15 January 2000

Optics Communications 174 Ž2000. 19–32

www.elsevier.comrlocateroptcom

Lichtenecker’s equation: applicability and limitations

A.V. Goncharenko ) , V.Z. Lozovski, E.F. Venger
Institute of Semiconductor Physics, National Academy of Sciences of Ukraine, 41 pr. Nauki, KieÕ 03650, Ukraine
Received 18 July 1999; received in revised form 15 October 1999; accepted 16 November 1999

Abstract

Lichtenecker’s equation for the effective dielectric function is considered with the help of spectral representation. The
spectral density function of resonances is determined and its behavior is analyzed. This analysis is carried out at different
values of a parameter specifying the composite topology. It is shown that Lichtenecker’s equation describes a specific
composite topology only. It is not reduced to the Bruggeman topology but may be represented as a spheroid system. q 2000
Published by Elsevier Science B.V. All rights reserved.

1. Introduction

Some progress achieved recently in physics of disordered media gives the possibility of looking at some
aspects of old phenomenological theories in a different way, to estimate their advantages and pitfalls,
application areas and limitations. One such old and well-known result is Lichtenecker’s equation for the
dielectric function of a two-phase composite, suggested in 1926 w1x. Lichtenecker’s idea was based on the
Wiener theory for bounds of effective dielectric function ´ Žor effective conductivity. of a composite w2,3x.
According to Wiener, for any two-phase composite one can write the lower
y1
f1 f2
´PW l s
ž ´1
q
´2 / Ž 1.

and upper
´PW u s f 1 ´ 1 q f 2 ´ 2 Ž 2.
bounds of its effective dielectric function. This means that the dielectric function, ´ , for a given physical system
must, in a sense, lie between these bounds. In Eqs. Ž1. and Ž2., f 1 and f 2 are the filling factors of the phases 1
and 2, respectively Žobviously, f 1 q f 2 s 1., and ´ 1 , ´ 2 are the dielectric functions of the corresponding phases.
The upper bound for this effective dielectric function is reached in a system consisting of plane-parallel layers
disposed along the field. The lower bound is reached in a similar system, but with the layers perpendicular to

)
Corresponding author. Tel.: q380-44-265-6020; fax: q380-44-265-5530; e-mail: avg@isp.kiev.ua

0030-4018r00r$ - see front matter q 2000 Published by Elsevier Science B.V. All rights reserved.
PII: S 0 0 3 0 - 4 0 1 8 Ž 9 9 . 0 0 6 9 5 - 1
20 A.V. Goncharenko et al.r Optics Communications 174 (2000) 19–32

the field. Similar results were obtained in Ref. w4x using the method of cross-sections. This method is based on
the fact that slicing a system by conducting surfaces does not decrease its conductivity Žpermittivity. and
dividing a system into a set of conducting tubes having insulating walls does not increase it. Starting from the
form of Eqs. Ž1. and Ž2., Lichtenecker assumed that the effective dielectric function of the considered composite
satisfies the equation
´ Lk s f 1 ´ 1k q f 2 ´ 2k Ž 3.
where the parameter k varies within the wy1,1x range. Thus, the extreme values of this k index correspond to
the Wiener boundary values. The parameter k may be considered as describing a transition from anisotropy at
k s y1 to anisotropy at k s 1 w5x. However, Lichtenecker’s equation may be also applied to isotropic
composites. In this case an assumption that their ´ is the same as one of diagonal components of a tensor of
some anisotropic composite effective dielectric function is used. Note also that Eq. Ž3. is consistent with other
approximations Že.g., the Looyenga w6x and Krawzenski w7x equations, k s 1r3 and k s 1r2, respectively..
These and other simple models for the effective dielectric function are also discussed in a review w8x Žand the
references cited therein..
It is obvious that each k value describes a specific microgeometry Žtopology. of a composite. One can
therefore expect that the area of applicability of Eq. Ž3. is wider than that of the well-known Maxwell Garnett
w9x and Bruggeman w10x equations that, in general, have no free parameters related to the topology Žfor the
Bruggeman’s theory the filling factor may be considered as a parameter describing the topology; in particular,
the filling factor specifies the percolation threshold.. Several examples of applications of Lichtenecker’s
equation can be found, particularly in Ref. w11x Žand references cited therein.. At the same time, it was not quite
clear for what systems this Eq. Ž3. is valid, and what is the range of its universality. In this work we will try to
answer these questions using, in particular, both graphic representation for ´ in the complex plane Re ´ –Im ´ ,
and Bergman’s analytical representation based on the resonance spectral density formalism.
It should be noted that Bergman’s representation contains the spectral density function which, as a rule, is
unknown. Lichtenecker’s equation contains the only parameter k that can be determined from experimental data
with relative ease. This fact is an additional reason of considering Lichtenecker’s equation in this work.
The paper is organized as follows. In Section 2 we review the simplest topologies of disordered media, as
well as the bounds and graphic representation for the domain of the effective dielectric function allowed values.
The description of the spectral ŽBergman. representation for the effective dielectric function is given in Section
3. Both these sections contain the known results but are necessary to understand the later sections. In Section 4
we consider Lichtenecker’s equation and find a spectral density functions corresponding to its particular cases.
Section 5 contains the results of numerical calculations and discussion. Finally, in Section 6 we give a brief
description of the main results obtained in this paper.

2. Topology and graphic representation

In this section we will analyze the topological aspects of the problem under consideration. First of all, it

l
should be noted that Eq. Ž3. is symmetrical Ži.e., dually invariant. relative to interchanging the phase indices
Ž1 2.. This means that topologies of phases 1 and 2 are similar. Such systems are called statistical w12x or
aggregate w13x. Another general kind of topology is said to be matrix w12x or cermet w13x one. These may be
represented in the form of particles of a dispersive phase 2 distributed over a continuous phase-matrix 1. The
most known and studied example of the matrix system is a dilute suspension of small spheres. In this case the
system effective dielectric function can be represented in the form of the Maxwell Garnett equation
´2 y ´1
´ MG s ´ 1 1 q df 2 Ž 4.
´ 2 Ž 1 y f 2 . q ´ 1Ž d y 1 q f 2 .
 A.V. Goncharenko et al.r Optics Communications 174 (2000) 19–32 21

where d denotes the space dimension. The inverted Maxwell Garnett equation for ´ MG ŽI. may be written if one
interchanges the roles of matrix and inclusions. From the considerations given below, it will be clear that
equations relative to the k-parameter, ´ L s ´ MG and ´ L s ´ MGŽI. , have no physical solutions, except the trivial
ones: k s 1, f 2 s 1, and k s y1, f 1 s 1.
The best known theory describing systems with an aggregate topology is Bruggeman’s symmetrical effective
medium approximation. Deducing Bruggeman’s equation

´ 1 y ´ Br ´ 2 y ´ Br
f1 q f2 s 0, Ž 5.
´ 1 q Ž d y 1 . ´ Br ´ 2 q Ž d y 1 . ´ Br

one implies that both phases have a form of spherical inclusions, and the effective medium itself plays a role of
matrix. Note, however, that the applicability area for Eq. Ž5. is wider than that for systems with such a specific
topology. Apparently, it might be more exact to say that the Bruggeman’s equation describes systems whose
light-scattering properties in a long-wavelength approximation are the same as those for an ensemble of spheres
Žconventional scatterers. of type 1 and type 2. Obviously, for these spheres to fill the space completely
Žcontinuously., it is necessary to assume that they are size-distributed in some manner. This distribution must
apparently also include the smallest spheres. We shall show later that a topology corresponding to Lichtenecker’s
equation cannot be Bruggeman’s topology. This means that Eq. Ž3. cannot be reduced to Eq. Ž5. for any k,
except the only trivial cases of f 1 s 0 and f 2 s 0.
Treating the problem of bounds for ´ , the most demonstrative and convenient way is the graphic
representation firstly suggested by Bergman w14x and, independently, Milton w15x. They called attention to the
fact that the domain of allowed values for ´ can be drawn in the complex plane Re ´ –Im ´ Žsee Fig. 1.. Then,
Eq. Ž1. corresponds to the circle passing through points ´ 1 , ´ 2 , and the origin of the coordinate system, and Eq.
Ž2. describes the straight line connecting the points ´ 1 and ´ 2 . As shown in Fig. 1, a section of this line and the
arc correspond to the upper and lower Wiener bounds, ´ Wu and ´ Wl , respectively. The domain disposed
between these segment and arc determines the set of all possible ´ values for a two-phase composite, regardless
of the phase volume fractions. Clearly, if f 1 s 0 Žthe system consists of phase 2 only. we have the point ´ 2 .
Conversely, if f 2 s 0, we obtain the point ´ 1. The points B Žon the circle. and A Žon the straight line.
correspond to some fixed non-zero value f 2 Žbearing in mind that f 1 s 1 y f 2 .. One can show Žsee, for instance,
Ref. w16x. that in this case the so-called Hashin—Shtrikman bounds w17x for effective ´ are the most general

Fig. 1. Graphic representation of the Wiener and Hashin–Shtrikman bounds.

22 A.V. Goncharenko et al.r Optics Communications 174 (2000) 19–32

ones. These are arcs belonging to the circles passing through three points Ž ´ 1 ,A,B. and Ž ´ 2 ,A,B.. In the
complex ´ plane these circles are given by parametric equations w14x
´2 y ´1
´ HS1 s ´ 2 1 y f 1 , Ž 6.
´ 2 y s0 Ž ´ 2 y ´ 1 .
and
1 Ž s0 y f 2 . Ž ´ 2 y ´ 1 . Ž 1 y s0 . Ž ´ 2 y ´ 1 .
´ HS 2 s ´ 2 1 y ½ s0 ´2
q f2
´ 2 y s0 Ž ´ 2 y ´ 1 . 5 . Ž 7.

It is easy to verify that Eqs. Ž6. and Ž7. are inverse in relation to changing ´ 1 ´ 2 and f 1 f 2 . If the
parameter s0 s 0, than Eq. Ž6. gives the point A, but when s0 s f 1 s 1 y f 2 , one has the point B. The point C
™ ™
corresponding to Eq. Ž4. can be obtained at s0 s f 1rd. Similarly, the inverse Maxwell Garnett equation Žthe
point D. can be obtained from Eq. Ž7. at s0 s f 2rd. Thus the change of the parameter s0 from 0 to f 2
corresponds to movement along the ACB arc. In a similar way, the change of the parameter s0 from 1 to f 1
corresponds to movement along the ADC arc. On the other hand, the point A corresponds to Eq. Ž3. at k s y1.
Thus, Eq. Ž3. may be considered as a parametric equation of some curve Žshown in Fig. 1 by the dotted line for
convenience.. This curve must lie between the ACB and ADB arcs Žin order for the ´ values as a solution of
Eq. Ž3. to fall into the region of ´ allowed values.. Apparently, one can state that this line is continuous when
changing the parameter k from 1 to y1 w18x.
It can be seen that Lichtenecker’s Eq. Ž3. is one of special cases realized for systems with an aggregate
topology. At the same time, one can expect that it describes a wide class of microgeometries, as a trajectory
corresponding to it in the complex plane passes through an infinite set of points and connects in passing two
boundary points ŽA and B. that, in a sense, correspond to opposite microgeometries.

3. Spectral representation

The generalized analytical Žspectral. representation suggested by Bergman allowed separation of the topology
and dielectric functions ´ 1,2 . The principal results concerning the spectral representation are given in Refs.
w16,19–22x. Here we shall summarize these results using notation and terminology of Ref. w22x.
It has been shown Žsee, e.g., Ref. w22x. that based on rather general assumptions Ždemands for system
macrohomogeneity and isotropy., one can write the effective dielectric function, ´ , of a two-phase composite as
° ´2 ´2 y1 y1
¶•
´ s ´ ~1 q f
1
1
¢ 2 C2 ž ´1
y1 q / H0qd xG Ž x .
2 ž ´1
y1 / qx
ß, Ž 8.

where G 2 Ž x . is the so-called spectral density function for medium 2 Žhere one uses a continuum Žintegral.
notation; Bergman used a discrete notation.. Similar equation can be also written via G 1Ž x ., the spectral density
function of medium 1 w22x.
These equations are to be completed by sum rules
1
C2Ž1. q H0qd xG 2Ž1. Ž x . s 1, Ž 9.

1 f 1Ž2.
H0q xG 2Ž1. Ž x.d xs
d
. Ž 10 .
In Eqs. Ž8. – Ž10., the variable of integration, x, is the generalized depolarization factor. Indeed, close
inspection of the integrand in Eq. Ž9. shows that it contains the polarizability of a spheroid whose depolarization
 A.V. Goncharenko et al.r Optics Communications 174 (2000) 19–32 23

factor is x Žsee, e.g., Ref. w23x.. The functions G 1Ž2. define some distributions of depolarization factors; these
are closely related to the spectrum of configuration Žgeometric. resonances for a separate component Žphase. of
the composite and depend on its microgeometry Žstructure.. Thus, a needle-shaped structure is in accordance
with low Žclose to zero. x values, while a disc-like structure is characterized by large Žclose to unit. x values.
The second term in the right side of Eq. Ž8. is the result of excluding a pole at the point x s 0 from the
integration domain. In other words, if the integration domain is expanded in such a manner as to include the
point x s 0, then the spectral density function should be taken in the form of G1Ž x . q C1 d Ž x . or G 2 Ž x . q

™™
C2 d Ž x ., where d Ž x . is the Dirac delta-function. The constants C1 and C2 have the special name of ‘percolation
strengths’ for phases 1 and 2, respectively w22x. To determine C2Ž1. , let ´ 2Ž1. `, while ´ 1Ž2. remains finite.
The integral in Eq. Ž8. can therefore be neglected, and if C2Ž1. ) 0, then ´ `. As a result, one obtains
1
C2Ž1. s
f 2Ž1.
lim
´ 2Ž1. ™ ` Ž ´r´ 2Ž1. .. Ž 11 .

In addition, the C2Ž1. coefficients satisfy the inequalities 0 F C2Ž1. F 1. Such a separation of the pole point x s 0
is convenient taking into account its special role. The issue is that this point corresponds to the so-called
percolation mode. Namely, for the case of percolation in the phase 1Ž2. we should set C1Ž2. ) 0.
As shown in Ref. w17x, the spectral density function G 2 Ž x . can be written as
1
G2 Ž x . s y
f2 p g ™0
lim Im  F Ž x q ig . 4 , Ž 12 .

where
F s 1 y ´r´ 1 . Ž 13 .
Note that if ImŽ ´r´ 1 . s 0, then one has to use the above-mentioned discrete notation, and one needs to change
the spectral density function by a set of discrete topological parameters w16x. For the widely known approaches
by Maxwell Garnett Ž4. and Bruggeman Ž5., the function G 2 Ž x . is well known and in the case of
three-dimensional Ž3D. composites it is, respectively,
1
G 2MG Ž x . s d x y Ž 1 y f2 . , Ž 14 .
3
and
1 2 1r2
G 2Br Ž x . s y9 x 2 q 6 x Ž 1 q f 2 . y Ž 3 f 2 y 1 . . Ž 15 .
4p
Ghosh and Fuchs w22x suggested a more general expression for the G 2 function. It is a generalization for Eq.
Ž15. and can be written as

° 3 (Ž x y x . Ž x y x l u
G Ž x . s~ 4 p
, xl -x-xu
2 x , Ž 16 .
¢0, x - x l or x ) x u
1
where x lŽ u . s
9
½ ( 5
4 q 3 y . 2 Ž 1 q 3 y . Ž 4 y 6 y . . Here the upper sign, Žy., corresponds to x l , and the lower
one, q , to x u , y s f 2 y f 2c , and f 2c stands for the critical filling factor Žthe percolation threshold. for the
Ž .
phase 2. According to the Bruggeman’s approximation Ž5., the percolation threshold f 2c s 1r3 w24x. It is easy to
check that in this case Eq. Ž16. transforms into Eq. Ž15..
24 A.V. Goncharenko et al.r Optics Communications 174 (2000) 19–32

4. Lichtenecker’s model

Although Lichtenecker’s model and Bergman’s representation are widely used when studying the composite
optical properties, we do not know of any works where the spectral density function for Lichtenecker’s model is
obtained or discussed. Let us obtain such a function and discuss its properties.
We assume that the effective dielectric function of a composite Žconsisting of two phases. can be determined
using Eq. Ž3. where an exponent, k, is specified by the system microgeometry. As it will be seen from following
speculations, the values of the parameter k s 0, "1 characterize some special types of microgeometries and
should be considered separately. Therefore, first of all we shall consider the most general case of k / 0, "1.

(a) k / 0, "1. Let us define real variables x and g using the relationship
y1
x q ig s Ž 1 y t . , Ž 17 .
where t s ´ 2r´ 1. Then for t k one can write
kr2
t k s A2 q g 2 B 2 cos k Ž w q p . q i sin k Ž w q p . , Ž 18 .
where
x 1 1
As 2
x qg 2
y 1, B s 2
x qg 2
g™0
, lim A s A 0 s
x
y 1, Ž 19 .

B
w s yarctg g ž / A ™0
, lim w s 0.
g
Ž 20 .

Let us introduce a parameter

P s 1 y f 2 1 y A k0 cos k p . Ž 21 .
As we shall see later, its sign specifies the correct choice of the Riemann surface sheet in the complex plane
Ž x,g .. Then, combining Eqs. Ž3., Ž13. and Ž17. one can obtain

° 1 y 1 y f2 Ž 1 y t k .
1rk

FŽ t. s ~ 1y ei p  f 2 Ž 1 y t k . y 14
1rk
, k)0 . Ž 22 .
¢1 y e yi p
 f 2 Ž 1 y t k . y 14
1rk
, k-0

It is taken into account in Eq. Ž22. that, when computing powers of a complex quantity, it is important to hold
the function on the fixed sheet of the Riemann surface. Under these conditions, the first row in Eq. Ž22.
corresponds to the case when P ) 0, and two lower rows describe the situation when P - 0. Using definitions
Ž19. and Ž20. and substituting Eq. Ž18. into Eq. Ž22., one has

°1 y w a q b x 2 1r2 k
f f

F Ž x q ig . s~
2
½ ž /
cos
k
q i sin ž /5
k
, P)0
. Ž 23 .
1r2 k f q sign k p
Ž . f q sign Ž k . p
¢1 y w a2 q b 2 x ½ ž
cos
k / ž q i sin
k /5 , P-0
 A.V. Goncharenko et al.r Optics Communications 174 (2000) 19–32 25

In these equations the next notations are used:

kr2
a s 1 y f 2 1 y Ž A2 q g 2 B 2 .
™0
cos k Ž w q p . , lim a s P ,
g

kr2
b s f 2 Ž A2 q g 2 B 2 .
™0
sin k Ž w q p . , lim b s f 2 A k0 sin k p ,
g

b q1, k)0
f s arctg ž /
a
, sign Ž k . s ½ y1, k-0
.

At last, in the limit g ™ 0 taken for FŽ x q ig . Žsee Eq. Ž23.. one can obtain from Eq. Ž12.
°sin f0

G2 Ž x . s Q Ž x . = ~ ž /
k
, P)0
, Ž 24 .
f 0 q sign Ž k . p
¢sin ž k / , P-0

where

f 2 A k0 sin k p 1 2 1r2 k
f 0 s arctg
ž P / , QŽ x . s
f2 p
Ž 1 y f 2 . q 2 f 2 A k0 Ž 1 y f 2 . cos k p q f 22 A20 k .

Eq. Ž24. is the final result of our calculations of the spectral density function in the most general case Ž k / 0,
"1.. As mentioned above, the special cases when k s 0 and k s "1 are to be considered individually.

(b) k s 0. This case was first considered in Ref. w25x. One can assume that the relevant topology is realized if a
system consists of two finely dispersed and well-mixed phases, so that one can prefer neither in parallel nor in
series connected layers. The resulting equation cannot be obtained by trivial substitution of k s 0 in Eq. Ž3..
Consider ´ as a function of two variables, ´ 1 and ´ 2 . Then the total differential of ´ may be written as

d ´ s ´ 1y k f 1 ´ 1ky1 d ´ 1 q f 2 ´ 2ky1 d ´ 2 . Ž 25 .
Setting k ™ 0, we obtain
d´ d´1 d´2
s f1 q f2 . Ž 26 .
´ ´1 ´2

Integrating this equation, one gets

ln ´ s f 1 ln ´ 1 q f 2 ln ´ 2 q const. Ž 27 .
Taking into account that ´ s ´ 2 if f 2 s 1, we find that const s 0 and the final result is
´ ´2
ln s f 2 ln . Ž 28 .
´1 ´1

Thus, it follows that

f2
´2
Fs1y ž /
´1
. Ž 29 .
26 A.V. Goncharenko et al.r Optics Communications 174 (2000) 19–32

Using Eqs. Ž18. – Ž20., one can write

f 2 r2
F Ž x q ig . s 1 y Ž A 2 q g 2 B 2 . exp  i f 2 Ž f q p . 4 . Ž 30 .
From this, it can be simply deduced that
1
G Ž0.
2 Ž x. s A 0f 2 sin Ž f 2 p . . Ž 31 .
f2 p

(c) k s 1. In this case ´ s Ž1 y f 2 . ´ 1 q f 2 ´ 2 , hence it follows that F s f 2 Ž1 y t . or, using Eqs. Ž18. and Ž12.
1 1r2
G Ž1.
2 Ž x. s
f2 p g™0
lim A2 q g 2 B 2 sin Ž p q f . . Ž 32 .

It can be seen that G Ž1.

2 is zero everywhere except the point where the quantity in square brackets becomes

™
infinite. The point of x s 0 is such one. Determining the G 2Ž1. Ž x . function values at this point, it is necessary to
pass to the limit in Eq. Ž32. using the condition x 0. For this purpose, we assume that the parameter x is very
small and in Eq. Ž32. keep the terms varying linearly with g .
1 1 g
G Ž1.
2 Ž x. s
f2 p g™0
lim ž x
y 1 sin / ž x Ž1yx . / . Ž 33 .

In the case of grx ™ 0, it follows from Eq. Ž33. that

Ž x ™ 0. s
1 g
f p ™
lim ž
x /
G Ž1.
2 s `. 2 Ž 34 .
™
2 g 0
x 0

Thus, for the function G 2 Ž x . one has

0, x/0
G Ž1.
2 Ž x. s ½ `, xs0
. Ž 35 .

There is the only function Žthe Dirac delta-function. that satisfies conditions Ž35.. Therefore, taking the
normalization condition Ž19. into account, we can state that

2 Ž x. sd Ž x. .
G Ž1. Ž 36 .
It is easy to check that substituting these results in Eq. Ž8. with C2 taken as zero yields Eq. Ž2..

(d) k s I1. In this case Lichtenecker’s equation gives ´y1 s Ž1 y f 2 . ´y1 y1

1 q f 2 ´ 2 , whence it follows that
F s f 2 Ž1 y t .rŽ f 2 q Ž1 y f 2 . t .. Using Eq. Ž17., we rewrite this expression in the form of
f2 x g g x
F Ž x q ig . s
C 2 2
x qg 2
Cq 2
x qg 2
Dyi ½ 2
x qg 2
Cq
x qg 2
2
D 5 , Ž 37 .

where
x 1
C s f2 y Ž 1 y f2 . ž 2
x qg 2 / g ™0
y 1 , lim C s f 2 y Ž 1 y f 2 . ž x
y1 , / Ž 38 .
g
D s Ž 1 y f2 .
x qg 2
2
g™0
, lim D s 0. Ž 39 .
 A.V. Goncharenko et al.r Optics Communications 174 (2000) 19–32 27

Fig. 2. The spectral density function of a two-phase composite with f 2 s 0.3 at different k ) 0 values: 1: k s 0.99; 2: k s 0.9; 3: k s 0.8; 4:
k s 0.7; 5: k s 0.6; 6: k s 0.5; 7: k s 0.4; 8: k s 0.3; 9: k s 0.2; 10: k s 0.1; 11: k s 0.01; and 12: k s 0.001. The behavior of G 2 Ž x .
function at small x Žcurves Žd. – Žf.. and big x Žcurves Ža. – Žc.. values is shown in the inserts: curves Ža. and d correspond to k s 10y3 ,
curves Žb. and Že. correspond to k s 10y4 , and curves Žc. and Žf. correspond to k s 10y5 .

Now using Eq. Ž12., one can obtain the expression for the spectral density function
1 1 g x
G Žy1.
2 Ž x. s
f2 p
lim
g ™ ½
0 C 2 2
x qg 2
Cq
x qg 2
2
D 5 . Ž 40 .

As can be seen from Eqs. Ž38. – Ž40., the function G Žy1.

2
Ž x . is zero everywhere except, perhaps, the point where
C s 0. Thus, to determine some possible non-zero value of the function G Žy1. 2
Ž x ., one should pass to the limit

Fig. 3. The spectral density function of a two-phase composite with f 2 s 0.3 at different k - 0 values: 13: k sy0.001; 14: k sy0.01; 15:
k sy0.1; 16: k sy0.2; 17: k sy0.3; 18: k sy0.4; 19: k sy0.5; 20: k sy0.6; and 21: k sy0.7.
28 A.V. Goncharenko et al.r Optics Communications 174 (2000) 19–32

Fig. 4. The spectral density function of a two-phase composite with f 2 s 0.3 at different k - 0 values: 22: k sy0.8; 23: k sy0.9; and 24:
k sy0.99. The 18a curve corresponds to k sy0.4 at x values close to 1.

™ ™
at g 0, x x 0 , where x 0 is the solution of the equation C s 0 under condition g s 0. It is easy to see that
x 0 s 1 y f 2 , and the passage to the limit in Eq. Ž40. yields G Žy1. Ž x . s `. Thus, we have
2

0, x / 1 y f2
G 2Žy1. Ž x . s ½ `, x s 1 y f2
. Ž 41 .

This means that

G Žy1.
2 Ž x . s d Ž x y 1 q f2 . . Ž 42 .
It is easy to check that substitution of this result in Eq. Ž8. with C2 taken as zero yields Eq. Ž1..
In Figs. 2–5 the results of numerical calculations for the spectral density function, G 2 , of a two-phase
composite for which the second phase filling factor f 2 s 0.3 are shown. As one can see from the figures, the
behavior of the curves in the limiting cases coincides with that determined by Eqs. Ž31., Ž36. and Ž42.. In the
final part of the paper, we shall discuss the behavior of the function G 2 for Lichtenecker’s model in detail. First
we shall make some general points that are important for understanding the further material.
There are two mechanisms determining the behavior of the resonance spectral density function. The first one
Žtopological. is the influence of a microgeometry or particle shape of the composite components. In the case of a
macroscopically homogeneous and isotropic system, its topology is effectively determined by phase percolation.

Fig. 5. The behavior of G 2 Ž x . function at k values close to 0 Žleft. and at k s 0 Žright.. Curves 1 and 2 correspond to k s 0.001 and
k sy0.001, respectively.
 A.V. Goncharenko et al.r Optics Communications 174 (2000) 19–32 29

In other words the fact of whether the system is below or above the percolation threshold plays an essential role.
It is commonly accepted that for spherical inclusions of phase 2 this threshold corresponds to the value
f 2 ( 0.18 Žsee, e.g., Ref. w26x.. However, in the general case which is the subject of our consideration, the
percolation may take place at any value of f 2 . Another mechanism determining the G 2 function behavior is the
polarization one. This means that the function G 2 is determined by some interaction between system
components or polarization currents. First of all, this mechanism is determined by the phase concentration
Žfilling factor.. With rising concentration, the dipole interaction increases and multipole interactions become
noticeable. This, in its turn, is reflected in the spectral density function behavior.

5. Results and discussion

Let us analyze the behavior of the spectral density function for a composite in the Lichtenecker’s model with
different values of k. For this purpose we shall consider first two extreme cases of k s 1 and k s y1, as well
as the intermediate case of k s 0, too. It is clear from the Section 1 that the cases of k s "1 can be realized in
systems Žcomposites. whose macroscopic symmetry is uniaxial Žsee also Ref. w16x. when light propagates along
their symmetry axes. In these cases ´ in Eqs. Ž1. and Ž2. is the transverse component of a tensor of the effective
dielectric function. In the case of k s 1 the composite is made of plane-parallel layers Ždiscs. which are also
parallel to the electric field w16x. Similar condition may take place, for instance, if one considers dielectric and
optical properties of superlattices under normal light incidence w27x. Obviously, a respective microgeometry for
the phase 2 can be imagined as the disc-like one with the discs disposed in parallel planes. In this case, one of
the disc depolarization factors takes the extreme value of L 3 s 1, and two other ones are L1 s L2 s 0 w28x. Here,
the resonance condition
y1
x s Re Ž 1 y ´ 2r´ 1 . s0 Ž 43 .
does not depend on the disc concentration. Eq. Ž43. corresponds to the depolarization factor L1. The semiaxis
ReŽ ´ 2r´ 1 . s 1, Im Ž ´ 2r´ 1 . G 0 corresponds to Eq. Ž43. at the complex plane introduced in the Section 2. In
the case k s y1 the composite is made of parallel needles which are perpendicular to the electric field. This
extreme case of topology is realized, in particular, for systems similar to porous silicon w29x and for zeolites.
The respective microgeometry for the phase 2 is cylindrical or needle-like one. In this case, one of the

A needle corresponds to an elongated spheroid in such an extreme case when its eccentricity l 1. The
spheroid has two resonance modes. If the wave vector is directed along the spheroid axis, only one of two
™
depolarization factors for needles takes the extreme value of L3 s 1, and the other two factors are L1 s L2 s 0.

modes is excited. It is obvious that this mode corresponds to the non-zero value of the d-function at the point
x s 1 y f 2 . Thus, this point can be determined from the equation
y1
x s Re Ž 1 y ´ 2r´ 1 . s 1 y f2 . Ž 44 .
™
Here, in the case of f 2 0, the depolarization factor corresponding to the system resonance coincides with the
depolarization factor of some averaged disc. Clearly, as the resonance position depends on the filling factor f 2 ,
in Eq. Ž44. at k s y1 one must take into account the interaction between discs. It is also necessary to bear in
mind that position of this resonance cannot correspond to the Maxwell Garnett resonance at x s Ž1 y f 2 .r3 s
f 1r3 Žsee Eq. Ž14.. at any f 2 value Žexcept the trivial case of f 2 s 1.. At the complex plane ŽRe ´ , Im ´ . Eq.
Ž44. describes a semicircle with a center at the point ReŽ ´ 2r´ 1 . s 1 y 1r2 f 1 and with a radius of 1r2 f 1.
To determine the topology corresponding to the case of k s 0, let us rewrite Eq. Ž28. in the form
´1 ´2
f 1 ln ž´/ q f 2 ln ž´/ s 0. Ž 45 .
30 A.V. Goncharenko et al.r Optics Communications 174 (2000) 19–32

It is apparent that in Eq. Ž45. the values a 1 s lnŽ ´ 1r´ . and a 2 s lnŽ ´ 2r´ . can be considered as dimensionless
effective polarizabilities Žeffective polarizabilities per unit volume. corresponding to the phases 1 and 2 Žsee,
e.g., Ref. w30x.. We shall show now that the case of k s 0 is in accordance with the topology of the composite
consisting of randomly oriented spheroids from substance types 1 and 2 which have a uniform shape-distribu-
tion. Let the composite consist of such randomly oriented spheroids distributed in shape with unit weight. Then
the dimensionless polarizability of such a spheroid of phase ‘i’ with depolarization factor L along its axis
w23,28x can be written as
´ i y ´m
a˜ Ž i. s , Ž 46 .
´m q L Ž ´ i y ´m .
where ´m is the dielectric permeability of the matrix. Let us assume, for further consideration, that an effective
media itself is the matrix. Then, the dimensionless effective polarizability of the i-phase can be determined by
averaging the expression Ž46. over spheroid shapes Žremember that the shape-distribution of the spheroids is
uniform.:
1 ´i
aŽ i. s a˜ Ž i. Ž L . d L s ln
H 0 ´ ž /
. Ž 47 .
As can easily be seen, Eq. Ž45. follows from Eq. Ž47.. This confirms our assumption relating the system
topology in the case of k s 0. Note that for more rigorous treatment, it is necessary to take into account a
possibility of spheroid volume changing with its shape. Bearing in mind that space can be filled completely by
spheroids of different volumes and shapes, we average Eqs. Ž45. and Ž47. over the spheroid shapes. At the same
time, we shall consider that spheroids of type 1 are distributed in shape with the distribution function, g 1Ž V .,
and have a maximum volume V1 , while spheroids of type 2 are distributed in shape with g 2 Ž V .-function and
their maximum volume is V2 . In order to determine the composite effective dielectric function, Eq. Ž45. is
transformed to
V1 ´1 V2 ´2
f1
H 0
dVg 1 Ž V . V ln
´ ž /
q f2
0
dVg 2 Ž V . Vf 2 ln
H ´ ž /
s 0. Ž 48 .
It is obvious that Eqs. Ž45. and Ž48. are equivalent if the condition
V1 V2
H0 dVg 1 Ž V . V s H0 dVg 2 Ž V . V s Vˆ Ž 49 .
applies. It is valid if the spheroid volumes of different phases are on average equivalent Žand equal to Vˆ .. Zero
lower limiting value of volume means that for continuous filling of space by spheroids of different shapes it is
necessary to take into account spheroids with an arbitrary small volume. The condition Ž49. is obviously valid
when the spheroids are similarly distributed in shape and V1 s V2 . ŽNote that using a long wavelength approach,
a final result must not depend both on particle size distribution, and V1 , V2 values.. Thus, one can state that in
the case of k s 0 Lichtenecker’s model describes a system of randomly oriented spheroids that are uniformly
distributed in shape, and have a similar distribution in the volume.
We now consider the evolution of G 2 Ž x .-curve when changing k from 1 to y1, i.e., the replacement of one
d-function, d Ž x ., by another, d Ž1 y f 2 ., in the spectral density function. Let us look at Figs. 2–5. The curves

™ ™
given there correspond to the fixed value of the filling factor, f 2 s 0.3, but the behavior of G 2 Ž x .-function will
be qualitatively the same for other f 2 values. One can see that if 0 - k - 1, then G 2 Ž x . ` when x q0. At

™
the same time, a new peak of the function G 2 Ž x . appears with decreasing k. Its position tends to the point x s 0
when k 0 from the right. At the point x s 0 the function G 2 Ž x . has a discontinuity since G 2 Ž x . s C2 / `.
To find C2 , let us take ´ s ´ L and substitute Eq. Ž3. in Eq. Ž11.. The result is
1
y1
C2 Ž k ) 0 . s f2k . Ž 50 .
 A.V. Goncharenko et al.r Optics Communications 174 (2000) 19–32 31

™ ™
It is easily seen that in this case C2 is positive. Thus, for k ) 0, C2 ) 0. This corresponds to percolation of both
phases in the system, independently of the filling factor. When k s 0, only one peak is present Ž G 2 Ž x . ` if
x q0.. With increasing x the function G 2 Ž x . slowly approaches zero Žat x s 1.. To find C2 for this case, let

™ ™
us use Eqs. Ž11. and Ž28.. The result is C2 Ž k s 0. s 0. By this it is meant that none of the phases percolates. At
k y0 the function G 2 Ž x . has its maximum value at x s 1. Here, when k y1 from the right, the position
of that maximum shifts to the point x s 1 y f 2 , and its amplitude behaves nonmonotonically Žfirst decreases,
then increases.. Using Eqs. Ž3. and Ž11. one can show that C2 Ž k - 0. s 0. Thus, there is no percolation in the
system if k - 0.
An interpretation of the function G 2 Ž x . behavior and its relation to composite topology is a highly intricate
problem. Obviously, in this situation a representation based on the distribution of ellipsoidal Žspheroidal. shapes
Žas an alternative to the Bergman’s one. is more convenient. If elementary scatterers of types 1 and 2 with a
spheroidal shape and some shape-distribution function, DŽ L., are considered, then Eq. Ž47. will take the form
1 1 ´i y ´
aŽ i. s a˜ Ž i. Ž L . D Ž L . d L s
H H D Ž L . d L. Ž 51 .
0 0 ´ q LŽ ´i y ´ .

The function DŽ L. s d Ž L. at k s 1, DŽ L. s 1 at k s 0, and DŽ L. s d Ž L y 1. at k s y1. In the general case,

DŽ L.-dependence is expressed through G-function, as was found in Ref. w11x.
It should be noted that our approach is limited by considering the well-known Lichtennecker’s equation
which does not take into account the effects of nonlocality. At the same time, the nonlocal effects can play an
essential role in the optical properties of the particle systems Žsee, e.g., Ref. w31x.. We assume, however, that an
approach similar to the effective medium method could be formulated for systems where the nonlocal effects are
taken into account. For example, we have generalized the local field method for the systems consisting of both
finite w32x and infinite w33x ensembles of small particles. The next step, we hope, could be averaging the field
over the particle ensemble and the calculation of the effective local field factor. Since the local field factor is
connected to the dielectric function of a system, there is a possibility of obtaining the effective dielectric
function of a composite system via dielectric functions of its components. We presume that this consideration
will be discussed elsewhere.

6. Summary

In this paper, Lichtenecker’s equation for the effective dielectric function of a two-phase composite has been
analyzed starting from a spectral representation. Analytical expressions for the spectral density function that are
suitable for all of the allowed values of the k-parameter determining the system topological properties have been
obtained. The main conclusion that follows from the analysis carried out is that Lichtenecker’s equation
characterizes a specific microgeometry of a system which can be reduced neither to the Maxwell Garnett
microgeometry nor to that of Bruggeman. It has been found that the special cases Ž k s 0, "1. of the system
microgeometry can be represented by some distribution of spheroidal particles. This conclusion can obviously
be extended to the case of arbitrary k. At the same time, starting from the graphic representation for ´-bounds in
the complex plane, one can state that a two-parameter representation is necessary to describe the range of all
possible effective dielectric function values.

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