho= (sADC o/F 1l)[(k-1)/lnk]'

(2)

If, after steady state has been reached, the gas is

suddenly removed from the outside surface of the
specimen, the mass spectrometer reading will drop
off as
h= ho{2:E ( -1)n exp[ - (rn2/P)Dt]l.

(3)

n=O

After a short time the mass spectrometer recorder trace

becomes a simple exponential decay with a time constant equal to
(4)
to=l2/rD.
The thickness of the specimen l, can be measured before
fabrication using a micrometer, to is measured on the
recorder trace and, therefore, D can be easily calculated
fromEq. (4).
The "time lag" method used by Barrer6 is also
A. Van Wieringen and N. Warmoltz, Physica 22,849 (1956).
R. C. Frank, D. E. Swets, and D. L. Fry, J. Appl. Phys. 29,
892 (1958).
10 R. C. Frank and J. E. Thomas, Jr., J. Phys. Chern. Solids
(to be published).
8
9

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19

D IFF U S ION CO E F F I C lEN T S 0 F HE L I U MIN F USE D QUA R T Z

applicable. This can be shown by integrating Eq. (1);

hdt= 1kJ+ (2Nto/rD)

f[( -1) n/n

DEGREES CENTIGRADE

750

2
]

....1

r-.r-,

I x 10

(5)

A plot of the integral against time becomes a straight

line after a short time due to the fact that the exponentials approach zero. The intercept of the straight line
with the time axis is found from the equation

1kJ- (2hJ2/12D) =0

r.~

(6)

'"
....

sri
6

f\,~.:::

I
S

10

12

14

16

18

20

1/T

22

24

26

2S

30

32

34

36

x 10

FIG. 3. Diffusion coefficients, D, as a function of temperature.

Rearranging Eq. (6) it is easily shown that

(7)

Therefore, the first part of the mass spectrometer curve

can be integrated with a planimeter and the integral
plotted against time. The linear portion of this curve
can then be extrapolated to the time axis and the effective time lag L determined. The diffusion coefficient
can be calculated from this.
The diffusion coefficients can also be calculated using
curve fitting techniques8 9 or the inflection point technique used by McAfee ll but it is believed that these
rely a little more on the judgment of the experimenter.
The permeability is obtained from the steady state
mass spectrometer reading ho which is multiplied by
Fl l/s{A[(k-l)/ InkJ} to give the permeation constant
P in the commonly used units. The factor
A[(k-l)/lnkJ
is the effective area. As can be seen from Eq. (2)

(8)

when the gas pressure outside of the specimen is one

atmosphere the concentration Co inside the surface is
considered to be the solubility S. Therefore,

preliminary plot of the diffusion coefficients against

l/TX 1000 had been made it was found that the curve
appeared to have two straight-line portions with a
connecting transition region. The actual data points for
eai:h of the straight-line portions of the curve were
then fed into an IBM 704 computer and the leastmean-square lines were calculated. The computer also
calculated the 95% confidence limits on these lines, as
well as the correlation coefficients. The least-meansquare curves and the 95% confidence limits have been
plotted in Fig. 3. The line in the upper temperature
range was calculated from 26 data points while that
in the lower range was calculated from 5 points. 12
The straight lines can be expressed mathematically by

D=Doe-E1RT,
where Do is the frequency factor, (a measure of the
frequency of vibration of the impurity in the interstitial
site); E is the activation energy; R is the gas constant;
and, T is the absolute temperature.
In the high-temperature range (300 0 -1034C) the
least-mean-square line through the points is represented by

(9)

Finally, after the diffusion coefficient and permeability

have been measured, the solubility can be calculated
from Eq. (9).

D= 7.40 X 10-4 exp( -

Values of the diffusion coefficients in the temperature

range from 24 to 1034C were calculated by both the
time lag and the decay methods. The values of D
found by the two methods agree quite well. However,
for reasons which will be described below, the decay
values are considered slightly more accurate and were
the values used to obtain the plot in Fig. 3. After a

661340 cal/g atom)

2/
RT
em sec.

In the lower temperature range the least-meansquare line through the points is represented by

RESULTS

K. B. McAfee, Jr., J. Chern. Phys. 28, 218 (1958).

~.f\,

.......

_1

11

".'.

f[( -1)n/n2]= -r/12.

P=DS.

r.. ..

1 x 10~

P= DCo= Permeability,

r..r-,

since

t=Pj6D= L=effective time lag.

24

100

200

'/>.~

-5

X{1-exp[-(rn 2/P)DtJ}.

400

D=3.04XI0-4 exp( -

558056 cal/g atom)

RT
cm2/sec.

The errors quoted are 0.67 times the standard deviation

of the slope of the lines multiplied by R.
As mentioned above, there was a slight but consistent
difference between the values for D found by the time
lag and decay methods. In all but two cases the diffu12

Actual values are listed in the Appendix.

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20

SWETS, LEE, AND FRANK

DEGREES CENTIGRADE
400

750

200

==

...01-< 1-:1-

==
=

--

--

100

-- - --

I'

10

13

,=
1=

1-

~t::::

-"-1

==

E
0
').
E

----i

12

.2-

FIG. 4. Permeability, P, and solubility, S, as a function of temperature.

~~

~-

1 x 10

-~

~=

ill

1-

!=

JONES
o WILLIAMS AND FERGUSON

~ ~%

-U-

I~
1=
1-

=
-

24

H-

'.

~t::::

==
~

~~
"

f-

~~-,
'~

F
f:

"

f-f--

1 x lO"

-'-=

'-

I:::F
I=~

I-tI-fI-f-

,,~

~--.

~r..,
,...~

BRM TEN AN D CLARK

o TSAI
AN D H f r n
NORTON

JONES
8
10 12

14

16

18

1/T

20

22
4
x 10

24

26

28

sion coefficients found by the time lag method were a

few percent higher than those found by the decay curve
method. After the possibility of calculation errors or
temperature effects was eliminated it was found that
there was a slight dependence of the time lag values
upon the pressure of the gas outside of the specimen.
The first half of the transient curve is obtained when
the specimen is subjected to a gas pressure whereas
all of the gas is removed from the chamber during the
decay portion of the curve. It was therefore assumed
that the gas pressure somehow changed the character
of the fused quartz lattice to affect the helium diffusion, and for this reason the decay values were used.
Unfortunately there was too much scatter in the time
lag results and their deviation from the decay values was
too small to establish a mathematical relation between
diffusion coefficient values and pressure.
The permeability P, was also measured and is plotted
against (l/T) X 1000 in Fig. 4. The units of Pare
atoms/sec em for a sample 1 em thick and a pressure
difference across the membrane of 76 em of Hg. The
solid lines in Fig. 4 are the least-mean-square lines
obtained from the points of the present work. The
dotted lines are the 95% confidence limits on the leastmean-square lines. The results of a number of other
investigations, converted to the same units, are also
plotted in Fig. 4 and show good agreement with the
present work. Barrer's3 permeability values are about a
factor of 5 or 6 below all the other values and have not
been included on the curve.

~~
30

I:::~

"'<ii~
32

I=f=

I-fI-t--

~ ~,
34

36

The solubility of helium in fused quartz can be found

by dividing the permeability by the diffusion coefficient
value at a given temperature. The units for the solubility are then atoms/cms for a pressure of 76 cm of Hg
outside of the sample. A plot of solubility vs (l/T) X
1000 is also shown on Fig. 4.
In the upper temperature range the equation for the
line is
S=1.28XI017

X exp( -

-1174120caljgatom)

RT

/3

atoms cm .

In the lower temperature range the straight line

portion of the curve is represented by

S= 1.99X 1017
X exp( -

~68060 cal/g atom)

RT

atoms cm.

The values of solubility found by Jones5 and also by

Williams and Ferguson7 are plotted on the curve and
show very good agreement with the present work.
It is particularly noteworthy that in both temperature ranges the heat of solution is negative. The solubility therefore decreases with increasing temperature.
The heat of solution is greater in the upper temperature
range than in the lower.

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D IFF U S ION

C 0 E F F I C lEN T S 0 F

DISCUSSION

Since the permeabilities and solubilities found by

Jones agree fairly well with the present work the diffusion coefficients calculated from P / S might also be
expected to agree fairly well. The diffusion coefficients
calculated by Barrer, 6 which have long been considered
the only values, are approximately two orders of magnitude lower than those reported here.
There was extremely good agreement between the
diffusion coefficient values obtained in this work from
the two specimens of different thicknesses. This indicates two things: (a) The fused quartz is of reproducible
quality (b) The diffusion coefficients are not a function
of the thickness of the specimens.
The fact that there is some correlation between the
time lag diffusion coefficient values and the pressure of
the helium outside of the specimen indicates the possibilityof the diffusion coefficient being increased when
the specimen is under compressive stress. McAfee
studied the effect of stress on the diffusion coefficients
of helium in Pyrex glass ll at room temperature but
found that the effect of compressive stresses was small
or nonexistent. In plastic materials such as iron the
increase in diffusion rate produced by subjecting the
specimen to stress is believed to be associated with
the movement of dislocations. 13 However, little is
known about dislocation-like defects in fused quartz
and therefore not much can be said about their effects
on the diffusion properties of interstitials.
Equation (4), from which values of D were found,
is obtained under the assumption that the laws of
simple diffusion are applicable. The results indicate
that this was a fair assumption for the following
reasons: (a) The decay curves exhibited a simple
exponential decay over most of the evolution process.
In general the tail end of the decay curve deviated
slightly from the exponential law but the quantity of
gas involved in this deviation was less than 1% of the
total gas evolved. (b) There was only a small difference
between the time-lag and the decay diffusion coefficient values, particularly at low-gas pressures. Under
these circumstances it seems justifiable to define a
constant diffusion coefficient at a given temperature.
A commonly accepted model for the lattice structure
of fused silica is that proposed by Zachariasen 14 which
considers the structure to be a random array of the
basic tetrahedra. Thus the lattice is believed to consist
of a rather wide assortment of sizes of the interstices.
The activation energy for the diffusion of impurities in
a crystalline lattice is considered to be the energy
required for the impurity atom to jump from one
interstitial site to another,l5 Therefore a variation in
"jumping" energy corresponding to the assorted sizes
13 P. Bastien and P. Azou, Proc. 1st World Met. Cong., 1951.
Am. Soc. Metals, p. 535.
14W. H. Zachariasen, J. Am. Chem. Soc. 54, 3841 (1932).
1& C. Wert and C. Zener, Phys. Rev. 76, 1169 (1949).

H ELI U MIN F USE D

QUA R T Z

21

of the interstices would be expected, and the activation

energy for diffusion would be an average of all possible
jumping energies.
The curve of the diffusion coefficients as a function of
temperature appears to have a straight line relationship
from 24 DC to 300 DC and from 300 DC to 1034 DC but the
slopes are slightly different for the two ranges and
therefore the activation energy for diffusion is slightly
different in each range. The change in activation energy
implies a change in the average jumping energy. It is
perhaps important to note that there is not only a
change in activation energy for diffusion but also a
change in the heat of solution. In looking for possible
explanations for this it is necessary to look for changes
in other physical properties which occur in the temperature range near 300 DC. Although vitreous or fused
silica does not exhibit the presence of inversion points
in the volume vs temperature curve, the crystalline
forms of silica do. Cristobolite and tridymite, in fact,
show very pronounced inversions in the temperature
range of 160 DC to 280 DC. There are also inversions in
the birefringency16 vs temperature curves in this range.
The existence of a change in activation energy for
helium diffusion in the temperature range in which an
inversion occurs in the crystalline forms of silica
suggests the possibility that there are characteristics of
the crystalline forms of silica which are carried over
into the vitreous form of the material. Several experiments, including those by Westman and Crowther 17
and also Prebus and Michene 18 indicate that the Zachariasen picture of the fused silica lattice may not be
entirely adequate. They suggest that instead of a
completely random arrangement, the glass lattice might
actually contain regions in which there is a repeating
and somewhat uniform structure. The notion of the
existence of extremely small crystallites in glass was
apparently proposed many years ago by Lebedev19
and much experimental work supporting the view has
been done in the Soviet Union. It is possible that fused
quartz in some subtle way retains some of the properties
of cristobolite and that this is what produces the change
in activation energy for the diffusion of helium in fused
quartz in the region near 300 DC.
Investigations of the permeation rate as a function
of the gas pressure indicate that at least in the hightemperature range the permeation rate is not a linear
function of the pressure. The exponent of the pressure is
slightly less than one. The permeation rate-pressure
relationship for helium in glass has been investigated
by a number of people l - 3 ,20 but apparently Urey20
16 R. B. Sosman, The Properties of Silica (Chemical Catalog
Company, New York, 1927).
17 A. E. Westman and J. Crowther, J. Am. Ceram. Soc. 37, 420
(1954) .
18 A. F. Prebus and J. W. Michener, Ind. Eng. Chem. 46, 147
(1954).
19 K, S. Evstropyev, The Structure of Glass, translated from
Russian (Consultants Bureau, Inc., New York, 1958), p. 9.
2<l W. D. Urey, J. Am. Chem. Soc. 54, 3887 (1932).

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22

SWETS, LEE, AND FRANK

TABLE I. Diffusion coefficients.
Temperature

814
857
854
605
608

1038
1034
1028
1032

Diffusion
coefficients
(10-7 (cm2/sec)

355.
387.
380.
158.
159.
613.

861
861
712
712
717
717
490
489
284

610.
584.
580.
401.
416.
408.
244.
237.
250.
248.
90.2
89.4
19.5

492
380
378
378
700
705
704
191
78
24
112
148

94.5
48.1
43.9
47.7
241.
245.
238.
7.28
1.06
.239
2.15
3.73

860

is the only one who found anything other than a linear

pressure relationship. He found that the permeation
rate was an exponential function of the pressure and the
exponent was slightly less than unity but varied with
the composition of the glass. Since helium cannot
dissociate and does not react with the silica, an exponnent less than one is difficult to explain. It might indicate that when the helium enters the quartz it passes
through an adsorption phase in which the amount
adsorbed is not a linear function of the pressure.
Although the diffusion of helium in fused quartz
appears to be relatively simple compared to other
TABLE II. Permeabilities.
Temperature
Permeabilities
(Oe)
(1011 Atoms/em sec)

1034
861
717
490
284
492
380
705
191
78
24
112
148

118.
86.1
62.8
22.2
6.92
27.3
15.3
55.8
3.00
.532
.151
.995
1. 76

diffusion systems it is probably not as simple as the

earlier investigators believed and a few minor discrepancies remain to be investigated in the future as
better methods become available.
ACKNOWLEDGMENTS

The authors wish to express their appreciation to

Arthur Dolenga for constructing the diffusion specimens and to Robert L. Williams for assistance with
the operation of the mass spectrometer and with
the data reduction. James E. Dallemand supplied
some helpful advice about the statistical treatment of
the data.
APPENDIX

The actual diffusion coefficient values used in plotting

the curve in Fig. 3 are given in Table 1. These values
were obtained by substituting the time constants of
the evolution curves into Eq. (4). The values above
the black line were measured using the specimen
TABLE III. Additional diffusion coefficient data.
Temperature

227
261
281
334
334
708
430
430
607
606

Diffusion
coefficients
(10-7 cm2/sec)

11.6
17.0
20.6
32.9
33.1
240.
64.0
68.0
177 .
170.

which was 1.48 mm thick and those below the line

were obtained using the specimen which was 0.905
mm thick.
The permeabilities used to obtain the curve in Fig.
4 are listed in Table II. There are more diffusion coefficient values than permeability values since some of the
tests were performed at reduced pressures to study the
effect of pressure on the permeation rate. The diffusion
coefficients calculated from the evolution curves did
not vary with the pressure and therefore they are as
valid as the values obtained using higher pressures and
are included. In the table of permeabilities the black
line again separates the data of the 1.48-mm thick
specimen from that of the O.90S-mm thick specimen.
Note. Since the initial writing of this paper additional
data has been taken which confirms that the InD vs
liT plot in Fig. 3 is best represented by two straight
lines rather than by one line with continuously varying
slope. The additional diffusion coefficient values are
given in Table III. As shown, many of these are taken
in the temperature range where the change in slope
occurs. All of these new points fall almost exactly on
the least-mean-square lines shown in Fig. 3.

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