Pram.~n.a-J. Phys., Vol. 28, No. 6, June 1987, pp. 661~67 © Printed in India.

Kramers-Kronig type of dispersion relation in nonlinear optics

P SEN and P K SEN

Department of Physics, Bhopal University, Bhopal 462 026, India
MS received31 October 1986; revised 31 March 1987
Abstract. The applicabilityof Kramers-Kronig(K-K) relation under nearly sharp resonant
transition regime in narrow-gap semiconductors has been established and consequently, a
generalized dispersion relation for nonlinear optical susceptibilityof a dielectricis derived.
This relation can be employedin the study of nonlinearoptical processesin solids as wellas in
plasmas over a wide frequencyspectrum.
Keywords. Kramers-Kronigdispersion relation; nonlinear optical susceptibility;nonlinear
refraction; nonlinear absorption.
PACS No. 42.65

1. Introduction

Kramers-Kronig (K-K) dispersion relations which connect the dispersive and

absorptive aspects of matter-radiation interaction processes are extremely useful in
many areas of physics. In particular, the utility of K-K relations in the determination of
different optical constants by reflectivity data as well as in the derivation of sum rules is
well known and needs very few physically well-founded assumptions (Landau and
Lifshitz 1959; Women t972).
The extension of K-K relations to the nonlinear regime is regarded as a difficult and
subtle problem because optical nonlinearity of a medium has been the origin of a
variety of phenomena in contrast to the simple absorptive and dispersive aspects of the
linear material response of the medium. Nonlinear refraction and absorption are two of
the vital properties of the medium which play critical roles in the observation of optical
bistability, optical phase conjugation via degenerate four-wave mixing and pulse
shaping, etc. These phenomena have large technological potential in integrated optics.
The investigations of such nonlinear optical effects could be much simplified if an
analytical tool similar to the K-K relations is available. Unfortunately, no such
relations seems to have yet been established.
The present literature reveals that there is a controversy about the applicability of
K-K relations in the nonlinear regime. Flytzanis (1975) commented that these relations
are applicable even in the nonlinear optical effects but are not so useful as in linear
optics. On the other hand, according to Yariv (1975), these relations are invalid because
of the presence of poles in both the upper and lower halves of complex co-plane and
violate the causality principle in the nonlinear regime. K-K relations were used by
Miller et al (1981) probably for the first time in nonlinear optics under the
approximation that the quantum mechanical phases of the carriers are randomized by
thermalizing collisions. They developed a semi-empirical theory that fits well with
661
662 P Sen and P K S e n

the experimentally Observed band-gap resonant nonlinear refraction in III-V semi-

conductors, viz InSb.
Keeping in view the above discussion, we have dealt with a couple of fundamental
questions: (i) whether the intensity-dependent optical susceptibility (X) can be regarded
as causal or not; (ii)what would have been the form of the K - K relation for the
nonlinear optical susceptibility of a crystal, that could, under band-gap resonant
. (3) )"in terms of the measured nonlinearity in
transition, yield nonlinear refraction (via Xr
absorption (via X~3));(iii) derivation of a generalized form of dispersion relation which
can enable one to estimate the nonlinear refractive index simply from the knowledge of
nonlinear absorption coefficient and vice versa over an arbitrarily wide photon energy
spectrum in a centrosymmetric crystal.

2. T h e o r e t i c a l formulations

To start with, we consider the generalized form of the nth order polarization in terms of
the response function as (Ducuing 1977)

x Ex2(t-z2)... E2.(t-%). (1)

Here, o(.) is the response function of nth order and E2,, E22,
A'~0,,21,22,,,,,2 M
E2. are • • •

the electric field amplitudes of the spatially uniform interacting waves. For an arbitrary
decomposition of the electric field, one can also have

P~")(t) = eo d091 d092 • " " d09. "(")

/~o, 4 1 , 4 2 .... , 2.(091,092,
" " " 09.)

x E2,(091)Ex~(092)... E2.(09.) exp[i(091+092+093 • • • +09.)t], (2)

Z(")
0', AI
being the nth order susceptibility tensor. This generalized expression for
, 22, . • • , 2n

the nth order polarization characterizes almost all possible types of nonlinearities like
nonlinear refraction and absorption (viz., 09; 09; - 09; to), harmonic generation (09. = n09),
sum and difference frequency mixing (viz., 092 = 092 +093), etc.
A relation between the optical susceptibility and the response function can be
obtained by comparing (1) and (2) whence one gets

Z(") 0 . t 2 1 ~ 2 2 , . . . '
2. (091,092, • • •
09,,)

=
f0fo fo d~1 d'c2 . . . dz.R~)~,,a2 . . . . . 2.(T1, z2 . . . . . z.)

x exp[-i(091~ 1 +092z2+ . • • +09.%)]. (3)

Equation (3) clearly indicates that the properties of the reponse function R (") will be
reflected in the corresponding properties of X(").
 Kramers-Kronig relation in nonlinear optics 663

We n o w restrict ourselves to the area of nonlinear refraction and absorption in the

semiconducting crystals duly irradiated by lasers. The total induced polarization can
be expressed as

P(co) = eoZ(Co) E(co) = e o I x u) + Z¢3) IEI 2 4- . . . "1 E(ca), (4)

where E(co) is the Fourier transform of the electric field E(t) of the p u m p laser. We also
assume that the m e d i u m is centrosymmetric in nature such that the nonlinear optical
susceptibilities of even orders (viz., Z ~z), Zt4). . . . ) vanish u n d e r parity considerations.
Nonlinearity expressed by (4) can have its origin in different types of mechanisms like (i)
b a n d nonparabolicity ( K h a n et a11980), (ii) intensity-dependent free electron-hole pair
generation (Jain 1982), (iii)interband transition saturation (Wherrett and Higgins
1982a), (iv)coherent radiation-exciton interaction (Sen 1982), etc.
While addressing ourselves to the question of developing a generalized dispersion
relation in nonlinear optics, we have considered g(co) to be intensity-dependent and
given by

Gt ( 1 4 - AIEI2 '~-1 (5)

/ •

E q u a t i o n (5) can be regarded as a model representation of Z(co) irrespective of its origin.

The symbols G 1, A, X and 7 have been defined in terms of the material parameters of
the crystals in table 1. It can be shown without m u c h difficulty that the usage of table 1
leads one to obtain the correct expression for X(co) for b o t h the models (iii) and (iv)
discussed in the preceding paragraph. This equation yields the various odd-ordered
optical susceptibility c o m p o n e n t s only if the excitation intensity ! ( = ½e0r/0 c l E t z) is

Table 1. Definition of terms used in equation (5).

Parameter Wberrett and Higgins (1982b)~ Sen (1984)b

GI e~'p~o 2 1 (^~ k2dk -'--7"Ng

2
mo~ hnz - o eon I~d0)lz
A 4TiT21lep,v/(m%h)l
2 g2ll~ 1(0)12/4h2
X toc~(k)- co (co1- f~,)- co
y 7"21 y,

°equations (12) and (19); bequations (17) and (18).

e~'Pcv is the transition dipole moment where e is the radiation
m(.D

polarization and pcvis the momentum matrix element, m is the electron

rest mass. I/al is the magnitude of the transition dipole moment and
I~,(0)1 corresponds to the ls Wannier-Mott exciton wave function. T1
and 7'2 are the population relaxation life time and dephasing time,
respectively, co,~(k)=%+hkZ/2m, with % being the band-gap fre-
quency and m, is the electron-hole pair reduced mass. oJ1 is the excitonic
effect incorporated band-gap frequency, y, is the renormalized damping
constant due to the self-energyof the excited pair state while ~, appears
due to the Stark broadening of the band edge.
664 P Sen and P K S e n

considerably small such that A IE] 2 <~(X 2 + 72) whence (5) reduces to

G1 G1AIEI 2 ( - 1)"GaA"IEI 2"

g(o~)=X+
i-y (X2+~,2) (X+iT) 4- . . . -+ (X2+72).(X+iT) (6)

with n = 0, 1, 2, 3. . . . For A tE[2~ ( X 2 + ~2), the present model breaks down. From (6),
it can be immediately recognized that the first term corresponds to Zt~)(~o) while the
second one yields Xt3~(o~)and so on. The response function R t2, + t~(t ) can be obtained
by taking the inverse Fourier transform of (6) as

Rt2"+l)(t)=(- 1)" GtA"lElZ"exp(-icnt)/[(X2+~2)"(X+iT)]do~ (7)

where we have taken

~(2n+ 1)/ • (-- 1)"Gx A"IE]2"

t¢°) =(~-~ + 72). (X + iy)"

Before proceeding further with Rt2n+ll(t), one has to check whether Z~2"+a)(oJ) is a
causal function or not. For t <0, R ~2"+~(t) must be evaluated in the upper half-plane
where exp(-itot) is bounded. It can be easily shown that Rtl~(t) has no singularity in
the upper half of the complex o~-plane and hence it vanishes. Rt3~(t) and other higher-
order response functions have poles in both the lower and upper half-planes. But at
t <0, E = 0 such that the integrands disappear. This leads one to conclude that the
generalized response function R ~2"+~(t) as well as 7t2"+t)(t) satisfy the principle of
causality.
We now attempt to establish the validity of the nonlinear K-K relations in obtaining
nonlinear refraction from the knowledge of nonlinear absorption and vice-versa in
terms of complex

~((2n + 1)(CO) ( = X~ln + 1) (t.O) + ix~2n+1) (t.O))"

From (6) and (7), one can find

g2.+ "(o~)1El 2"=(- (1)"a"l EI2"G~X

X 2 ..]- ~2) n + l (8a)
and
g2.+.(~)lEi2n=(- I)n+ I A"IEI2"Gx Y (8b)
(X2+~2) "+1

While applying K-K relations to the third-order nonlinear optical susceptibility under
certain approximations, Miller et al (1981) found the results to agree well with
experimental observations. Thus we first examine the correctness of equation (8) for
n = 1 in obtaining Z~3) from the knowledge of g[ a) and vice-versa. We obtain

_1 P.V. f5 xl3)(°Y)dc°'
co' = ( ~3 +1~ X2 2 /7( 3)L) (co) (9a)
7t --(2)
 Kramers-Kroni# relation in nonlinearoptics 665

and

--nl P.V. f+~ Z~a)(co')d°Y=X2(l

co'- co + (9b)

From equations (9), it may be noted that under near band-gap resonant transitions
with X2~V 2, approximate K-K dispersion relations can be established for the
nonlinear regime and may be regarded as the mathematical expression of the
approximation taken by Miller et al (1981). The applicability of K-K relations in
nonlinear optics is thus severely restricted within a very narrow frequency spectrum
(X 2 ~)~2). This has stimulated our interest in developing a generalized dispersion
relation which can be employed in the study of nonlinear optical effects over a broad
frequency spectrum.
We proceed along a line similar to that followed usually to derive K-K relations in
linear optics and arrive at the generalized K-K relations applicable to nonlinear optical
susceptibility of any arbitrary order. It is well known that K-K relations are obtainable
by using a Cauchy integral formula under the causal limit. Consequently, these
relations are restricted only to analytic response functions. Although Xt2" + x)(co) IE[2" is
causal it does not satisfy the Cauchy-Reimann conditions of analyticity. It is due to this
non-analyticity of Z ~2"+ 1)(09)]EI2" that exact K-K relations could not be obtained
resulting in (9). To avoid this shortcoming, we define a new function

X,(2n + 1)(0)) --~.( X 2 ._1_~2)n ~(2n + 1) ((D) (lO)

which is causal and satisfies the Cauchy-Reimann conditions for analyticity as well.
The application of Cauchy integral formula to this function finally leads to the
following relations:

and

(X'2 +Y2)" Xl2*+~)(co')=-lp'v'f~

(X2+y2)*Z('2~+',(co)dcon
_ (co-co') (11b)

where X' represents X with co being replaced by co'. For n=0, (11) yields

Z,")(CO')= I P.V.
f~_ Z~l)(co)dco
~ (co-co') (12a)

and

xl,)(co,)=_lp.v.f~ z;'(co)d~° (12b)

(co-co') •
Equations (12) are the well known K-K dispersion relations in linear optics. For n = 1,
we obtain the dispersion relations for the complex third-order susceptibility Z (3) and so
on for n = 2 , 3 . . . .
666 P Sen and P K S e n

3. Results and discussion

Equations (11) are applicable over an arbitrarily chosen frequency spectrum although
the pump power has to be restricted within a certain limit such that the condition
A IE 12 ,~ (X 2 + V2) is satisfied. The validity of (11) can be tested by applying these to the
well-known phenomena of nonlinear optical effects in solids as well as in plasmas. As an
example, we consider the phenomena of nonlinear refraction and absorption under low
power resonant excitation regime in direct-gap semiconductors like InSb, GaAs, GaSb
and InAs where the coherent radiation-exciton interaction model has been employed
(Sen 1984, 1986). One finds (Sen 1984, equation (22))

N/z'I~1(0)]" y,
~(~3) (09) = ~o~3 [((0 _ (.Dgr)2 _]_~)2 ] 2 . (13a)

Subsequently, one may use this equation in (1 l a) choosing 09- 098r= X and ~, = 7 to
obtain

N/~'l~kl(0)l 4 09-09,r
Z~3~(09)- eoh3 [(09_09,r)6 +y2] 2 . (13b)

Equation (13b) is exactly identical with that obtainable from (19) of Sen (1984).
The results obtained by using the expression for ~t3~(09) of the interband
transition saturation model (Wherrett and Higgins 1982b) also lead one to the same
conclusion and confirms the validity of(11) in the study of nonlinear dispersion in semi-
conducting crystals. The same equations can also be successfully employed in cor-
relating the nonlinear magneto-absorption and magneto-refraction studied earlier
(Sen 1983, 1986). Quite interestingly, the nonlinear plasma dispersion arising due to
the relativistic complex oscillatory electron fluid velocity depending upon various
powers of the pump intensity is another important area where (11) can be employed
satisfactorily.
It may be inferred that (11) are valid for all such kinds of nonlinear optical processes
for which the nonlinearity resembles with the form obtainable from (5) irrespective
of the nature of its origin. However, equation (11) is restricted to the study of non-
linear refraction and absorption in solids duly irradiated by moderately low power
lasers. The possibility of extending the present formulations to two-photon ab-
sorption and nonlinear wave-wave coupling will be the subject matter of a future
publication.

4. Conclusions

It may be noted that the model relations represented by (11) can be regarded as the
appropriate dispersion relations dealing with nonlinear optical properties of centro-
symmetric solids and plasmas. This may be of immense help in the study of nonlinear
refraction and absorption processes which are the origins of a class of non-
linear phenomena like optical bistability, optical phase conjugation, laser pulse
shaping, etc.
 Kramers-Kronig relation in nonlinear optics 667

Acknowledgments

The authors are indebted to Professor R K Singh and Dr S Guha for constant
encouragement. PS acknowledges financial support from CSIR, New Delhi.

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