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Transient ballistic and diffusive phonon heat transport in thin films
A. A. Joshi and A. Majumdar
Department of Mechanical and EnvironmentaI Engineering, University of California, Santa Barbara,
California 93106
(Received 20 January 1993; accepted for publication 17 March 1993)
Ballistic and diffusive phonon transport under small time and spatial scales are important in
fast-switching electronic devices and pulsed-laser processing of materials. The Fourier law
represents only diffusive transport and yields an infinite speed for heat waves. Although the
hyperbolic heat equation involves a finite heat wave speed, it cannot model ballistic phonon
transport in short spatial scales, which under steady state follows the Casimir limit of phonon
radiation. An equation of phonon radiative transfer (EPRT) is developed which shows the
correct limiting behavior for both purely ballistic and diffusive transport. The solution of the
EPRT for diamond thin films not only produces wall temperature jumps under ballistic
transport but shows markedly different transient response from that of the Fourier law and the
hyperbolic heat equation even for predominantly diffusive transport. For sudden temperature
rise at one film boundary, the results show that the Fourier law and the hyperbolic heat equation
can significantly over- or underpredict the boundary heat flux at time scales smaller than the
phonon relaxation times.
31 J. Appl. Phys. 74 (I), I July 1993 0021-8979/93/74(1)/31/9/$6.00 @ 1993 American Institute of Physics 31
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perature jumps under ballistic transport as demonstrated
by both the Monte Carlo simulations and the EPRT. In
this article, the transient EPRT is used to analyze heat
transport under both short time and spatial scales. The
results are compared with those obtained from the Fourier
law and the hyperbolic heat equation to demonstrate the
differences in the predictions and the errors that one might
make if the classical laws are used.
L-Q
II. THEORY
The theory developed in this section can be applied to
any medium where phonon heat transport is the dominant
mode. Consider a dielectric film of thickness L, initially at
temperature T,,. At time t=O, the temperature at x=0 is
increased to T1 while the temperature at x= L is main-
tained at To, as schematically shown in Fig. 1. Such a
L<<Q
situation arises when a dielectric film is sandwiched be-
tween two metallic films. Since the electron-phonon mean
free path in metals is much smaller than the phonon mean
g = c(T1 - Tz ) - Casimir Limit free path in the dielectric film, the two interfaces can be
assumed to be thermalizing black boundaries at fixed tem-
peratures. The following dimensionless variables are de-
fined:
32 J. Appl. Phys., Vol. 74, No. 1, 1 July 1993 A. A. Joshi and A. Majumdar 32
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B. Hyperbolic heat equation
The hyperbolic heat equation (HHE) can be obtained
by combining Eq. (4) with the energy balance equation Dielectric or
x
33 J. Appl. Phys., Vol. 74, No. 1, 1 July 1993 A. A. Joshi and A. Majumdar 33
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where ,u=cos 0. Note that the local equilibrium intensity Once the intensity is evaluated from Eqs. (24) and (25) as
distribution p, is a function of temperature only which in a function of time, position, and frequency, the heat flux
turn depends on the location x. The heat flux at any point can be calculated from Eq. (20) as
can then be defined as
dX,t)=+ j-;--l j-;Dpr,-(x,w,p)dw dp
q=z c v,(e,~)N,(x,t)~(cl)~(w)
P Q 1 OD
OD
+ pI,‘Cw,pL)dw dp (28)
=
s p=o s 0
pL(w,~2)d~ df-h (19)
s R=4rr s 0 and the temperature can be calculated by the relation
where dfl is the incremental solid angle shown in Fig. 3. In
terms of 0 and 4 the incremental solid angle is dfl
=sin 8 dtl dt$. If the phonon intensity is assumed to be
independent of the azimuthal angle I$, then the heat flux 1 “D 1
can be written as -L(x,p)dp do. (29)
=z s m=o s p=-1
q=2p 1
OD/-4i,(w,~)d~ dp. Equation (29) uses the BoseEinstein statistics as the equi-
IS--I
0 librium phonon distribution.‘2
If the EPRT in Eq. ( 18) is integrated over p and w in the It should be noted that Eqs. (24) and (25) are wave
range - 1 <p < 1 and 0 <o < wg then the following equa- equations with speeds VP which will produce intensity
tion is derived: waves that are attenuated due to scattering represented by
p,PW
--I,l
Q(@,T)
dpdw. (21)
the right-hand side of the equations. These equations are
solved using the explicit upstream differencing method, i.e.,
using backward differencing in space when the wave is
traveling in the positive x direction [Eq. (24)] and using
Under the first law of thermodynamics given in Eq. (10) it
forward differencing in space when it is traveling in the
is clear that the right-hand side of Eq. (21) is equal to
negative x direction [Eq. (25)]. In both equations forward
zero. Although Eq. (21) suggests that the integral over all
difference in time was used ensuring At<Ax/( v 1~1) to
frequencies is equal to zero, we simplify the calculations by
make it stable. The frequency range (0 < o < tic) for o was
invoking a more stringent condition of equality at every
divided into 29 divisions and the range of cosine of the
frequency,
angle ( - 1 <p < 1) was divided into 19 divisions. The grid
size As was chosen to be 0.025. These discretizations gave
ro,[W=~j-~lZ,d~. (22 a numerical error of less than 1%.
34 J. Appt. Phys., Vol. 74, No. 1, 1 July 1993 A. A. Joshi and A. Majumdar 34
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TABLE I. Physical properties of type-IIa diamond. Rayleigh law in the large-wavelength range and projected
area of the defect in the small-wavelength regime, and in-
Lattice constant a 3.51 iis volves a smooth transition between them.r7 The Umklapp
Specific heat C 517.05 [J/kg Klb at 300 K
hlass density p 3510 kg/m3 b
relaxation time ru is approximated asts
Debye temperature 6o 1860 K”
Speedof sound Y 12 288 m/s
v=A(T/@Dw)exp(~dyT), (36)
Constant A in Eq. (36) 163.94’ where A is a nondimensional constant which depends on
Stefan-Boltzmann constant o 50.47 [W/m’ K”]
the atomic mass, the lattice spacing, and the Gruinessen
‘Ashcroft and Mermin (see Ref. 12). constant12 and y is a parameter representing the effect of
9ouloukian and Buyco ‘(see Ref. 13). crystal structure. This relation predicts the thermal con-
See explanation in text. ductivity to vary as /z - T3 exp (BD/yT) which has been
observed experimentally for several materials.4 The value
of A has been calculated by Majumdar’ and is given in
for the effective relaxation time. Instead, we defined an Table I. The room-temperature thermal conductivities of
acoustical thickness qL of the medium in Sec. II as type-IIa diamond with different concentrations of 13C iso-
r]L= L/vTR= L/I, (32) tropic impurity were measured by Anthony et al. l9 and are
listed in Table II. Using Eq. (2) for thermal conductivity,
similar to the optical thickness defined in photon radiative we calculated the effective mean free path. Using the rela-
transfer.’ One must note that the mean free path is a sta- tions for ri and TV and the Matthiessen rule we separated
tistical quantity such that the probability p that a particle the contributions of impurity scattering and Umklapp scat-
can transverse a distance x without scattering is p tering and listed them in Table II. The phonon frequency
-exp( -x/1).16 Therefore, when vL= L./l-O, the proba- used for the calculations is that dominant in energy. This is
bility of no scattering event is p-+ 1. Then the transport is calculated from the relation tidorn = k,T. It was encour-
purely ballistic and the medium can be called acoustically aging to observe that the mean free path for Umklapp
thin. If boundary scattering is included in Eq. (3 1) then scattering is independent of the impurity concentration as
the largest value of qL would be unity for which the prob- expected.
abilityp=O.37. Therefore the purely ballistic limit cannot
be represented if the relaxation time for boundary scatter- IV. RESULTS
ing is included in Fq. (3 1). In this limit Majumdar’
showed that the Casimir limit can be obtained from the In this section results are presented for transient heat
EPRT. Under diffusive transport rlL+ r~) and the medium transport in thin diamond films of thicknesses 0.1, 1.0, and
is acoustically thick for which the EPRT produces the 10 ,um, initially at a temperature of 300 K, when the tem-
Fourier law. perature of one boundary of the film is suddenly increased
The relaxation time T, for impurity scattering can be by AT=O.l K. From Table II, the mean free path of pho-
approximated as nons under three different concentrations is calculated to
be of the order of 1 pm. Therefore, for films of thickness of
Tf= l/aqqv, (33) the order of 1 pm or less, macroscopic heat transport laws
where a is a constant of the order of unity, v is the number cannot be applied.20 The relaxation time ‘~jl, in HHE was
of scattering sites per unit volume or defect density, and p’, calculated as I/v where I is the effective mean free path and
the scattering cross section, is assumed to vary ass u is the speed of sound. From the values in Tables I and II,
?-Rwas calculated to be 36.5 ps for a 0.07% concentration
~=7rR2[$/(X4+1)]. (34) of 13C. This impurity concentration is used for all the cal-
In the above equation, R is the radius of the lattice imper- culations of heat transport.
fection and x is the size parameter defined as Figure 4 shows the temperature profile in a diamond
thin film of thickness L=O. 1 ,um at dimensionless times of
~=2rR/A=wR/v, (35) r=O.l, ~=1.0, and steady state. This film thickness is
and A is the phonon wavelength. The assumed scattering smaller than the mean free path and therefore partially
cross section in Eq. (34) has correct limiting behaviors of ballistic heat transport is expected. At ~=0.1, the Fourier
TABLE II. Thermal conductivities and mean free paths of type-Ha diamond at room temperature for different concentrations of 13C isotope. MFP
denotes mean free path.
35 J. Appl. Phys., Vol. 74, No. 1, 1 July 1993 A. A. Joshi and A. Majumdar 35
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equation, these diffusion effects are seen because the relax-
ation time rR (w ) at some phonon frequencies is very short.
1.0
These phonon modes relax and give rise to some degree of
0.6 --0- EPRT diffusion which are absent in the solutions of HHE which
- Fowief assumes only an effective rs. As dimensionless time in-
0.6 creases to 1.O, the Fourier limit predicts a steady-state tem-
--El- Hyperbolic
a perature profile. Note that if the phonon transport is purely
0.4
ballistic, r= 1 corresponds to the time it takes for the pho-
nons emitted from one boundary to reach the other. The
temperature discontinuity wave predicted by the HHE
reaches only c-O.6 with very little amplitude decay. This
is because the speed of heat wave propagation is v/v’3 as
-0.2 ’ * ’ m ’ * ’ * ’ - ’
0.0 0.2 0.4 0.6 0.6 1.0 discussed earlier in Sec. III. The EPRT predicts that the
1.2) . , . I - ‘ - I * ,
effect of the temperature increase at the boundary {=O,
begins to affect the vicinity of G$=1.0.
1.0 At steady state, it is clear that both the Fourier limit
and HHE show the same linear temperature profile as can
be seen from the solutions in Eqs. (8) and ( 14). Temper-
0.6
ature jumps at the boundaries are not predicted by either of
a these’methods. In contrast the EPRT predicts the temper-
0.4 ature jumps that are observed in the Monte Carlo simula-
tion of Klitsner et a2.l Dimensionless temperature jumps of
0.2 0.2 at both the boundaries were calculated by the EPRT
=--O- EPRT
- Foufier for a film thickness of 0.1 pm. The time to reach 99.99% of
0.0
+ Hypebolic steady state was ~~~“0.7 for Fourier law, qs =20 for the
-0.2 HHE, and rss=13.55 for the EPRT. The response of the
0.0 0.2 0.4 0.6 0.6 1.0 material to sudden changes in boundary conditions, pre-
dicted by the EPRT, is much slower than that of Fourier
1.2, . I . , - I ’ I - ,
limit because heat waves travel at a finite speed. However
L=O.lpm Steady State
it is faster compared to the HHE because the heat wave
I L
--O- EPRT predicted by the HHE moves at a speed of v/u”J and con-
r
0.6 -D- Fourier, Hyperbolic tinues to get reflected from both the boundaries. Since the
thickness of the film is small compared to the mean free
0.6
path, the heat wave has to undergo multiple reflections
a
before its amplitude attenuates sufficiently and steady state
0.4
is reached; hence, the response is slower. Phonon reflection
0.2 is not observed in the EPRT because the boundaries are
assumed to be thermalizing black boundaries and not re-
0.0 flecting boundaries.
Figure 5 shows the temperature profiles in a diamond
-0.2
0.0 0.2 0.4 0.6 0.6 1.0 film of thickness L= 1.0 pm at dimensionless times of
5 r=O.l, r= 1.0, and steady state. This figure is qualitatively
similar to Fig. 4. The Fourier law again predicts a well-
established temperature profile within the film compared to
both the HHE and the EPRT at all the times shown. The
FIG. 4. Variation of dimensionless temperature profiles predicted by the
EPRT, Fourier law, and hyperbolic heat equation as functions of dimen- most obvious difference is that the HHE predicts the tem-
sionless time for a diamond tilm of thickness 0.1 pm. Here 8= (T- To)/ perature wave to attenuate because of stronger diffusion
(Tt - Te), r=t/(Z/u) and 9=x/L. The wave nature of hyperbolic heat effects. The time to reach 99.99% of steady state predicted
equation and the ballistic transport in the form of temperature jumps at
the boundaries predicted by EPRT is clearly seen. The Fourier law clearly
by the Fourier law and HHE is rss=7 and by the EPRT is
overpredicts the rate of evolution of temperature protiles. rss=47.5. The reason for a faster response by the HHE
compared to the smaller-thickness case is that the ampli-
tude decay is substantial due to more dominant diffusion
law predicts a well-established temperature profile within effects arising from larger film thickness such that multiple
the film thickness. The HHE as expected predicts a tem- reflections from the boundaries are negligible. The temper-
perature discontinuity traveling as an attenuating wave ature jump predicted by the EPRT ( -0.03) is also con-
across the film thickness. The amplitude attenuates because siderably less than for the case of smaller thickness.
of diffusion. The EPRT predicts a temperature rise at the Figure 6 shows the temperature profiles in a diamond
boundary f;=O, decaying due to diffusion to the initial tem- film of thickness L = 10 pm at dimensionless times of r= 1,
perature near 6=0.2. Although the EPRT is also a wave r= 10, and steady state. The temperature profiles are quite
36 J. Appl. Phys., Vol. 74, No. 1, 1 July 1993 A. A. Joshi and A. Majumdar 36
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0.8
* EPRT 0.8 * EPRT
- Fourier IA - Fcurler
0.6 * Hyperbolic 0.6 - * Hyperbolic
CD a
0.4 0.4 -
0.2
0.0
-0.2’ * ’ * ’ ’ ’ . ’ * ’ -0.2 ’ * ’ * ’ - ’ * ’ =
0.0 0.2 0.4 0.6 0.8 1.0 0.0 0.2 0.4 0.6 0.8 1.0
1.2 1.21 . g . , . , . 1 .
L= 10pm z=lO
* EPRT
0.8 0.8 - ~- v- 9~ F
rcuner
0.8 0.6 - -Q- Hyperbolic
(D a
0.4 0.4 -
0.2 -
0.0 0.0 -
-0.2 -0.2 1
0.0 0.2 0.4 0.8 0.8 1.0 0.0 0.2 0.4 0.6 0.8 1.0
1.21 . , . , . , . , . 1.23 . , . , . , . , .
1.0 1.0
- EPRT * EPRT
0.8 0.8
* Fourier, Hyperbolic -Cl- Fourier, Hyperbolic
0.6 0.6
CD a
0.4 0.4
9.2 0.2
0.0 0.0
-0.2’ . ’ . ’ * ’ . ’ * ’ -0.2 1
0.0 0.2 0.4 0.6 0.8 1.0 0.0 0.2 0.4 0.8 0.8 1.0
5 5
FIG. 5. Variation of dimensionless temperature protiles predicted by the FIG. 6. Variation of dimensionless temperature profiles predicted by the
EPRT, Fourier law, and hyperbolic heat equation as functions of dimen- EPRT, Fourier law, and hyperbolic heat equation as functions of dimen-
sionless time for a diamond film of thickness 1 pm. The definitions of 0, sionless time for a diamond film of thickness 10 pm. The definitions of 8,
r, and 6 are as defined in Fig. 4. The wave nature of hyperbolic nature is r, and 5 are as defined in Fig. 4. Diffusion effects are clearly evident. Here
decreased due to diffusion. Temperature jumps predicted by the EPRT again the rates of evolution of temperature profiles predicted by the Fou-
are also much lower due to diffusion. The Fourier law again overpredicts rier law and HHE are much higher compared to EPRT.
the rate of evolution of the temperature profiles.
37 J. Appl. Phys., Vol. 74, No. 1, 1 July 1993 A. A. Joshi and A. Majumdar 37
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--C-- EPRT --0- EPRT
---Fwfer
--Cl- Hyperbolic
_.
f
*g lo-’
2 ;O-J
*.,,,,,,)
,,,,,,,,
,,,,,,,,
,;,.,.,,,
.,,_
s ,,.22
10” 1o’2 10-l lo0 10’ IO2 10” ,10-’ 10-l loo 10’
Nondimensional Time, ‘C Nondimensional Time, Z
FIG. 7. Variation of dimensionless wall heat flux, Q=q/o( T;‘- 7$, as a FIG. 8. Variation of dimensionless wall heat Bux defined in Fig. 7 as a
function of dimensionless time defined in Fig. 4 for a diamond film of function of dimensionless time defined in Fig. 4 for a diamond film of
thickness 0.1 pm. The Fourier law clearly overpredicts wall heat flux and thickness 1 pm. The Fourier law again clearly overpredicts wall heat flux
the HHE underpredicts it as small time scales. At steady state both the and the HHE underpredicts it as small time scales. At steady state both
classical laws overpredict the wall heat tlux as has been demonstrated by the classical laws underpredict the wall heat flux slightly.
Majumdar (see Ref. 8).
terms with respect to time shown in Eq. (8) until steady tions match exactly after dimensionless time of r- 1. This
state is reached. The nondimensional boundary heat flux is because the wavelike nature of the temperature discon-
predicted by the EPRT remains constant at about 2 for tinuity predicted by the HHE is dominant early on when
r < 0.1. During this period, the intensity wave emitted from the heat wave has not decayed substantially. The boundary
one boundary does not reach the other boundary. Between heat flux predicted by the EPRT decays with time until it
0. 1 < r < 1, the dimensionless boundary flux decreases due reaches steady state; however, under transient conditions,
to diffusion and thermalization at the film surface. The the flux predicted by the EPRT is more than that predicted
boundary flux then reaches the steady state value of 1 at by Fourier law. The reason is that since the transient re-
r> 1 in accordance to the Casimir limit. The boundary sponse of the EPRT is slower than the Fourier law, the
heat flux predicted by the HHE, however, initially decays temperature gradient predicted by the EPRT is always
weakly with time, but later starts to oscillate while being more than that predicted by the Fourier law at any time
decayed at the same time as can be seen in Eq. ( 15). This before reaching steady state. Since in acoustically thick
can be explained as follows. At small times, the tempera- films the heat flux is proportional to the temperature gra-
ture gradient at the wall is very small; therefore, when Eq. dient, a higher-temperature gradient implies a larger heat
(9) is evaluated for the boundary heat flux, the right-hand- flux.
side term can be neglected, leading to an exponential decay
with respect to time. As time increases the heat wave
emerging at the boundary c=O in the reflection of the
wave which arrives at g=O after reflecting from g= 1 with
102e . “.‘..‘I . “..“1 . ..““‘( “.“.“I . “‘.“,I ’ “““I
a decayed amplitude. This leads to a higher-temperature
gradient at the boundary and the boundary heat flux in- r-
LI- 10n.m
--O- EPRT
creases. These multiple reflections of the temperature wave x 10’ -l=Wkf
cause oscillations in the boundary heat flux which eventu- 2
: F
--Cl- Hyperbolic
ally decay.
Figure 8 shows the variation of the dimensionless
boundary heat flux as a function of time for a film of thick-
ness 1.0 pm. This figure is similar to Fig. 7 qualitatively
except for the results of HHE. In this figure, the heat flux
decays at a higher rate for the HHE compared to Fig. 6
because of more dominant diffusion effects. In this case
also the heat wave emerging at the boundary c=O, reflects
off from the boundary c=l and arrives at c=O causing an Nondimensional Time, Z
increase in temperature gradient. However, here the heat
wave has attenuated substantially and the increase in wall FIG. 9. Variation of dimensionless wall heat flux defined in Fig. 7 as a
function of dimensionless time defined in Fig. 4 for a diamond tilm of
heat flux is not as much as in the previous case. thickness 10 pm. The HHE underpredicts the wall heat flux at small time
Figure 9 shows the boundary heat flux results for a film scales. At steady state both the classical laws underpredict the wall heat
of thickness 10 pm. The HHE and the Fourier law predic- flux slightly.
38 J. Appl. Phys., Vol. 74, No. 1, 1 July 1993 A. A. Joshi and A. Majumdar 38
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V. SUMMARY AND CONCLUSIONS ported by the National Science Foundation. A. Majumdar
gratefully acknowledges the support of NSF through the
To analyze phonon heat transport under both short Young Investigator Award.
time and spatial scales, this study develops an equation of
phonon radiative transfer (EPRT) similar to the one used
for photons in thermal radiative transfer. This equation
was used to study the transient thermal response of dia-
mond thin films under ballistic and diffusive phonon trans- ’S. M. Sze, Ph.ysicsof Semiconductor Devices, 2nd ed. (Wiley, New York,
port. The results of the EPRT indicate a wavelike response 1981).
for phonon intensity and temperature which under ballistic ’W. W. Duley, Laser Processing and Analysis of Materials (Plenum, New
York, 1983).
transport decays to a steady-state temperature profile with ’W. Kurz and D. J. Fisher, Fundamentals of Solidification (Tram-Tech,
temperature jumps at the boundaries. The jumps are in Zurich, 1989).
accord with Monte Carlo simulations and are characteris- 4J. M. Ziman, Electrons and Phonons (Oxford University Press, London,
tic of ballistic phonon transport. Comparison of results 1960).
with that of the Fourier law and the hyperbolic heat equa- 5H. B. G. Casimir, Physica 5, 495 ( 1938).
‘R. Siegel and J. R. Howell, ThermaI Radiation Heat Transfer, 2nd ed.
tion (HHE) suggest the following: (i) The Fourier law (Hemisphere, New York, 1982).
assumes diffusive transport and infinite wave speed and ‘T. Klitsner, J. E. VanCleve, H. E. Fischer, and R. 0. Pohl, Phys. Rev.
cannot be used for heat transport for short time and spatial B 38, 7576 (1988).
scales; (ii) the HHE predicts the wavelike solution but not *A. Majumdar, J. Heat Transfer 115, 7 (1993).
‘M. N. Ozisik, Radiative Transfer and Interactions with Conduction and
the temperature jumps under ballistic transport, therefore,
Convection (Wiley, New York, 1973).
the HHE could be used for transport under short time “D. D. Joseph and L. Preziosi, Rev. Mod. Phys. 61, 41 (1989).
scales but not for short spatial scales; (iii) the EPRT can “F. Claro and G. D. Mahan, J. Appl. Phys. 66,4213 (1989).
be used to study heat transport under both short time and “N. W. Ashcroft and N. D. Mermin, Solid State Physics (Saunders,
spatial scales. Philadelphia, 1976).
“Y. S. Touloukian and E H. Buyco, Thermophysical Properties of Matter
Under a sudden temperature jump at a lilm surface, (IFI/Plenum, New York, 1970), Vol. 5.
the EPRT predicts that the surface heat flux could be as 14C. Kittel, Introduction to Solid State Physics, 6th ed. (Wiley, New York,
high as twice the steady-state Casimir limit for ballistic 1986).
transport. The EPRT predictions also show that heat flux “J. Callaway, Phys. Rev. 113, 1046 (1959).
results can be significantly different from those predicted I6 J . H . Jeans, The Dynamical Theory of Gases, 4th ed. (Dover, New York,
1954), p. 257.
by the Fourier law and the HHE. “D. Walton and E. J. Lee, Phys. Rev. 157, 720 ( 1967).
“P. G. Klemens, in Solid State Physics, edited by F. Seitz and D. Turn-
ACKNOWLEDGMENTS bull (Academic, New York, 1958), Vol. 7, pp. l-98.
“T . R . Anthony, W. F. Banholzer, J. F. Fleischer, L. Wei, P. K. Kuo, R.
The authors would like to thank M. Kulkarni (Ari- L. Thomas, and R. W. Pryor, Phys. Rev. B 42, 1104 (1990).
zona State University) for his help. This work was sup- *‘M. I. Flik and C. L. Tien, J. Heat Transfer 112, 872 (1990).
39 J. Appl. Phys., Vol. 94, No. 1, 1 July 1993 A. A. Joshi and A. Majumdar 39
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