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VOLUME 18, NUMBER 23 PHYSICAL REVIEW LETTERS 5 JUNE 1967

i s e to give detailed information on the conduc- edited by J. G. Daunt, D. O. Edwards, F. J. Milford,


t i o n - e l e c t r o n spin-flip c o r r e l a t i o n time in the and M. Yaqub (Plenum Press, New York, 1965), p. 933;
ground state and will be c o n s i d e r e d in detail G. Knapp, J. Appl. Phys. 38, 1267 (1967); M. D. Day-
in a subsequent publication. bell and W. A. Steyert, Phys. Rev. Letters 18, 398
(1967).
We would like to thank D r . M. D. Daybell and 5
M. A. Ruderman and C. Kittel, Phys. Rev. 96, 99
D r . W. A. Steyert for communication of t h e i r (1954); T. Kasuya, Progr. Theoret. Phys. (Kyoto) Jj>,
r e s u l t s p r i o r to publication; P r o f e s s o r J . R. 45 (1956); K. Yosida, Phys. Rev. 106, 893 (1957).
6
Schrieffer for continued i n t e r e s t in t h e s e e x p e r - Note that there is a correlated spin density within a
i m e n t s ; and P r o f e s s o r P . P i n c u s for s e v e r a l coherence length of the impurity but this spin density,
helpful d i s c u s s i o n s . We also thank M r . T o m being part of the singlet, is flipping quantum mechani-
cally at a high frequency and will not contribute to the
Lake for m e a s u r i n g the r e s i s t i v i t y r a t i o of the
Cu nmr linewidth. We also note that the spatial spin
Cu:Fe s a m p l e . P r o f e s s o r K. Yosida kindly correlation found from the variational solution of Ref. 3
supplied u s with a p r e p r i n t of h i s s u s c e p t i b i l - is identical with those found by Nagaoka (Ref. 2) and by
ity calculation p r i o r to publication. Takano and Ogawa (Ref. 2).
7
H. Suhl, Solid State Commun. 4, 487 (1966).
8
*A contribution from the Laboratory for Research on J. Owen, M. Brown, W. D. Knight, and C. Kittel,
the Structure of Matter, University of Pennsylvania. Phys. Rev. 102, 1501 (1956); T. Sugarawa, J. Phys.
Work supported by the Advanced Research Projects Soc. (Japan) 14, 643 (1959).
9
Agency; the Air Force Office of Scientific Research, J. Friedel, Metallic Solid Solutions (W. A. Benjamin,
Office of Aerospace Research, U. S. Air Force, under Inc., New York, 1963), Chap. XIX.
10
Grant No. AF-AFOSR-1149-66; and the National Sci- Takano and Ogawa, Ref. 2; A. J. Heeger and M. A.
ence Foundation under Grant No. NSF GP4178. Jenson, to be published; K. Yosida and H. Ishii, to be
1
J. Kondo, Progr. Theoret. Phys. (Kyoto) 32, 37 published.
U
(1964). J. P. Franck, F. D. Manchester, and D. L. Martin,
2
P. W. Anderson, J. Appl. Phys. 37, 1194 (1966). Proc. Roy. Soc. (London) A263, 499 (1961).
12
Y. Nagaoka, Phys. Rev. 138, A1112 (1965); Progr. G. White, Can. J. Phys. 33, 119 (1955).
13
Theoret. Phys. (Kyoto) 37, 13 (1967). K. Yosida, M. W. Klein and R. Brout, Phys. Rev. 132, 2412
Progr. Theoret. Phys. (Kyoto) 36, 875 (1966). F. Taka- (1963).
14
no and T. Ogawa, Progr. Theoret. Phys. (Kyoto) 3j5, J. A. Cureaga, B. Dreyfus, R. Tournier, and
343 (1966). J. R. Schrieffer, J. Appl. Phys. 3_8, 1143 L. Weil, in Proceedings of the Tenth International Con-
(1967). J. Kondo, Progr. Theoret. Phys. (Kyoto) 36>, ference on Low Temperature Physics (to be published).
15
429 (1966). P. W. Anderson, Phys. Rev. 124, 41 (1961).
3 16
A. J. Heeger and M. A. Jensen, Phys. Rev. Letters It should be noted that the resistivity results are
18, 488 (1967). also in agreement with the resonant-scattering theory
4 as worked out by H. Suhl and D. Wong, Physics 3*, 17
G. J. Van den Berg, in Proceedings of the Ninth In-
ternational Conference on Low Temperature Physics, (1967); H. Suhl, Phys. Rev. Letters JL8, 743 (1967).

RELAXATION AND RECOMBINATION TIMES OF QUASIPARTICLES


IN SUPERCONDUCTING Al THIN FILMS
B a r r y I. Miller and Aly H. Day em
Bell Telephone Laboratories, Murray Hill, New Jersey
(Received 14 April 1967)

Recently 1 t h e r e h a s been c o n s i d e r a b l e i n t e r - i s accompanied by the e m i s s i o n of a phonon


e s t in the decay of excited q u a s i p a r t i c l e s in of energy 2A.4>5
s u p e r c o n d u c t o r s . It h a s been conjectured 1 that We have m e a s u r e d for the f i r s t t i m e r ^ in
an excited q u a s i p a r t i c l e of energy E decays thin aluminum films at 0.37°K and find that
v i a a t w o - s t e p p r o c e s s . The f i r s t c o n s i s t s of Tj d e c r e a s e s exponentially a s a function of
a r e l a x a t i o n in t i m e rT to energy A, w h e r e ( £ - A ) / A and is - 0 . 5 X 1 0 " 8 s e c at ( £ - A ) / A = 1.0.
2A i s the energy gap of the s u p e r c o n d u c t o r . We have a l s o m e a s u r e d r ^ a s a function of
This p r o c e s s o c c u r s p r i m a r i l y by e m i s s i o n t e m p e r a t u r e and find that at 0.37°K, r ^ ~ 1.0
of a phonon of energy £ - A . 2 > 3 The second s t e p x 10~ 6 s e c and that it d e c r e a s e s with i n c r e a s -
i s r e c o m b i n a t i o n in t i m e rR of two q u a s i p a r - ing t e m p e r a t u r e up to T ~ 1.2°K. At t e m p e r a -
t i c l e s at energy A to form a Cooper p a i r and t u r e s above 1.2°K,6 rR a p p e a r s to i n c r e a s e

1000
VOLUME 18, NUMBER 23 PHYSICAL REVIEW LETTERS 5 JUNE 1967

In Fig. 2 we show a series of I-V curves tak-


en on diode 2 at 0.37°K for various voltages
on diode 1. Here Ax = 0.221 mV and A2 = 0.571
mV. We note that for F 1 = 2A1 (curves 0 to 10)
all the curves are similar to one another. For
these biases on diode 1 all the injected quasi-
particles are at E ~ Ax and the change in the
quasiparticle population is proportional to TR.
At biases where Vx>2AX we note that in the
region F 2 <A 2 -A 1 each curve deviates from
i s
* predecessor, in contrast to the similarity
between the curves obtained at F 1 = 2A1. These
deviations occur for the following reason. The
FIG. 1. Sample geometry. injected quasiparticles are now in the energy
slightly. range A1<E<V1-AX. Because of the singular-
The measurements were performed on two ities in the quasiparticle density of states in
superimposed superconducting tunnel diodes the Al films, the injected quasiparticle distri-
(Al/Al 2 0 3 /Al/Al 2 0 3 /In in the present case) bution will have one singularity at E = Vx-Ax
formed by the successive evaporation of three and another at E = A r The singularity at E = Vx
film stripes as shown in Fig. 1. Care was tak- -Ax should, according to theory, produce a
en to insure that the top and bottom stripes jump in the current I2 at V2= VT = A1 + A2-VV
were not in contact. The Al/Al 2 O s /Al diode The height of this jump should be proportion-
(diode 1) is biased such that quasiparticles al to rT(E). Experimentally this jump is round-
are injected into the center aluminum stripe ed off and shows up as a deviation between the
and, depending on the relaxation and recombi- successive curves depicted in Fig. 2. The round-
nation times, causes an increase in the steady- ing off of the current jump is probably due to
state quasiparticle distribution in the center thermalization and the finite width of the In
film. This new distribution is probed by the gap edge (30 /iV).
second diode (Al/Al 2 0 3 /In) and shows up on In order to evaluate r^ we consider only those
its I-V characteristic. 7 In order to obtain a curves corresponding to injection at F 1 = 2A1.
measurable change in the I-V curve due to in- For a given injection current I19 the number
jection, it is necessary to make the center of excited quasiparticles tunneling into the mid-
stripe as thin as possible. dle stripe is not proportional to Iv but rather

V.,(nnV) I^mA)
0 0 0
2 2A 0.2
4 2A 0.4
6 2A 0.6
8 2A 0.8
10 2A +0.091A 1.0
12 2A +0.140A 1.2
14 2A +0.348A 1.4
16 2A +0.584A 1.6
18 2A +0.835A 1.8
20 2A + 1.040A 2.0

V2 (MICROVOLTS)

FIG. 2. I-V curve for diode 2 (Al/Al 2 0 3 /In) for different values of injection biases on diode 1 at 0.37°K. V? is
indicated for curve 14.
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VOLUME 18, NUMBER 23 PHYSICAL REVIEW LETTERS 5 JUNE 1967

to (Ix-I±°), w h e r e Ij° i s the contribution of t h e r - bination time i s given by


mally excited p a r t i c l e s . R e f e r r i n g to the s e m i -
A1ev(l)AI2(VR)
conductor model of excitations in a s u p e r c o n -
(1)
ductor, one can easily find that the c u r r e n t R A12 lAC^-IJ >
due to t h e r m a l l y excited p a r t i c l e s i s composed
w h e r e AfyiVft) i s the change of I2 c o r r e s p o n d -
of two equal p a r t s , one c r e a t i n g and the other
ing to a given injection c u r r e n t It; v(l) and^4 x
d e s t r o y i n g an equal n u m b e r of excited q u a s i -
a r e the volume and a r e a , r e s p e c t i v e l y , of the
p a r t i c l e s in the middle film. We a s s u m e , t h e r e -
second s t r i p e common to diode 1; A12 i s the
fore, that at F 1 = 2A 1 a l l the injected q u a s i p a r -
a r e a of the c e n t e r s t r i p e common to diodes
t i c l e s lie in a n a r r o w energy band at the top
1 and 2 (see F i g . 1); and C = v2(oo)/2eN1(0) is
of the Al gap. In the steady state the change
a constant for a given diode. H e r e a2(°°) i s the
in the c u r r e n t I2 at any b i a s F 2 ^ A 2 - A 1 i s p r o -
conductivity of diode 2 in the high-voltage l i m -
portional to T^il^Ij0). B e c a u s e of the i n s t a - it, and 2 ^ ( 0 ) = 3.33X10 22 eV""1 c m " 3 i s the n o r -
bility n e a r the negative r e s i s t a n c e region we m a l density of s t a t e s for both spins in Al. 8 In
choose a fixed b i a s F 2 = 0.6 mV which l i e s at our c a s e C = 1.97xl0~ 2 4 C s e c ^ 1 c m 3 for the
a stable point in the t e m p e r a t u r e range of i n - diode used in r u n 12.
t e r e s t . At this b i a s the q u a s i p a r t i c l e s n e a r
In o r d e r to obtain r^{E) it i s n e c e s s a r y to
the top of the Al gap tunnel to the In film into
compute the jump in c u r r e n t I2 expected at F 2
a fairly constant density of s t a t e s whose v a l -
= F ^ = A^ + A 2 - F ^ and then c o m p a r e with the
ue is 1.4 t i m e s the n o r m a l state density. With
e x p e r i m e n t a l jump. F r o m tunneling theory 9
t h i s in mind it i s easy to show that the r e c o m -
one finds that the jump in c u r r e n t i s p r o p o r t i o n -
al to

1 1 fFi-e (E-V^E
[E-V^E + V^dE
+ V^dE V
K11--A
A11 71
W= lim

If we denote the m e a s u r e d i n c r e m e n t in c u r r e n t
at VT = A2 + A1-Vi by AI2(VT) then which gives a much s t r o n g e r t e m p e r a t u r e d e -
pendence than that indicated in Fig. 3(a). We
AI^V^N^vd) Ax
find that for A / k T > 3, rR~exp(0.3A/£T). At
r (V - A ) (2)
Wo i H a ^ o o ) A12 p r e s e n t we a r e unable to account for this d i s -
crepancy.
Since we a r e i n t e r e s t e d in the s t e a d y - s t a t e
In F i g . 3(b) we plot rT v s ( E - A 1 ) / A 1 at 0.37°K.
population at E = V1-A1 due to the r e l a x a t i o n
We find that r T ( E - A ) = l . l l x l O " 7 e x p [ ~ 3 . 3 4 ( E
from E = F 1 ~A 1 , any e x c e s s population from
- A ) / A ] . The fact that rT i s at l e a s t an o r d e r
t h e r m a l t a i l s extending up from e n e r g i e s E < Vx
of magnitude l e s s than Tn m e a n s that all inject-
- A 1 m u s t be taken out. We find that the best
ed q u a s i p a r t i c l e s f i r s t r e l a x to the top of the
way to achieve this i s to take A^iVj) a s the
gap and then r e c o m b i n e a s d i s c u s s e d e a r l i e r .
difference in c u r r e n t at Vrp between the given
In the p r e s e n t e x p e r i m e n t it i s difficult to m e a -
curve and i t s p r e d e c e s s o r , the l a t t e r c u r r e n t
s u r e TT a s a function of t e m p e r a t u r e b e c a u s e
being n e a r l y equivalent to the t h e r m a l tail o r i g -
inating from e n e r g i e s E< 7 1 - A 1 . of the l a r g e t h e r m a l q u a s i p a r t i c l e population
at higher t e m p e r a t u r e s .
In F i g . 3(a) r ff i s plotted a s a function of t e m -
Several f a c t o r s have to be taken into account
p e r a t u r e . r ^ w a s d e t e r m i n e d by plotting A ^ ^ )
in d e t e r m i n i n g T ^ and r^ by the p r e s e n t m e t h -
v s Ix a t v a r i o u s t e m p e r a t u r e s and taking the
od. These a r e (1) heating of the diode by the
slope of this curve a s (I^Ij0) goes to 0. Thus
we obtain the dependence of Tp on t e m p e r a t u r e dc power input, (2) diffusion of the q u a s i p a r -
in the limit of z e r o injection. The t e m p e r a t u r e t i c l e s away from the common a r e a of the diode,
dependence of r ^ h a s been calculated by Schrief- and (3) l o s s of excited q u a s i p a r t i c l e s in the
fer who finds that for A/kT» 1 c e n t e r film due to s t r a i g h t through tunneling 1 0
w h e r e an injected q u a s i p a r t i c l e t r a v e r s e s the
r ~(A/£T)1/2exp(A/£T), second film and tunnels d i r e c t l y into the top
H

1002
V O L U M E 18, N U M B E R 23 PHYSICAL REVIEW LETTERS 5 JUNE 1967

1 1 1 1 than the width of the s t r i p e s . Diffusion e r r o r s

IT]
8 • RUN 12 a r e thus only about 10%. The s t r a i g h t - t h r o u g h
o RUN 13
6 tunneling p r o c e s s will give r i s e to an e x c e s s
c u r r e n t I0 in addition to I2 and m a k e s rR ; and
4 (a) •{ rT appear l a r g e r . We find that I2r/I2< 10~ 5 .
3
i The o v e r - a l l absolute e r r o r s in m e a s u r i n g
TR and Tj, a r e about 30% and come mainly from
e r r o r in m e a s u r i n g film t h i c k n e s s . We a l s o
H
studied the v a r i a t i o n of A^iV^) o v e r a wide
r a n g e of injection c u r r e n t Ix at v a r i o u s t e m p e r -
a t u r e s . The c u r v e s obtained have a n u m b e r
icr7
of i n t e r e s t i n g f e a t u r e s which will be d e s c r i b e d
8
in a l a t e r publication. Among t h e s e f e a t u r e s
i i 1
6 i 1 1 1 1 1
we find the following: (1) &I2(VR) = ° f o r h"1i°
A/kT < 0 showing that indeed the c u r r e n t from t h e r -
mally excited q u a s i p a r t i c l e s does not produce
6 - \ net excitations in the middle film. (2) F o r the
4
- r a n g e of v a l u e s of Ix at F 1 ~ 2 A 1 , the behavior
\
of AiV^t 7 ^) is such as to show c l e a r l y the d e -
2
\ c r e a s e of TR with i n c r e a s i n g steady state q u a -
s i p a r t i c l e population. This is p a r t i c u l a r l y p r o m
10"8 - \ inent at low t e m p e r a t u r e s w h e r e the original
„ 8 t h e r m a l population is r e l a t i v e l y s m a l l .
16 \ In conclusion, we have developed a method
by which we have m e a s u r e d rR and T™ a s a
4
(b) \ function of t e m p e r a t u r e and energy, r e s p e c t i v e -
-
ly. In addition to this we a r e able to m e a s u r e
2 the dependence of 7v> on q u a s i p a r t i c l e density
\ at a given t e m p e r a t u r e and the energy profile
of the excited q u a s i p a r t i c l e s . By using t h e s e
10"» .. „ 1 1. I 1 1
techniques we a r e b e t t e r able to u n d e r s t a n d
the q u a s i p a r t i c l e r e l a x a t i o n and r e c o m b i n a t i o n
p r o c e s s e s in s u p e r c o n d u c t o r s . In the future
FIG. 3. (a) Plot of TR vsA/kT. T h e indicated e r -
we plan a further study of Al a s well a s other
r o r s a r e r e l a t i v e e r r o r s only, (b) Plot of TJ« VS ( E ~ A ) /
A at 0.37°K. T h e indicated e r r o r s a r e r e l a t i v e only. s u p e r c o n d u c t o r s using t h e s e t e c h n i q u e s .
We wish to thank S. J . Buchsbaum, P . K.
Tien, P. W. Anderson, W. L. McMillan, and
film (In). Heating will c a u s e the total n u m b e r B. N. Taylor for many valuable d i s c u s s i o n s ;
of q u a s i p a r t i c l e s to r i s e and will thus cause a l s o W. R. Wolff, J . J . Wiegand, and M r s . A A.
Tft and rT to a p p e a r l a r g e r than they a r e . A P r i t c h a r d for technical a s s i s t a n c e . We a l s o
s e r i e s of m e a s u r e m e n t s w e r e made on the r i s e wish to thank B . N . Taylor for a copy of his
in t e m p e r a t u r e of the middle film a s a function unpublished t h e s i s .
of injected power by noting the change of the
Al e n e r g y gap, a s m e a s u r e d by diode 1, a s
*W. E i s e n m e n g e r and A. H. Dayem, P h y s . Rev. L e t -
a function of input power from diode 2. In this t e r s 1 8 , 125 (1967).
way we w e r e able to e s t i m a t e the heat r i s e of 2
J . B a r d e e n , G. Rickayzen, and L. T e w o r d t , P h y s .
the middle film and we find that any e r r o r i n - Rev. JL13, 982 (1959).
3
troduced by heating is l e s s than 10% at the i n - L . Tewordt, P h y s . Rev. 127, 371 (1962); 128, 12
jection levels used in d e t e r m i n i n g rR and r ^ . (1962).
4
Diffusion will r e d u c e the number of q u a s i p a r - J. R. Schrieffer and D. M. G i n s b e r g , P h y s . Rev. L e t -
t e r s 13, 204 (1962); D. M. G i n s b e r g , P h y s . Rev. L e t t e r s
t i c l e s p r e s e n t and thus cause rR and rT to a p -
_8, 207 (1962).
p e a r s m a l l e r than they a r e . We find the dif- 5
It i s also possible for the r e c o m b i n a t i o n to o c c u r via
fusion length of q u a s i p a r t i c l e s in the middle photon e m i s s i o n . E. B u r s t e i n , D. N. Langenberg, and
film to be about 2 x i 0 ~ 3 cm, much s m a l l e r B. N. T a y l o r [Phys. Rev. L e t t e r s (B, 92 (1961)] have

1003
V O L U M E 18, N U M B E R 23 PHYSICAL REVIEW LETTERS 5 JUNE 1967

shown that photon e m i s s i o n lifetime ~0.4 s e c in Pb ' T h i s i s the s a m e method u s e d by B. T a y l o r to m e a -


which i s much s m a l l e r than t h e phonon lifetime ~ 1 0 ~ 7 s u r e r e c o m b i n a t i o n t i m e s in Al. B . T a y l o r , t h e s i s ,
s e c (see Ref. 4). University of Pennsylvania, 1962 (unpublished).
6 8
T h e t r a n s i t i o n t e m p e r a t u r e for t h e s e films was T . P . Sheenen, P h y s . Rev. 149, 370 (1966).
9
~1.45°K. We find that 2A(0)/kTc ~ 3.5. See B. A b e l e s , I. Giaever and K. M e g e r l e , P h y s . Rev. 122, 1101
R. W. Cohen, and G. W. Cullen, P h y s . Rev. L e t t e r s JL7, (1961).
10
631 (1966). B. N. T a y l o r , P r i v a t e communication.

H O T - E L E C T R O N - P H O N O N I N T E R A C T I O N S IN G a P

E . M. C o n w e l l
Bayside Laboratory,
R e s e a r c h C e n t e r of General Telephone & E l e c t r o n i c s L a b o r a t o r i e s I n c o r p o r a t e d ,
B a y s i d e , New York
(Received 24 A p r i l 1967)

In a r e c e n t L e t t e r , W i l l i a m s and Simon 1 c l a i m only important s c a t t e r i n g p r o c e s s , even in r e l -


to have d e t e r m i n e d by d i r e c t m e a s u r e m e n t the atively p u r e m a t e r i a l , since the mobility c a l -
m e a n free path for e n e r g y l o s s to phonons of culated for this m e c h a n i s m i s g r e a t e r than the
e n e r g e t i c e l e c t r o n s in G a P . The mean free o b s e r v e d mobility. 4 ' 5 It h a s been speculated
path they obtain i s , however, of questionable that acoustic deformation-potential s c a t t e r i n g
significance since it i s based on a g r e a t l y o v e r - i s the other p r o c e s s of i m p o r t a n c e , 5 but it could
simplified view of h o t - e l e c t r o n t r a n s p o r t in well be that that p r o c e s s i s s c a t t e r i n g among
this m a t e r i a l . T h i s i s t r u e also of p r e v i o u s the equivalent (100) v a l l e y s . The l a t t e r i s the
d e t e r m i n a t i o n s of t h i s m e a n free path. 2 predominant s c a t t e r i n g p r o c e s s for the (100)
It i s a s s u m e d by W i l l i a m s and Simon that m i n i m a in silicon. In support of this hypoth-
the e n e r g y l o s s p e r collision i s 0.050 eV, the e s i s , Epstein 6 notes that the Hall mobility at
longitudinal optical (LO) phonon energy at the 300° and above shows a somewhat s t r o n g e r
c e n t e r of the Brillouin zone. 3 This type of p h o - t e m p e r a t u r e dependence than could be a c c o u n t -
non may well be predominant for l o s s e s of low- ed for by a combination of polar and i n t r a v a l -
e n e r g y e l e c t r o n s . P o l a r optical s c a t t e r i n g i s ley a c o u s t i c - m o d e s c a t t e r i n g .
known to be important at low fields in GaP at The r a t e of e n e r g y l o s s of an e l e c t r o n of e n -
room t e m p e r a t u r e . 4 ' 5 It i s not, however, the e r g y & to polar modes i s 7

dS
AN + i)cosh-1L -N - s i n n " 1 '
IF
po
(2mS)1/2 L ql
7
\K(JQ, ql \#a>, a)
w h e r e e i s the e l e c t r o n i c c h a r g e ; ooi and Nqi the angular frequency and number, r e s p e c t i v e l y , of
LO phonons; and E0 an effective field whose magnitude i s a m e a s u r e of the coupling to the LO p h o -
n o n s . If (1) i s plotted v e r s u s 5 , it is found that for the slowest e l e c t r o n s (dS/dt)^o>0, indicating
net gain. A s S i n c r e a s e s , (dS/dt)„Q b e c o m e s negative and its magnitude i n c r e a s e s . The magnitude
of the l o s s r a t e r e a c h e s a m a x i m u m and then d e c r e a s e s a s S i n c r e a s e s further, eventually a s ln8/8l/z.
F o r G a P t h i s m a x i m u m i s r e a c h e d at S -AHu>i or 0.2 eV. The r a t e of l o s s of e l e c t r o n s in the itti
valley due to i n t e r v a l l e y s c a t t e r i n g i s given by 8

2
dS\ D. (m .) 3 / 2
(2)
It). ~LJ 21/2TIF
T?rp
2
' L
qij ij 0j qtj ij Oj
J
w h e r e the sum i s taken over all possible final v a l l e y s ; D^ and a># "ij a r e the coupling constant and a n -
gular frequency, r e s p e c t i v e l y , for the t r a n s i t i o n i^j; Nqij is the number of phonons with angular

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