Electromagnetic scattering

by an aggregate of spheres

Yu-lin Xu

We present a comprehensive solution to the classical problem of electromagnetic scattering by aggregates

of an arbitrary number of arbitrarily configured spheres that are isotropic and homogeneous but may be
of different size and composition. The profile of incident electromagnetic waves is arbitrary. The
analysis is based on the framework of the Mie theory for a single sphere and the existing addition
theorems for spherical vector wave functions. The classic Mie theory is generalized. Applying the
extended Mie theory to all the spherical constituents in an aggregate simultaneously leads to a set of
coupled linear equations in the unknown interactive coefficients. We propose an asymptotic iteration
technique to solve for these coefficients. The total scattered field of the entire ensemble is constructed
with the interactive scattering coefficients by the use of the translational addition theorem a second
time. Rigorous analytical expressions are derived for the cross sections in a general case and for all the
elements of the amplitude-scattering matrix in a special case of a plane-incident wave propagating along
the z axis. As an illustration, we present some of our preliminary numerical results and compare them
with previously published laboratory scattering measurements.
Key words: Scattering, particles, aggregates.

1. Introduction Kerker.6 This is an example of a particle with a

Light scattering by a small body or a collection of
small objects whose sizes are comparable to the
wavelength of the incident radiation is a problem of
great interest to a broad range of scientific disciplines.
To date, exactly solvable problems include the scatter-
ing of a plane electromagnetic wave by a few highly
symmetric types of single particles and by arbitrary
configurations of parallel, infinite cylinders. Per-
haps the scattering theory that is most widely used is
that for a homogeneous sphere of arbitrary size and
refractive index, known as Mie theory, which was
developed by Lorenz1 and Mie.2 The complete solu-
tion for homogeneous, infinitely long, circular cylin-
ders was first given by Lord Rayleigh3 for the case of
perpendicular incidence and by Wait4 for the case of
oblique incidence. The problem of homogeneous
spheroids was solved by Asano and Yamamoto.5 A
solution for the problem of scattering by a homoge-
neous sphere coated with a homogeneous layer of
uniform thickness was first obtained by Aden and-
The author is with the Department of Astronomy, P.O. Box
112055, University of Florida, Gainsveille, Florida 32611-2055.
Received 3 October 1994; revised manuscript received 8 February
1995.
0003-6935@95@214573-16$06.00@0.
r 1995 Optical Society of America.
spatially variable refractive index; their theory can
also be generalized to a radially stratified sphere.
The mutual interaction complicates light scatter-
ing by ensembles of particles. The problem there-
fore requires the use of an addition theorem to
transform the relevant basis functions from a coordi-
nate system centered on the scatterer to other refer-
ence systems centered outside the scatterer. Using
an addition theorem for cylindrical waves, Twersky7–9
was able to calculate the scattered field produced by a
plane wave striking an arbitrary configuration of
parallel infinite cylinders.
For multiple scattering by spheres, it is necessary
to decompose the scattered field of a sphere into
spherical waves that impinge on the other spheres.
Although Mie theory expresses the scattered field in
the form of spherical vector wave functions by using
the center of the sphere as the origin of the reference
system, the problem of interacting spheres requires
that one seek representations of the scattered field by
the use of the same set of basis spherical vector wave
functions that refer to any other arbitrary origin.
In 1954, Friedman and Russek10 reported a deriva-
tion of such an expansion, or addition theorems for
spherical scalar-wave function. With the develop-
ment of addition theorems for spherical vector wave
functions in the 1960’s by Stein11and Cruzen,12 it
became, in principle, feasible to solve theoretically for

20 July 1995 @ Vol. 34, No. 21 @ APPLIED OPTICS 4573

the scattering properties of arbitrary aggregates of
spheres. Since then, considerable progress has been
made toward a solution for multisphere systems,
especially by Liang and Lo,13 Bruning and Lo,14,15
Fuller and Kattawar,16,17 and Mackowski.18 The
reader is referred to an article by Fuller19 for a
historical review. A general literature survey is be-
yond the scope of this paper; we cite only the most
closely related papers.
In 1971, Bruning and Lo published the first compre-
hensive solution for a two-sphere chain,14,15 complete
with experimental verification. These authors ap-
plied the standard electromagnetic boundary condi-
tions to the surfaces of the two spheres with addition
theorems and were able to solve the resulting linear
equations for the interactive scattering coefficients by
the use of direct matrix inversion. Later, Fuller and
Kattawar introduced the order-of-scattering meth-
od16,17 as an alternative and more effective way of
solving for the coefficients in an attempt to reduce a
2L-sphere scattering problem to a sequence of interact-
ing pairs. Their strategy was to extend Bruning and
Lo’s solution pairwise to the more complicated case of
an arbitrary cluster of spheres. In 1991, Mack-
owski18 rederived the addition theorems for vector
spherical harmonics and obtained a set of recurrence
relations for effective calculation of the addition coef-
ficients. This scattering problem of interacting
spheres is also independently investigated by Bor-
ghese et al.,20–22 who handled the vector scattering
problem through Debye potentials and by Wang and
Chew,23 who developed a recursive T-matrix approach
for the solution. Borghese et al.20,21 appear to have
been the first to present explicit expressions for the
cross sections of the sphere clusters. Other research
conducted on the scattering cross sections includes
that of Gérardy and Ausloos24 and of Mackowski.18
Gérardy and Ausloos provided a correct expression for
extinction cross sections of the aggregates through an
integral of the Poynting flux of the scattered field.
In addition to the scattering and extinction cross
sections, Mackowski also derived an expression for
the absorption cross sections of the multisphere sys-
tems by integrating the Poynting flux at the surface of
each sphere in the cluster. A brief discussion of the
Müller matrix of a two-sphere system can be found in
a paper by Fuller et al.25
However, the solution of the problem of interacting
spheres appears to be still incomplete; missing is a
derivation of explicit expressions of the amplitude-
scattering matrix and therefore the Müller matrix
and the polarization properties. The calculation of
the angular distribution of the scattered field and the
state of polarization is important or even essential in
many applications.
In this paper the intent is to present a complete
general solution to the problem of interactive electro-
magnetic scattering by clusters of arbitrarily config-
ured nonidentical spheres. The profile of incident
beams is arbitrary. The only assumption made on
the incident electromagnetic field is that the incident
4574 APPLIED OPTICS @ Vol. 34, No. 21 @ 20 July 1995
waves can be expressed by elementary spherical
waves. The framework of the multisphere scatter-
ing theory follows closely from the Mie theory. In
Section 3, based on a superposition principle in terms
of vector spherical harmonic expansions, we extend
the classic Mie theory to a general case of an arbitrary
profile of incident beams. In Section 4 the extended
Mie theory is applied to all the constituents of the
cluster of spheres and results in a linear system in
which one is to solve for the interactive scattering
coefficients. In Section 5 an asymptotic iteration
method is suggested to solve the resultant linear
equations for the interactive scattering coefficients,
which uses a numerical factor to improve the conver-
gence property of the linear system. Section 6 briefly
discusses the construction of the total scattered field
of the entire cluster and provides expressions for the
internal fields of each sphere in the primary reference
system. Section 7 is devoted to the discussions of
cross sections and the elements of the amplitude-
scattering matrix. Some comparison of our prelimi-
nary numerical results with laboratory microwave
measurements is given in Section 8.
2. Statement of the Problem
Consider a cluster of L isotropic, homogeneous, and
nonintersecting spheres with known radii a j and
known complex refractive indices N j, j 5 1, . . . , L.
Throughout this paper, any single integer in a right-
hand superscript, such as j in a j, indicates that the
quantity is related to the jth sphere. These spheres
are confined to a finite volume. In a three-dimen-
sional coordinate system whose origin is at the center
of the j0th sphere 1below we refer to this coordinate
system as the primary system2, the position vector of
the center of any other jth sphere is denoted by dj0, j,
which extends from the center of the j0th to the center
of the jth sphere. For any pair of spheres in the
cluster, the jth and the lth, the relative position
vector is defined by dj,l 5 dj0,l 2 dj0, j, and dj,l $ a j 1 al.
Suppose that the incident beams illuminating each
sphere in the cluster can be represented by elemen-
tary spherical waves about the center of each sphere.
The incident electromagnetic waves are monochro-
matic but arbitrary in profile. The scattering proper-
ties of such a cluster of spheres are to be examined
analytically.
3. Generalization of the Mie Theory
To investigate the scattering properties of the cluster
of interacting spheres, we need to determine the
interactive scattering coefficients for each sphere
individually, similar to what Mie theory does for a
single sphere. However, in this case the spherical
constituents in the cluster can no longer be consid-
ered as isolated, and the assumption of a plane
incident wave is no longer valid. We need to handle
a more general case than the classic Mie theory. The
problem of generalizing the Mie theory was consid-
ered by Gouesbet et al.26,27 as well as by Barton et al.28
These authors studied the scattering properties of a
sphere located in a Gaussian laser beam, using a 2. Expansion of the Scattered, Internal, and
Bromwich scalar formulation. Our study of the mul- Incident Fields
tisphere case leads to the same result, though in a In terms of the spherical vector wave functions, the
totally different manner. The basic derivation is as scattered field 1Es, Hs2 and the internal field 1EI, HI2 of
follows: an individual sphere, say, the jth sphere in the
A. Expansion of Electromagnetic Fields cluster, can be expanded as
To solve scattering problems, it is desirable to express ` n
electromagnetic fields in terms of infinite-series expan-
sions at all points in space. In our case the fields are
Es1 j2 5 o o
n51 m52n
iEmn3a jmnN132 j 132
mn 1 bmnMmn4,

to be expanded in terms of elementary spherical ` n

waves about a fixed center. k
1. Spherical Vector Wave Functions
Hs1 j2 5
vµ o o
n51 m52n
Emn3b jmnN132 j 132
mn 1 amnMmn4,

Time-harmonic electric and magnetic fields E and H ` n

in a sourceless, isotropic, and homogeneous medium

are divergence free and must satisfy the vector wave
EI1 j2 5 2 o o
n51 m52n
iEmn3d jmnN112 j 112
mn 1 cmnMmn4,

equations ` n
kj
2
= 3 = 3 E 2 k E 5 0, = 3 = 3 H 2 k H 5 0, 2
112 HI1 j2 5 2 o o
vµ j n51 m52n
Emn3c jmnN112 j 112
mn 1 dmnMmn4, 142

where k 2 5 v2Eµ, k is the wave number, v is the

where
circular frequency of the wave, E is the dielectric
constant, and µ is the permeability of the medium. 1n 2 m2!
In spherical polar coordinates 1r, u, f2, the linear Emn 5 0 E0 0 in12n 1 12 . 152
independent vector field solutions of the vector wave 1n 1 m2!
equations are the vector spherical functions M and N The introduction of Emn is desired for keeping the
that, in the specific component form, may be written formulation of the multisphere-scattering theory con-
as sistent with that of the Mie theory. It ensures that
M1J2 1J2
mn 5 3iuipmn1cos u2 2 iftmn1cos u24zn 1kr2exp1imf2,
all the expressions in the multisphere theory turn out
to be identical to those in the Mie theory when one is
z1J2
n 1kr2 dealing with a cluster containing only one sphere and
N1J2 m
mn 5 irn1n 1 12P n 1cos u2 exp1imf2
kr illuminated by a single plane wave. When m 5 1,
1 3iutmn1cos u2 1 ifipmn1cos u24 2n 1 1
E1n 5 En 5 0 E0 0 in . 162
1 d n1n 1 1)
3 3rz1J2
n 1kr24exp1imf2, 122
kr dr
This is what appears in the Mie theory 1see Bohren
where ir, iu, if are unit vectors in the spherical and Huffman,29 chapter 42. The superscript 132 or 112
polar-coordinate system; z1J2 appended to the vector spherical harmonics indicates
n is appropriately selected
from any of the four spherical Bessel functions: the that the generating function is specified by the Han-
first kind jn, the second kind yn, or the third kind 1also kel function of the first kind, h112 n , or the Bessel
called spherical Hankel functions of the first and function of the first kind, jn, respectively. Also, k j is
second kind2 h112 122
n and hn , denoted by J 5 1, 2, 3, or 4,
the wave number inside the jth sphere, and µ j is the
m
respectively; Pn 1cos u2 is the associated Legendre permeability of the same sphere. Throughout this
function of the first kind and of degree n and order m, paper a single integer in parentheses has the same
n, and m are integers with 1 # n , ` and 2n # m # n, meaning as in a right-hand superscript. In Eqs. 142,
and with definitions for the functions we associate the internal coefficient d with the scatter-
ing coefficient a and the internal coefficient c with the
m scattering coefficient b. Again, this agrees with
pmn1cos u2 5 Pm
n 1cos u2,
sin u Bohren and Huffman. The readers should, however,
be aware of a different notation; for example, both van
d de Hulst31 and Kerker32 associate c with a and d with
tmn1cos u2 5 Pm
n 1cos u2. 132
du b.
Similarly, the incident field that strikes the surface
Recursion formulas for pmn and tmn are given in of the jth sphere is assumed to have the form
Appendix A. Here both the vector spherical harmon-
ics 1Mmn, Nmn2 and the angular functions 1tmn, pmn2 are ` n

denoted by the order m first and the degree n last.

This notation agrees with that used by Bohren and
Ei1 j2 5 2 o o
n51 m52n
iEmn3p jmnN112 j 112
mn 1 q mnMmn4,

Huffman,29 but the one that is commonly used in the k ` n

arbitrary-incident-beam literature28,30 has the order
of m and n reversed.
Hi1 j2 5 2
vµ o o
n51 m52n
Emn3q jmnN112 j 112
mn 1 p mnMmn4, 172

20 July 1995 @ Vol. 34, No. 21 @ APPLIED OPTICS 4575

where the incident waves from all the possible sources
are included. Here the harmonic time dependence
exp12iwt2 of the fields is assumed and suppressed.
B. Extension of the Mie Theory to a General Application
Still using the jth sphere as an example, we impose
the standard boundary conditions at the surface of
the sphere:
Ei1 j2 1 Es1 j2 2 EI1 j24 3 i rj
5 3Hi1 j2 1 Hs1 j2 2 HI1 j24 3 ir j 5 0. 182
In a component form, these boundary conditions at
In Eqs. 1102 the prime indicates a differentiation with
respect to the argument in parentheses. x j and m j
are the size parameter and the relative refractive
index of the jth sphere, respectively, and are given by
2pN 0a j kj Nj
x j 5 ka j 5 , mj 5 5 , 1112
l k N0
where l is the wavelength of the incident waves in the
surrounding medium and N 0 is the refractive index of
the surrounding medium. The four simultaneous
linear equations 1102 can be solved for the four intera-
tive coefficients: a jmn, b jmn, c jmn, d jmn. The interac-
tive scattering coefficients are given by

µ1m j22jn1m jx j23x jjn1x j248 2 µ jjn1x j23m jx jjn1m jx j248

a jmn 5 p jmn,
µ1m j22jn1m jx j23x jh112 j j 112 j j j j j
n 1x 248 2 µ hn 1x 23m x jn1m x 248

µ jjn1m jx j23x jjn1x j248 2 µ jn1x j23m jx jjn1m jx j248

b jmn 5 q jmn, 1122
µ jjn1m jx j23x jh112 j 112 j j j j j
n 1x 248 2 µhn 1x 23m x jn1m x 248

Similarly, the coefficients of the internal field are

given by

µ jjn1x j23x jh112 j j 112 j j j

n 1x 248 2 µ hn 1x 23x jn1x 248
c jmn 5 q jmn,
µ jjn1m jx j23x jh112 j 112 j j j j j
n 1x 248 2 µhn 1x 23m x jn1m x 248

µ jm jjn1x j23x jh112 j j j 112 j j j

n 1x 248 2 µ m hn 1x 23x jn1x 248
d jmn 5 p jmn. 1132
µ1m j22jn1m jx j23x jh112 j j 112 j j j j j
n 1x 248 2 µ hn 1x 23m x jn1m x 248

Equations 1122 and 1132 can be written as

r j 5 a j are a jmn 5 a jn p jmn, b jmn 5 b jnq jmn, 1142
Eiu1 j2 1 Esu1 j2 5 EIu1 j2, Eif1 j2 1 Esf1 j2 5 EIf1 j2, c jmn 5 c jn q jmn, d jmn 5 d jn p jmn, 1152

Hiu1 j2 1 Hsu1 j2 5 HIu1 j2, Hif1 j2 1 Hsf1 j2 5 HIf1 j2.
192
From the orthogonality of exp1imf2, together with the
expansions 142 and 172 and the expressions for the
spherical vector harmonics 122, the above boundary
conditions give rise to four linear equations contain-
ing the interactive coefficients:
jn1m jx j2c jmn 1 h112 j j j j
n 1x 2b mn 5 q mn jn1x 2,
µ3m jx jjn1m jx j248c jmn 1 µ j3x jh112 j j
n 1x 248b mn
5 q jmnµ j3x jjn1x j248,
µm jjn1m jx j2d jmn1 µ jh112 j j j j j
n 1x 2a mn 5 p mnµ jn1x 2,
3m jx jjn1m jx j248d jmn 1 m j3x jh112 j j
n 1x 248a mn
5 p jmnm j3x jjn1x j248.
1102
where a jn, b jn, c jn, d jn,
are exactly the Mie coefficients
for the isolated jth sphere 3see Borhen and Huff-
man,29 equations 14.522 and 14.5324.
This result is the same as that obtained by Goues-
bet et al. and by Barton et al. It clearly reveals that
the radiative scattering response of a homogeneous
sphere to an arbitrary beam can be directly related to
the Mie scattering properties of that sphere and the
profile of the electromagnetic waves that are incident
upon it. No matter how complicated the incident
field, the scattering coefficients 1and therefore the
scattering properties2 of a sphere, whether isolated or
not isolated, can be easily determined with Eqs. 1142 if
the expansion coefficients of the incident field can be
explicitly found. The scattering coefficients in a gen-
eral case are just the linear modifications of Mie
coefficients by the expansion coefficients of the inci-
dent field. Thus, to investigate the scattering behav-
ior of a sphere in a general case, the only new task
involved is to determine the expansion coefficients
that describe the incident field.

4576 APPLIED OPTICS @ Vol. 34, No. 21 @ 20 July 1995

4. Description of the Total Incident Field for a Spherical
Constituent
From the discussions in Section 3, one can see that for
the multisphere problem at hand, we need to seek an
explicit description of the total incident field for each
sphere in the cluster. To determine the interactive
coefficients 1a jmn, b jmn, c jmn, d jmn2 of the jth sphere, we
need to determine the expansion coefficients
1 p jmn, q jmn2 of the incident field of the same sphere.
The electromagnetic field that is incident upon the
surface of the jth sphere consists of two parts: 112 the
original incident waves and 122 the scattered fields of
all the other spheres in the cluster, which can be
written as

Ei1 j2 5 E01 j2 1 o E 1l,

lfi j
s j2,

Hi1 j2 5 H01 j2 1 o H 1l,

lfi j
s j2. 1162

Fig. 1. Geometry of the multisphere scattering problem.

Throughout this paper, two integers separated by a
comma in parentheses or in a right-hand superscript
l, j imply a translation from the lth to the jth
coordinate system. To obtain analytical expressions
for the total incident field striking the surface of each and the projection of k on the x–y plane. In Eq. 1192
sphere, the initial incident waves, and all the scat- ix, iy, and iz are the unit vectors of the Cartesian
tered fields of the other spheres must be expanded coordinate system. Usually, two different polariza-
about the center of the sphere. The last of these can tion modes of the incident plane wave are considered:
be accomplished by the use of the translational addi- the transverse magnetic mode 1TM2, which corre-
sponds to the case in which the electric vector vibrates
tion theorem for vector spherical harmonics.
in the incident plane, and the transverse electric
mode 1TE2, which corresponds to the case in which the
A. Expansion of the Initial Incident Waves magnetic vector vibrates in the incident plane. The
incident plane is defined by the z axis and the incident
The original incident waves are assumed to be expand-
wave vector k. For the TM mode, the expansion
able about the center of each sphere and, for the jth
coefficients are
sphere, i.e., in the jth coordinate system, the incident
field has the form
p j,mnj 5 exp1ik · dj0, j2p0mn, q j,mnj 5 exp1ik · dj0, j2q0mn,
` n
1202
E01 j2 5 2 o o
n51 m52n
iEmn3 p j,mnj N112 j, j 112
mn 1 q mnMmn4,
where
` n
k
H01 j2 5 2 o o
vµ n51 m52n
Emn3q j,mnj N112 j, j 112
mn 1 p mnMmn4. 1172
p0mn 5
1
3tmn1cos a2cos b 2 ipmn1cos a2sin b4,
n1n 1 12
For use below, we introduce 1
q0mn 5 3tmn1cos a2cos b 2 ipmn1cos a2sin b4.
p0mn 5 p jmn
0, j0
, q0mn 5 q jmn
0, j0
, 1182 n1n 1 12
1212
where superscript 0 indicates that the quantity is
related to the initial incident waves and the primary B. Addition Theorems for Spherical Vector Wave Functions
system. All these expansion coefficients of the initial
incident waves that drive the whole scattering pro- To transform the waves scattered by an individual
cess are supposed to be known for the problem under sphere into the incident waves of other spheres in the
consideration. An example is as follows. cluster, we need to describe the same scattered field in
Suppose as shown in Fig. 1, that the cluster is alternative forms, each form referring to a different
illuminated by a plane wave characterized by a wave coordinate system but with exactly the same common
vector k, basis vector functions. The connections between the
alternative representations of the same field are
k 5 k1ix sin a cos b 1 iy sin a sin b 1 iz cos a2, 1192 provided by the addition theorems, i.e., the expansion
of the basis set of one representation in terms of the
which indicates that there is an incident angle a with basis set of another. Such addition theorems for the
respect to the z axis and an angle b between the x axis spherical vector wave functions have been obtained

20 July 1995 @ Vol. 34, No. 21 @ APPLIED OPTICS 4577

by Stein11 and Cruzan.12 The translational addition After interchanging 1m, n2 with 1µ, n2 and rearranging
theorem is represented by12 the expansion coefficients, we have
` n ` n
Mmn 5 oo
n50 µ52n
1A0mn mn
µn M8µn 1 B0µn N8µn2, Es1l, j2 5 2 o o
n51 m52n
iEmn 3 pl,mnj N112 l, j 112
mn 1 qmnMmn4,

` n
` n
k
Nmn 5 oo
n50 µ52n
1B0mn mn
µn M8µn 1 A0µn N8µn2, 1222 Hs1l, j2 5 2 oo
vµ n51 m52n
Emn3ql,mnj N112 l, j 112
mn 1 pmnMmn4, 1252

where Mmn and Nmn are the basis vector spherical

wave functions about an origin O and M8µn and N8µn are where
about another diplaced origin O8; M8µn and N8µn are of ` n
the same form as Mmn and Nmn; A0mn mn
µn and B0µn are the
so-called translation or addition coefficients, given in pl,mnj 5 2 oo
n51 µ52n
3alµn Aµn l µn
mn1l, j2 1 bµn Bmn1l, j24 1l fi j2,
Appendix B. These translation coefficients depend
on the relative separation and direction of the dis- ` n
placed origin O8 with respect to O. ql,mnj 5 2 oo
n51 µ52n
3alµn Bµn l µn
mn1l, j2 1 bµn Amn1l, j24 1l fi j2.

C. Total Incident Field of a Constituent Sphere

1262
From the addition theorem, the translation of the
vector spherical wave functions from the lth to the jth Special attention should be paid to the translation
coordinate system takes the form coefficients in Eqs. 1262: A0µn µn
mn and B0mn have been
µn µn
` n replaced by Amn and Bmn, respectively. The relations
between 1A0µn µn µn µn
mn, B0mn2 and 1Amn, Bmn2 are as follows:
M132
mn1l2 5 o o 3A0
n50 µ52n
mn
µn 1l, j2M112 mn 112
µn1 j2 1 B0µn 1l, j2Nµn1 j24,

Eµn 12n 1 121n 1 m2!1n 2 µ2!

` n
Aµn
mn 5 A0µn
mn 5 i
n2n
A0µn
mn,
N132
mn1l2 5 oo
n50 µ52n
3B0mn
µn 1l, j2M112
µn1 j2 1 A0mn
µn 1l, j2N112
µn1 j24. Emn 12n 1 121n 2 m2!1n 1 µ2!
Eµn 12n 1 121n 1 m2!1n 2 µ2!
1232 Bµn
mn 5 B0µn
mn 5 i
n2n
B0µn
mn.
Emn 12n 1 121n 2 m2!1n 1 µ2!
Because Nmn and Mmn in either the lth or the jth
coordinate system have exactly the same form, the 1272
coordinate system indicator for these two basis vector
According to Eqs. 172, 1162, 1172, 1252, and 1262, the
functions is suppressed below. Also, in practical
expansion coefficients of the total incident field of the
applications of our problem, we do not need to include
jth sphere are given by
the modes with index n 5 0, based on the forms of the
vector field solutions discussed in Subsection 3.A.1. L L
Consequently, the scattered field of the lth sphere has
an expansion in the jth coordinate system as follows:
p jmn 5 o
l51
pl,mnj , q jmn 5 oq
l51
l, j
mn 1282

` n ` n

Es1l, j2 5 o o
n51 m52n
iEmn almn A 5o n51 µ52n
o 3A0mn 112
µn 1l, j2Nµn
or in detail,

6
11,L2 ` n
1 B0mn 112
µn 1l, j2Mµn4 p jmn 5 p j,mnj 2 oo o
lfi j n51 µ52n
3alµn Aµn l µn
mn1l, j2 1 bµn Bmn1l, j24,

` n

1 blmn 5o o
n51 µ52n
3B0mn 112
µn 1l, j2Nµn
q jmn 5 q j,mnj 2
11,L2

oo o
` n

3alµn Bµn l µn
mn1l, j2 1 bµn Amn1l, j24,

6B
lfi j n51 µ52n
112
1 A0mn
µn 1l, j2Mµn4 ,
1292
` n ` n

Hs1l, j2 5
k
o o
vµ n51 m52n
Emn blmn A 5o o n51 µ52n
3A0mn 112
µn 1l, j2Nµn
where the first term on the right-hand side refers to
the initial incident waves and the second term refers
to the fields scattered by other spheres.
1 B0mn 112
µn 1l, j2Mµn4 6
` n 5. Solution of the Interactive Coefficients
1 almn 5o
n51 µ52n
o 3B0mn 112
µn 1l, j2Nµn A. Linear System of the Interactive Coefficients
By inserting Eqs. 1292 into Eqs. 1142, we arrive at a set
1 A0mn 112
µn 1l, j2Mµn4 . 6B 1242 of linear equations that contains the interactive

4578 APPLIED OPTICS @ Vol. 34, No. 21 @ 20 July 1995

scattering coefficients: introduced the order-of-scattering technique to solve
the linear system. However, actual computations
11,L2 ` n

a jmn 5 a jn 5 p j,mnj 2 oo o
lfi j n51 µ52n
3alµn Aµn
mn1l, j2
indicate that convergence of the order-of-scattering
technique is not guaranteed once the number or the
sizes of the spheres exceed a certain limit.18 An
1 blµn Bµn
mn1l, j24 , 6 alternative way to solve for the interactive scattering
coefficients is to use an iteration method that is
11,L2 ` n discussed below.
5
b jmn 5 b jn q j,mnj 2 oo o
lfi j n51 µ52n
3alµn Bµn
mn1l, j2

B. Asymptotic Iteration Method for Solving the Coefficients

1 blµn Aµn
mn1l, j24 .6 1302 To solve for the interactive scattering coefficients, a jmn
and b jmn, an asymptotic iteration method that uses
Lo and his colleagues 1Liang and Lo, Bruning and Lo2 Eqs. 1142 and 1292 repeatedly can be used. The itera-
were to our knowledge the first to derive a similar tion may take the following form:
result for the interactive coefficients of two-sphere
systems. Fuller and Kattawar later extended the 1. Starting with 0a jmn 5 0b jmn 5 0. From Eqs. 1292
application of the same form of linear equations to
it follows that
clusters of spheres. It is no surprise that the interac-
tive coefficients of a sphere in the cluster are deter-
mined by three major factors: 112 the physical proper-
1
p jmn 5 p j,mnj , q jmn 5 q j,mnj ,
1
1322
ties of the sphere itself, represented by the Mie
coefficients; 122 the interacting properties of the clus- and from Eqs. 1142
ter determined by the configuration of the cluster and 1 l
the physical properties of all the spheres in the aµn 5 aln1plµn, 1 l
bµn 5 bln1qlµn. 1332
cluster, implied in p jmn and q jmn; and 132 the profile of
In Eqs. 1322 and 1332 the prescript integer indicates the
the incident waves, implied in p j,mnj and q j,mnj . Two sequential number of the iteration; the notation 1µ, n, l2
things are worth noting here:
is equivalent to 1m, n, j2. Only Mie scattering is
involved at this stage.
1. We need only to solve the linear system for the
2. In a similar manner, we next use the new
scattering coefficients a jmn and b jmn, because there
values of the scattering coefficients in Eqs. 1292, and
exist simple relations between the interactive scatter-
ing coefficients and the internal coefficients: the procedure is continued by the process
11,L2 ` n
d jna jmn 2 a jnd jmn 5 0, c jnb jmn 2 b jnc jmn 5 0. 1312 i
p jmn 5 p j,mnj 2 oo o
lfi j n51 µ52n
3i21a lµn Aµn
mn1l, j2
2. The highest order N required for convergence
for the cluster is approximately the largest value in 1 i21blµn Bµn
mn1l, j24,
Mie calculations for all the constituents. For a single 11,L2 ` n
homogeneous sphere of size parameter x, Bohren and
Huffman suggest a value slightly larger than x be
i
q jmn 5 q j,mnj 2 oo o
lfi j n51 µ52n
3i21a lµn Bµn
mn1l, j2
sufficient. In their code BHMIE they use a criterion
1x 1 4x1@3 1 22. Examining Eqs. 1142 shows that the 1 i21blµn Aµn
mn1l, j24, 1342
same criterion should hold for a cluster of spheres if
i l
the largest size parameter is taken among all the aµn 5 11 2 f 2i21alµn 1 falniplµn,
spheres.
i l
bµn 5 11 2 f 2i21blµn 1 f blniqlµn, 1352
In the linear system 1302, all the Mie coefficients, a jn,
b jn, c jn, and d jn, are calculated by the Mie theory for all until all the coefficients show no significant improve-
the individual spheres, p j,mnj and q j,mnj are the expansion ment.
coefficients of the incident waves, and there are
2LN1N 1 22 unknown interactive scattering coeffi- The numerical factor f 10 , f # 12 is introduced in Eqs.
cients in 2LN1N 1 22 linear equations, provided that 1352 to improve the convergence property of the linear
the system is convergent after n 5 N. This linear system. In our actual calculations, some multi-
system can be written in the form of a matrix sphere systems do not converge if f 5 1, but they do
equation in which the translation coefficients consti- converge when the value of f is reduced to, say, 0.7.
tute the coefficient matrix. In principle, the un-
known interactive coefficients can be solved by the
6. Total Scattered Field and the Internal Fields
use of direct matrix inversion. But the direct solu-
tion is often not feasible in practice whenever the Once all the interactive coefficients, a jmn, b jmn, c jmn, and
number of spheres or the size parameters of some d jmn, are found, the total scattered field of the entire
spheres in the cluster is large. Fuller and Kattawar cluster in the primary coordinate system can be

20 July 1995 @ Vol. 34, No. 21 @ APPLIED OPTICS 4579

obtained when the translation addition theorem is cients. When electromagnetic waves illuminate a
applied again, which is expressed in the forms collection of particles, the electromagnetic energy of
the incident radiation is usually not only scattered
` n
but also absorbed by the particles. The presence of
Es 5 o o
n51 m52n
iEmn3amnN132 132
mn 1 bmnMmn4, the particles results in extinction of the incident
waves. Similar to the approach used by Bohren and
k ` n Huffman29 for deriving the expressions for cross sec-
Hs 5 o o
vµ n51 m52n
Emn3bmnN132 132
mn 1 amnMmn4, 1362 tions of a single sphere, we obtain the expressions for
cross sections of a cluster of spheres by calculating the
net rate at which electromagnetic energy crosses the
where surface of an imaginary sphere enclosing the whole
L ` n cluster. Here we consider only the case in which the
surrounding medium is nonabsorbing.
amn 5 oo o
l51 n51 µ52n
3alµn Aµn l µn
mn1l, j02 1 bµn Bmn1l, j024,
An electromagnetic wave of arbitrary polarization
L ` n
can be represented by a column vector, the Stokes
vector, the four elements of which are the Stokes
bmn 5 oo o
l51 n51 µ52n
3alµn Bµn l µn
mn1l, j02 1 bµn Amn1l, j024. 1372 parameters. In general, the state of polarization of
an incident wave is changed on interaction with
In Eqs. 1372 use has been made of the properties scatterers, with the exception of perfectly symmetric
particles. Thus it is possible to represent the scatter-
Aµn
mn1 j0, j02 5 dµmdnn, 1382 ing properties of scatterers by a 4 3 4 scattering
matrix, known as the Müller matrix, that describes
Bµn
mn1 j0, j02 5 0, 1392 the relation between the incident and the scattered
Stokes vectors. All the information about angular
where dµm or dnn is the Kronecker delta. Also, we scattering by a collection of particles is contained in
assume that the series expansion 1372 of the scattered its scattering matrix. The form of the scattering
field is uniformly convergent. Therefore we can ter- matrix reflects general properties of the scatterers.
minate the series at n 5 N, and the resulting error This scattering matrix is related to the 2 3 2 ampli-
will be arbitrarily small if N is sufficiently large. tude-scattering matrix that describes the relation
This representation of the total scattering coefficients between the amplitudes of the incident and the
defined by Eqs. 1372 has been discussed by Borghese et scattered fields. A derivation of analytical expres-
al.21 and by Mackowski.18 sions for the four elements of the amplitude-scatter-
In a similar manner, the expressions for the inter- ing matrix is given below. Also, a derivation of the
nal fields of each sphere in the primary coordinate expressions for the cross sections from the far-field
system can be obtained by the use of approximation and the optical theorem is given, and
` n
it confirms that the results are consistent with those
obtained with the exact integration.
EI1 j, j02 5 2 o o
n51 m52n
iEmn3d j,mnj0N112 j, j0 112
mn 1 c mn Mmn4,

kj ` n A. Extinction and Scattering Cross Sections

HI1 j, j02 5 2 o o
vµ j n51 m52n
Emn3c j,mnj0N112 j, j0 112
mn 1 d mn Mmn4, Once we have obtained the internal and the scattered
electromagnetic fields, we are able to determine the
1402 Poynting vector at any point in space. For any point
outside the cluster, the complex Poynting vector 1i.e.,
where the time-averaged Poynting vector2 S can be written
as29
` n

c j,mnj0 5 oo
n51 µ52n
3c jµn Aµn j µn
mn1 j, j02 1 d µn Bmn1 j, j024, S 5 Si 1 Ss 1 Sext, 1422

` n where
d j,mnj0 5 oo
n51 µ52n
3d jµn Bµn
mn1 j, j02 1 c jµn Aµn
mn1 j, j024. 1412
Si 5 1⁄2 Re1Ei 3 H*i 2, Ss 5 1⁄2 Re1Es 3 H*s 2,

The translation coefficients in either Eqs. 1372 or 1412
are essentially the same as those used in Eqs. 1302
except that the former are governed by the Hankel
function of the first kind and the latter are governed
by the Bessel function of the first kind.
7. Scattering Properties of the Sphere Cluster
With all the interactive scattering coefficients solved,
we now proceed to derive expressions for the scatter-
ing properties of the cluster in terms of these coeffi-
Sext 5 1⁄2 Re1Ei 3 H*s 1 Es 3 H*i 2. 1432
The superscript * stands, as usual, for the complex
conjugate. Si, the complex Poynting vector associ-
ated with the incident wave, is independent of posi-
tion if the surrounding medium is nonabsorbing.
Ss is the complex Poynting vector of the scattered
field. Sext may be interpreted as the term that arises
from the interaction between the incident and the
scattered waves. Let Wa be the rate at which electro-

4580 APPLIED OPTICS @ Vol. 34, No. 21 @ 20 July 1995

magnetic energy is absorbed by the scatterers, Ws be where the argument cos u of the functions pmn and tmn
the rate at which energy is scattered across the has been suppressed for succinctness, and the Riccati–
surface A, and Wext be the sum of the energy absorp- Bessel functions are defined by
tion and the energy scattering rates. Then we can
write29 cn1r2 5 r jn1r2, jn1r2 5 rh112
n 1r2. 1492
Wa 5 Wext 2 Ws, 1442
By substituting the series expansions 1482 into the
where integral 1462 for Ws and integrating the resulting
product series term by term, we obtain
Wext 5 2 e
A
Sext · irdA, Ws 5 2 e A
Ss · irdA, 1452
2p 0 E0 0 2 ` n
1n 2 m2!
and A is the surface of an imaginary sphere that
Ws 5
kvµ0 o o
n51 m52n
n1n 1 1212n 1 12
1n 1 m2!
encloses the scatterers. Equations 1452 can also be
written in the form29 3 Re12ij*nj8namna*mn 1 ijnj8* mn2,
n bmnb* 1502
2p p

Wext 5
1
2
Re ee
0 0
1EifH*su 2 EiuH*sf
where we have used the relations

1n 2 m2! 2
2 EsuH*if 1 EsfH*iu2r2 sin ududf,
2p p
EmnE*mn 5 0 E0 0 212n 1 122 31n 1 m2!4 , 1512

Ws 5
1
2
Re ee 0 0
1EsuH*sf 2 EsfH*su2r2 sin ududf,
e
2p

exp1imf23exp1im8f24*df
1462 0

where r, the radius of the imaginary sphere, is 5 2pdmm8, 1522

arbitrary. According to Eqs. 1172 and 1362 and expres-
p
sions 122, the components of the incident and the
scattered fields are, respectively,
` n
e0
1pmnpmn 1 tmntmn2sin udu
exp1imf2
Eiu 5 oo
n51 m52n
Emn12ip0mnc8ntmn 1 q0mncnpmn2
kr
,
5 dnn
2n1n 1 12 1n 1 m2!
. 1532
` n
2n 1 1 1n 2 m2!
exp1imf2
Eif 5 oo
n51 m52n
Emn1iq0mncntmn 1 p0mnc8npmn2
kr
,
In Eq. 1502, j*nj8n and jnj8*n are functions of r, the
arbitrary radius of an imaginary sphere. When r is
` n
k sufficiently large, the spherical Hankel function of the
Hiu 5
vµ0 n51 m52n o o Emn first kind is asymptotically given by
exp1imf2 12i2nexp1ikr2
3 1ip0mncntmn 2 q0mnc8ntmn2 , ,
kr h112
n 1kr2 , kr :n2, 1542
ikr
` n
k
Hif 5
vµ0 o o
n51 m52n
Emn and the Riccati–Bessel function jn and its derivative
j8n with respect to kr are given by
exp 1imf2
3 1iq0mnc8npmn 1 p0mncntmn2 , 1472 jn , 12i2n11exp1ikr2, j8n , 12i2nexp1ikr2, 1552
kr
` n
exp1imf2 whence
Esu 5 oo
n51 m52n
Emn12iamnj8ntmn 2 bmnjnpmn2
kr
,
ijnj8*
n 5 2 ij*
nj8n 5 1. 1562
` n
exp1imf2 The scattering cross section is thus
Esf 5 oo
n51 m52n
Emn12ibmnjntmn 2 amnj8npmn2
kr
,

` n Ws
k Csca 5
Hsu 5
vµ0 o o
n51 m52n
Emn Ii
` n
exp 1imf2 4p
3 1iamnjnpmn 1 bmnj8ntmn2
kr
, 5
k2 o o
n51 m52n
n1n 1 1212n 1 12

n
k `
1n 2 m2!
Hsf 5
vµ 0 o o
n51 m52n
Emn 3
1n 1 m2!
1 0 amn 0 2 1 0 bmn 0 22, 1572

exp 1imf2 where Ii is the incident irradiance, which is k 0 E0 02@

3 1ibmnj8npmn 2 amnjntmn2 , 1482
kr 2vµ0. Similarly, by substituting the expansions 1472

20 July 1995 @ Vol. 34, No. 21 @ APPLIED OPTICS 4581

and (48) into the integral 1462 for Wext and using Eqs. in a matrix form,
1512, 1522, and 1532, we obtain the extinction cross
Es exp3ik1r 2 z24 S2 S3 Ei
1E 2 3S S 41E 2 ,
section as
5 (63)
's 2ikr 4 1 'i
Wext
Cext 5
Ii where the elements Sj 1 j 5 1, 2, 3, 42 of the amplitude-
` n
scattering matrix S depend, in general, on both u and
4p f. The components 1Es, E's2 and 1Ei, E'i2 of the
5
k2 o o
n51 m52n
n1n 1 1212n 1 12
scattered and the incident fields are parallel and
perpendicular to the scattering plane, respectively.
1n 2 m2! The scattering plane is uniquely defined by the direc-
3 Re1 p0mn
* amn 1 q0mn
* bmn2. 1582 tion of the incident wave vector k and the scattering
1n 1 m2!
direction ir. For a general case, these parallel and
Here we have used the relations perpendicular components do not have simple rela-
tions with the transverse-field components 1Eu, Ef2.
Re1 p0mna*mn2 5 Re1 p0mn*amn2, However, there is a special case in which explicit
expressions for the elements of the amplitude-
Re1q0mnb*mn2 5 Re1q0mn*bmn2. 1592 scattering matrix can be found.
If a single plane-incident wave is considered and
Also, when r is sufficiently large, the incident wave vector k defines the z axis of the
reference system, the two components of the incident
n1n 1 12p
cn1r2 , cos r 2 3 2 4, electric field for an arbitrary linear polarization angle
b are
n1n 1 12p
c8n1r2 , 2 sin r 2 3 2 4, Ei 5 E01cos f cos b 1 sin f sin b2,
E'i 5 E01sin f cos b 2 cos f sin b2, 1642
2i1c8nj*n 1 c*nj8n2 5 i1cnj8* n j8n2 5 1.
n 1 c8* 1602
where b 5 0 corresponds to a case of the plane
The absorption cross section is simply obtained by x-polarized incident wave and b 5 90° to the
y-polarized incident wave. Thus we have
Cabs 5 Cext 2 Csca. 1612
Es Esu
B. Expressions for the Far Field and the
1E 2 5 12E 2
's sf
Amplitude-Scattering Matrix
exp3ik1r 2 z24 S2 S3 E0 cos1f 2 b2
The scattered field in the far zone of the ensemble is
often of practical interest. When the asymptotic
5
2ikr 3S S 43E sin1f 2 b24 .
4 1 0
1652

expressions 1552 of the Riccati–Bessel functions for the

scattered electric field are substituted into the series This case is illustrated in Fig. 2. Using expressions
1482, the resulting transverse components are 1622 and the equations

` n 1n 2 m2!
exp1ikr2 1n 2 m2! p2m,n 5 1212m11 pmn,
Esu , E0
2ikr o o
n51 m52n
12n 1 12
1n 1 m2!
1n 1 m2!
1n 2 m2!
3 1amntmn 1 bmnpmn2exp1imf2, t2m,n 5 1212m tmn, 1662
1n 1 m2!
` n
exp1ikr2 1n 2 m2!
Esf , E0
2ikr o o
n51 m52n
12n 1 12
1n 1 m2!
leads to

3 1amnpmn 1 bmntmn2i exp1imf2. 1622 S2 cos1f 2 b21 S3 sin1f 2 b2

` n
In practical applications, these series are supposed to
be truncated at some n 5 N, and the resultant error
5 o o 1C
n51 m50
mn cos mf 1 Fmni sin mf2,
incurred because of the truncation is assumed to be
insignificant. However, we still write the summa- S4 cos1f 2 b21 S1 sin1f 2 b2
tion over a range of 11, `2 about n. Because of the ` n
linearity of the boundary conditions, the amplitude of
the scattered field is a linear function of the ampli- 5 i o o 1U
n51 m50
mn cos mf 1 Jmni sin mf2,
tude of the incident field. The relation between
incident and scattered fields is conveniently written- 1672

4582 APPLIED OPTICS @ Vol. 34, No. 21 @ 20 July 1995

where scattering matrix can be derived to be
` n
2n 1 1 1n 2 m2!
Cmn 5 3
1 1 d0m 1n 1 m2!
1amntmn 1 bmnpmn2 S21u, f2 5 o o 5C
n51 m50
mn cos31m 2 12f 1 b4

1 1212m1a2mntmn 2 b2mnpmn2 , 4 1 iFmn sin31m 2 12f 1 b46,

` n

Fmn 5
2n 1 1 1n 2 m2!
31n 1 m2! 1a
mntmn 1 bmnpmn2
S31u, f2 5 2 o o 5C
n51 m50
mn sin31m 2 12f 1 b4
1 1 d0m

2 1212m1a2mntmn 2 b2mnpmn2 , 4 2 iFmn cos31m 2 12f 1 b46,

` n

2n 1 1 1n 2 m2!
S41u, f2 5 2 o o 5iU mn cos31m 2 12f 1 b4
Umn 5 3
1 1 d0m 1n 1 m2!
1amnpmn 1 bmntmn2
n51 m50

2 Jmn sin31m 2 12f 1 b46,

m
2 1212 1a2mnpmn 2 b2mntmn2 , 4 ` n

S11u, f2 5 o o 5iU mn sin31m 2 12f 1 b4

2n 1 1 1n 2 m2! n51 m50
Jmn 5 3
1 1 d0m 1n 1 m2!
1amnpmn 1 bmntmn2
1 Jmn cos31m 2 12f 1 b46. 1692

1 1212m1a2mnpmn 2 b2mntmn2 . 4 1682 With the four elements of the amplitude-scattering

It follows that the four elements of the amplitude-
matrix known, the scattering matrix, i.e., the Müller
matrix, which relates the incident and the scattered
Stokes parameters, can be found easily 3for example,
see Bohren and Huffman,29 equations 13.1224. One
must always bear in mind that Eqs. 1692 are valid only
when the z axis is parallel to the direction of propaga-
tion of the plane-incident wave. For this particular
case, we derive the cross sections from the optical
theorem as a check of Eqs. 1572 and 1582, which we
obtained for a general case in Subsection 7.A. We
use V for the vector scattering amplitude, which is
related to the scalar amplitude-scattering matrix S as
follows:

V 5 3S2 cos1f 2 b2 1 S3 sin1f 2 b24iu

2 3S4 cos1f 2 b2 1 S1 sin1f 2 b24if. 1702

Accordingly, the cross sections can be obtained by the

use of the following equations29:
2p p

Csca 5 ee 0 0
0V02
k2
sin ududf, 1712

4p
Cext 5 Re31V ·iV2u504, 1722
k2

where

iV 5 ix cos b 1 iy sin b 5 sin u cos1f 2 b2ir

Fig. 2. When the direction of propagation of a plane-incident
wave is parallel to the z axis, the components of the scattered field
1Es, E's2 are rather simply related to the components of the
incident wave 1Ei, E'i2. In this case Es 5 Eus, E's 5 2Efs and
the incident electric vector is in the x–y plane.
1 cos u cos1f 2 b2iu 2 sin1f 2 b2if. 1732
By inserting Eqs. 1672 and 1682 into Eqs. 1712, we
again obtain the scattering cross section, which is of
exactly the same form as in Eq. 1572. With u 5 0,

20 July 1995 @ Vol. 34, No. 21 @ APPLIED OPTICS 4583

Eqs. 1672 become and Eqs. 1212, which give rise to

S210, f2cos1f 2 b2 1 S310, f2sin1f 2 b2 exp12ib2

p01n 5 q01n 5 ,
` 2
2n 1 1
5 o
n51 2 0
p21n 52
exp12ib2
, 0
q21n 5
exp12ib2
. 1782
2n1n 1 12 2n1n 1 12
3 3a1n 1 b1n 2 n1n 1 121a21n 2 b21n24cos f
As a result, from Eqs. 1722, or equivalently from
`
2n 1 1
1 o
n51 2 4p
Cext 5 Re3S1024, 1792
k2
33a1n 1 b1n 1 n1n 1 121a21n 2 b21n24i sin f,
S410, f2cos1f 2 b2 1 S110, f2sin1f 2 b2 we arrive at

` `
2n 1 1 4p
52 o
n51 2
Cext 5
k2 o 12n 1 12Re3 p *a
n51
0
1n 1n 1 q01n*b1n

0* 0*
3 3a1n 1 b1n 1 n1n 1 121a21n 2 b21n24i cos f 1 n21n 1 1221 p21n a21n 1 q21n b21n24, 1802
`
2n 1 1 This agrees with what we obtained in Eq. 1582, which
1 o
n51 2 turns out to be exactly the same result because p0mn 5
q0mn 5 0 for all normal modes with m fi 61 in this case.
3 3a1n 1 b1n 2 n1n 1 121a21n 2 b21n24sin f, 1742
C. Summary of the Expressions for Scattering Properties of
where we have used the following properties: the Clusters
1 The results obtained so far in this section are summa-

5
m 5 21 rized as follows:
2
pmn112 5 n1n 1 12 1a2 For the general case, the cross sections are
m51 given by Eqs. 1572, 1582, and 1612; no general explicit
2
expressions for the elements of the amplitude-
0 otherwise, scattering matrix are given.
1b2 When the direction of propagation of a plane-
1

5
incident wave is parallel to the z axis, the formula for
2 m 5 21
2 the scattering cross section remains the same as in
Eq. 1572; the expression for the extinction cross section
pmn112 5 n1n 1 12 1752 is simplified as shown in Eq. 1802, because the expan-
m51
2 sion coefficients for all the modes other than m 5 61
vanish in this case, and the expressions for the
0 otherwise. elements of the amplitude-scattering matrix are given
by Eqs. 1692 with 1682 for an arbitrary polarization
From Eqs. 1702, 1732, and 1742 it follows that angle of b. When b 5 0, the incident plane wave is x
polarized, and when b 5 90°, it is y polarized. For
Re3S1024 5 Re31V · iv2u504 these two particular states of linear polarization of
the plane-incident wave, the explicit expressions for
`
the extinction cross section and the four elements of
5 o 12n 1 12Re3 p *a
n51
0
1n 1n 1 q01n*b1n the amplitude5scattering matrix can be written as
`
0* 0* 2p
1 n21n 1 1221 p21n a21n 1 q21n b21n24, 1762 x
C ext5
k2 o 12n 1 12
n51
where we have also used the relations from the
properties of complex numbers 3 Re3a1n 1 b1n 2 n1n 1 121a21n 2 b21n24,
`
2p
Re31a21n 1 b21n2exp12if24 5 Re31a*21n 1 b*21n2exp1if24, y
C ext 5
k2 o 12n 1 12
n51
0 0*
Re1 p21n a*21n2 5 Re1 p21n a21n2, 3 Re5i3a1n 1 b1n 1 n1n 1 121a21n 2 b21n246,
0 0*
Re1q21n b*21n2 5 Re1q21n b21n2, 1772 1812

4584 APPLIED OPTICS @ Vol. 34, No. 21 @ 20 July 1995

 ` n orientation for six sets of sphere chains, each consist-
S x21u, f2 5 oo
n51 m50
ing of two or three identical spheres in various
intersphere separations. For all the cases, the axis
3 3Cmn cos1m 2 12f 1 iFmn sin1m 2 12f4, of symmetry of each sphere chain is perpendicular to
either the scattering plane 1x–z plane2 or the incident
` n wave vector 1along the z axis2. In other words, it is
S x31u, f2 5 2 oo
n51 m50
always parallel to the y axis. The polarization com-
ponents of scattering intensities i11 and i22 correspond
to the scattered-field components, perpendicular or
3 3Cmn sin1m 2 12f 2 iFmn cos1m 2 12f4,
parallel to the scattering plane, respectively. In our
` n calculations,
S x41u, f2 5 2 oo
n51 m50 i11 5 0 S y11u, 02 0 2,
3 3iUmn cos1m 2 12f 2 Jmn sin1m 2 12f4, i22 5 0 S x21u, 02 0 2. 1842
` n

S x11u, f2 5 oo
n51 m50
These dimensionless quantities are independent of
the measurement or computational units used. The
physical and geometric parameters of the chains of
3 3iUmn sin1m 2 12f 1 Jmn cos1m 2 12f4, spheres are listed in Table 1. Figure 3 shows the
1822 comparison of our theoretical calculations against the
corresponding experimental data for these sphere
` n chains.
S y21u, f2 5 2 oo
n51 m50
9. Remarks
3 3Cmn sin1m 2 12f 2 iFmn cos1m 2 12f4,
1a2 The Mie theory is a special case of the multi-
` n sphere theory described above. For the Mie case,
S y31u, f2 5 2 oo
n51 m50
i.e., the case of a linearly polarized plane-incident
wave propagating along the z axis, all the formula-
3 5Cmn cos31m 2 12f4 1 iFmn sin1m 2 12f6, tions turn out to be in complete agreement with the
Mie formulation when L 5 1. When the plane-
` n incident waves is x polarized, Eqs. 1142, 1182, 1292, and
S y41u, f2 5 oo
n51 m50
1782 show that

an bn
3 3iUmn sin1m 2 12f 1 Jmn cos1m 2 12f4, a1n 5 , b1n 5 ,
2 2
` n

S y11u, f2 5 oo
n51 m50 a21n 5 2
an
, b21n 5
bn
, 1852
2n1n 1 12 2n1n 1 12
3 3iUmn cos1m 2 12f 2 Jmn sin1m 2 12f4,
1832

with Cmn, Fmn, Umn, and Jmn given by Eqs. 1682, and
the superscript x or y indicates the state of polariza- Table 1. Sphere-System Parameters
tion of the incident plane wave. No. of Single-
Spheres Sphere Complex Dimensionless
in the Size Refractive Separation
8. Some Preliminary Numerical Results Chain Parameter Index Parameter
The formulation described in this paper has been ID n x m 5 m8 2 im9 ks a
implemented in a computer code. We do not intend 1 2 3.083 1.61 2 i0.004 6.166
to discuss the numerical results in detail. Some of 2 2 3.083 1.61 2 i0.004 8.030
our numerical calculations are presented for illustra- 3 2 4.346 1.63 2 i0.010 9.940
tion. The theoretical predictions are compared with 4 2 4.346 1.63 2 i0.010 10.760
the laboratory scattering measurements obtained by 5 3 3.083 1.61 2 i0.004 6.166
Wang and Gustafson33 through a microwave analog 6 3 3.083 1.61 2 i0.004 7.520
technique. The examples shown here are the angu- as is the center-to-center separation distance between the two

lar distributions 1phase functions i11 and i222 at a fixed neighboring spheres.

20 July 1995 @ Vol. 34, No. 21 @ APPLIED OPTICS 4585

 1b2 As shown in Section 7, Eqs. 1692 are valid only
when the direction of propagation of a linearly polar-
ized plane-incident wave defines the z axis of the
reference coordinate system. In fact, for the case of a
plane-incident wave that is usually considered in
practice, this restriction does not lose any generality.
When the wave vector is initially not parallel to the z
axis, we can always rotate the primary coordinate
system so that the z axis of the new system is
consistent with the incident wave vector. This is a
trivial matter of relative geometric orientation
1c2 Although this paper is basically devoted to a
general scattering theory for multisphere systems
and does not specifically discuss the numerical tech-
niques needed in practical applications, it is worth
mentioning here that the calculation of the transla-
tion coefficients is critical to the problem. As pointed
out above, the addition theorems play a key role in
developing the scattering theory for a multisphere
system. In practical applications, calculating the
vector addition coefficients, i.e., the translation coeffi-
cients, is not without difficulty. The evaluation of
these coefficients requires the determination of the
so-called Gaunt coefficients by the use of a definite
integral of a product of three associated Legendre
Fig. 3. Angular distributions of six sphere chains. The param- functions, as shown in Appendix B. These Gaunt
eters of these sphere chains are listed in Table 1. 112–162, identifica- coefficients are closely related to Clebsch–Gordan
tion numbers of the sphere chains involved. The dotted curve in coefficients, which are often encountered in quantum
each panel is the theoretical prediction for i11, and the solid curve is mechanics,34,35 especially in the calculation of transi-
for i22. The open circles in each panel are the laboratory scatter-
tion amplitudes. Mackowski18 has obtained a set of
ing measurements for i11, and the filled circles are for i22.
recursion relations for the translation coefficients
that bypass the calculation of the Gaunt coefficients.
which, together with Eqs. 1572, 1812, and 1822, leads to We have developed an algorithm to calculate the
Gaunt coefficients directly, which enables us to evalu-
`
2p ate the vector addition coefficients expeditiously.
x
C sca5
k2 o 12n 1 121 0 a 0
n51
n
2
1 0 bn 0 22, Also, a new microwave laboratory has been set up
recently in our department by Gustafson, and the new
`
2p facility is expected to provide more scattering measure-
x
C ext 5
k2 o 12n 1 12Re1a
n51
n 1 bn2, ments of better quality soon. Our numerical and
experimental results will be discussed in details in
S x21u2 5 Sx21u, f2 papers that are now in preparation.
` 1d2 In Section 6, we discussed the total scattered
2n 1 1 field from the sphere cluster as a whole. The single-
5 o n1n 1 12 1a t
n51
n n 1 bnpn2,
field representation described there is based on reex-
pansions of all the individual scattered fields from the
S x31u2 5 Sx41u2 5 S x31u, f2 5 S x41u, f2 5 0, spherical constituents about a common origin. Our
S x11u2 5 Sx11u, f2 actual calculations show that this may be not the best
`
way to construct the total scattered field. We encoun-
2n 1 1 tered some numerical problems in some cases.
5 o n1n 1 12 1a p
n51
n n 1 bntn2, 1862
Further research needs to be done before useful
conclusions can be drawn.
where we have defined pn 5 p1n, tn 5 t1n. When the
plane-incident wave is y polarized, we have
ian ibn Appendix A: Recurrence Formulas for pmn, tmn
a1n 5 2 , b1n 5 2 ,
2 2
Definitions
ian ibn
a21n 5 2 b21n 5 , 1872 ,
2n1n 1 12 2n1n 1 12 mPm
n 1x2
pmn 5 ,
and from Eqs. 1572, 1812, and 1832 similar expressions 11 2 x 221@2
can be obtained for the cross sections and the ampli-
tude-scattering matrix. These results are exactly dPm
n 1x2
tmn 5 11 2 x 221@2 , 21 # x # 1. 1A12
the same as in the Mie theory. dx

4586 APPLIED OPTICS @ Vol. 34, No. 21 @ 20 July 1995

Recurrence Relations n1n
2n 1 1
2n 1 1 n1m
A0mn
µn 1l,
µ n2n
j2 5 1212 i
2n1n 1 12 p50n2n0o 12i2 p
pmn11 5 xpmn 2 pmn21,
n 2 m1 1 n2m11 3 3n1n 1 12 1 n1n 1 12 2 p1 p 1 124
21m 1 12x 3 a1m, n, 2 µ, n, p2h112
p 1kdl, j2
pm11n 5 pmn
11 2 x 221@2
3 Pm2µ
p 1cos ul, j2exp3i1m 2 µ2fl, j4,
1m 1 121n 1 m21n 2 m 1 12 2n 1 1
2 pm21n, B0mn µ n2n
m21 µn 1l, j2 5 1212 i
2n1n 1 12
m fi 1, n1n

1@2
n12n 2 12 3 o
p50n2n0
12i2 pb1m, n, 2µ, n, p, p 2 12
pnn 5 11 2 x2 p1n2121n212, n fi 1,
n21
1A22 3 h112 m2µ
p 1kdl, j2Pp 1cos ul, j2exp3i1m 2 µ2fl, j4,
1B12
n2m11 n11
tmn 5 pmn11 2 xpmn, m fi 0,
m m where
2n 1 1 n11
t0n11 5 xt0n 2 xt0n21, 1A32 b1m, n, 2µ, n, p, p 2 12
n n
2p 1 1
1n2 m2! 5 31n 2 µ21n 1 µ 1 12a1m, n, 2µ 2 1, n, p 2 12
m11
2p 2 1
p2mn5 1212 pmn,
1n 1 m2! 2 1 p 2 m 1 µ21 p 2 m 1 µ 2 12
pmn12x2 5 1212n1mpmn1x2, 1A42 3 a1m, n, 2µ 1 1, n, p 2 12
1n2 m2! 1 2µ1 p 2 m 1 µ2a1m, n, 2µ, n, p 2 124, 1B22
t2mn5 1212m tmn,
1n 1 m2!
and the a1m, n, µ, n, p2 terms are defined by
tmn12x2 5 1212n1m11tmn1x2. 1A52
Pm µ
n 1cos u2Pn 1cos u2
Special Values n1n

p00 5 0, p015 0, p10 5 0, p11 5 1,

5 o
p50n2n0
a1m, n, µ, n, p2Pm1µ
p 1cos u2, 1B32

t00 5 0, t0,1 5 211 2 x 221@2, t10 5 0, t11 5 x, which can be also written as
1A62
2p 1 1 1 p 2 m 2 µ2!
1 a1m, n, µ, n, p2 5
122
5
m 5 21 2 1 p 1 m 1 µ2!
162n11
1
tmn1612 5
162n11
n1n 1 12
3 2 4 m51
3 e 21
Pm µ m1µ
n 1x2Pn 1x2Pp 1x2dx. 1B42

0 otherwise, In Eqs. 1B12, 1dl, j, ul, j, fl, j2 are the spherical coordinates
of the center of the lth sphere in the jth coordinate
1
122
5
2162n m 5 21 system. For the translational coefficients used in
Eqs. 1372 and 1412, h112 p is replaced by jp.
n1n 1 12 For the scattering theory presented in this paper,
tmn1612 5
162n 3 2 4 m51
1A72
the translation coefficients defined above need a slight
modification, which is shown by Eqs. 1272.
0 otherwise.
The author thanks Bo Å. S. Gustafson for inspiring
this paper and for many useful discussions and S. F.
mn mn
Appendix B: Translation Coefficients A0mn , B0mn Dermott, the Chairman of the Department of As-
A0mn
µn 1l,j2 and B0mn
µn 1l, j2 are the translation coeffi-
tronomy of the University of Florida, for continuing
cients needed for the transformation from the lth to support and encouragement. Special thanks also go
the jth coordinate system.19 to S. F. Dermott and Bo Å. S. Gustafson for improv-

20 July 1995 @ Vol. 34, No. 21 @ APPLIED OPTICS 4587

ing the English. The author also expresses his appre-
ciation to graduate students S. Jayaraman and S.
Kortenkamp for their careful review of the manuscript.
The author is deeply grateful to an anonymous ref-
eree for his valuable comments and careful reading of
a previous version of this paper. This work was
supported by NASA through grants NAGW-2482,
NAGW-1923, and NAGW-2775.
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