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2010 IEEE Nanotechnology Materials and Devices Conference

Oct 12 - 15, 2010, Monterey, California, USA

FrA1-1.4

A Second Order Approximation for the Quasistatic


Properties of a Nanoegg
Sami Smaili and Yehia Massoud
Department of Electrical and Computer Engineering
Rice University
Houston, TX 7005
massoud@rice.edu
AbstractBreaking the symmetry in plasmonic
nanoparticles offers additional degrees of freedom
that can be utilized to increase the tunability of
such nanoparticles. Metallic shells with non-concentric
dielectric cores possess such properties, where the core
displacement affects the wavelength at which plasmon
resonance occurs. It remains important to have analytical
formulation for the properties of such nanoparticles
especially for the design and optimization for nanoparticle
based devices. In this paper we present an analytical
formulation for capturing the resonant properties of
asymmetrical nanoparticles based on the quasistatic
approximation of Maxwells equations.

I. I NTRODUCTION
Small in size and showing unique resonance
properties, metallic nanoparticles have been used
in applications like cancer treatment and chemical
sensing [1], and each application and setting poses
its own constraints and requirements on the performance of the particle. It is therefore desirable to
have as much degrees of freedom in the nanoparticle
used so that the varying requirements in different contexts can be met. Tunability of nanoparticles stem from the dependence of the resonance
properties on different factors such as size and
shape, where, for example, the resonance properties of nanoshells and nanorods depend on their
aspect ratios [1], [2]. Asymmetry has been proposed
to add more degrees of freedom, thus increasing
the tunability of nanoparticles; the properties of a
nanoshell with non-concentric dielectric core and
shell depends, in addition to the aspect ratio, on
the displacement of the inner core with respect to
the center of the shell [3].
With the wide range of settings in which
nanoaprticles are used, developing efficient method978-1-4244-8897-1/10/$26.00 2010 IEEE

ologies for the analysis and properties of the


nanoparticles becomes critical. On the one hand,
more degrees of freedom enable more flexibility
in the design of the nanoparticles, but put more
burdens on the simulation and analysis due to the increased number of parameters to consider. Typically,
the properties of asymmetric nanoparticles like the
nanoeggs are studied using numerical techniques
like the finite-difference time domain or the finite
element method [3], [4]. However, it is desirable to
have more efficient tools to allow for better design
and analysis of the nanoparticles properties. One
approach is to utilize the fact that small nanoparticles have sizes much smaller than the exciting
wavelength [5]. Under these conditions, quasistatic
analysis of the scattering of electromagnetic fields
by these particles becomes justified; the quasistatic
approximation is easy to solve and yields efficient
and accurate results. Having efficient models that
capture the properties of the nanostructure at hand is
important particularly because of the varying environments under which current and future nanostructures are to operate within, and the many variables
that can affect the performance of nanostructures
[6][29]. Having efficient models for the nanostructure allows the use of design optimization schemes
to predict the parameters combination that results
in optimal performance of the nanosystem under
the conditions imposed by the given application
[23], [30][45]. This is also particularly important
in nanoscale systems where process variations become more significant [42], [46][56]. Finally, with
efficient models, the performance of nanoscale systems can be efficiently evaluated before fabrication,
which would enhance the yield [57][75].
In this paper we study the behavior of non-

267

concentric core-shell particles [3] in the quasistatic


regime. We develop an analytical formulation for the
scattering of light by nanoeggs by solving Laplaces
equation for the electric potential. At the heart of
our method lies the translation theorem for spherical
harmonic functions, which is utilized to change the
origin of the function expansions in different regions
of the nanoegg.
II. M ETHOD F ORMULATION
Metallic nanoparticles typically resonate at wavelengths much larger than their size [5]. In such a
situation Maxwells equations can be solved in the
quasistatic regime where the electric field satisfies
E = 0 and so there is a scalar field, the electric
potential, such that E = and satisfies
Laplaces equation 2 = 0 [76]. Additionally,
the potential function should satisfy the boundary
conditions at the metal-outer medium interface and
the core-metal interface, given by the continuity
of the tangential electric and normal displacement
fields. In out formulation, we denote by out , m ,
and d the potential function in the outer medium,
the metallic shell, and the dielectric core of the
particle. The dielectric core is centered at the point
Cd and the metallic shell is centered at the point
Cm , with the vector v = CdCm (with magnitude
v) denoting the displacement of the core so that
v = 0 corresponds to a concentric core-shell structure (nanoshell). Finally, we denote the spherical coordinates with the origin at Cm (r1 , 1 , 1 ), and the
coordinates with the origin at Cd by (r2 , 2 , 2 ). The
potential function in the three different regions can
be expressed in terms of the spherical coordinates
by expanding it in a series of spherical harmonic
functions [76],
2
out = B1out r1 cos1 + Aout
1 r1 cos1

2
+ Aout
2 r1 3(3cos1 1)

(1)

m = B1m r1 cos1 + B2m r12 cos(3cos12 1) (2)


2
m
2
+Aout
1 r1 cos1 + A2 r1 3(3cos1 1)
d = B1d r2 cos2 + B2d r22 cos(3cos22 1)

(r2 = a). However, since the potential functions in


different media are represented in one of the two
coordinate systems (out and m around Cm while
d around Cd ), applying the boundary conditions
in one of the two systems can become complicated.
Instead, when we apply the conditions on the core
surface, we use an equivalent representation of m
in the coordinate system around Cd by utilizing the
translation theorems of spherical harmonic functions
[77]. The potential m is then given as
2
m = (B1m vB2m )m r2 cos2 + Am
1 r2 cos2
+ (B2m )r22 (3cos22 1)
m 3
2
+ (Am
(4)
1 v + A2 )r2 (3cos2 1)

The boundary conditions given by


(5)

1out
1m
out
|r=b = m
|r=b

(6)

2m
2d
|r=a =
|r=a

(7)

1out
1
|r=b = m m |r=b

(8)

out

2m
2
|r=a = d d |r=a
(9)
r
r
together with (4) and the condition that at large
distances from the particle, the electric potential
is equal to the potential of the incident field
(limr out = inc ), the coefficients in the potential expansions in (1),(2), and(3) are solved for.
In solving for the coefficients, we use the fact that
the Legendre functions of order 1 and 2, cos and
3cos 1, are orthogonal ( [76]) so that each of
the boundary conditions yields 2 equations for the
coefficients, totaling to 8 equations. The condition
at infinity gives B1out = Eo where Eo is the
incident field, so that the 8 equations obtained from
the boundary conditions contain 8 unknowns (Aout
1 ,
out
m
m
m
m
d
d
A2 , B1 , A1 , B2 , A2 , B1 , and B2 ).
m

(3)

truncating the series at the second order, which


satisfies the efficiency and accuracy tradeoff. The
coefficients in the expressions in (1), (2), and (3)
are determined by applying the boundary conditions
at the surfaces of the shell (r1 = b) and the core

1out
1m
|r=b =
|r=b

III. S IMULATION R ESULTS


The resonance behavior of plasmonic nanoparticles is manifested as a peaking in the field enhancement (ratio of scattered field to incident field)
of the nanoegg. We used our analytical formulation
presented in section (II) to study the behavior of the

268

3.5
(a)
v/(ba)

Field Enhancement

0
0.5
0.99

2.5

1.5

0.5
200

400

600

800

1000

1200

1400

Wavelength (nm)
9
(b)
8

v/(ba)
0
0.5
0.99

Field Enhancement

7
6
5
4
3
2
1
0
200

400

600

800

1000

1200

1400

Wavelength (nm)
15
(c)

Field Enhancement

v/(ba)
0
0.5
0.99

10

0
200

400

600

800

1000

1200

an outer radius of 20nm and inner radii of 13nm


(a), 16nm (b) and 19nm (c). The figure shows that,
regardless of the aspect ratio of the particle, the
resonance wavelength red-shifts as the displacement
of the core increases. Moreover, we notice that for
thinner metallic shells (smaller difference between
the outer and inner radii), the maximum change
in the resonance wavelength as compared to a
nanoshell (0 core displacement) is more than that
for particles with a thinner shell. The maximum
change in resonance wavelength corresponds to a
displacement equal to the difference between the
inner and outer radii. Finally, the change in the
resonance wavelength between the nanoeggs with
different shell thickness is due to the fact that the
resonance wavelength depends on the aspect ratio of
the particle. Nanoeggs and nanoshells have two resonance wavelengths corresponding to the symmetric
(lower energy) and antisymmetric (higher energy)
modes as discussed in [4], [78]. However, the lower
energy modes for small nanoshells dominates the
higher one and so the field enhancement shows
only one peak as seen in the blue solid lines in all
panels of figure (1). The higher energy modes for
nanoeggs, on the other hand, can produce significant
field enhancements relative to the lower energy
modes, even for small nanoeggs. This can be seen
in panel (c) of figure (1) where two peaks in the
field enhancement are shown for nanoeggs with a
non-zero core displacement (green dashed lines and
red xs). The field enhancement at both resonance
wavelengths increase as the core displacement increases, but the higher energy resonance mode is not
significant for nanoeggs with smaller aspect ratios
(panels (a) and (b) in figure (1)).
IV. C ONCLUSION

1400

Wavelength (nm)

Asymmetrical nanoparticles offer to play an important role in many applications involving resonatFig. 1. Field enhancement for a nanoegg with an outer radius of ing particles such as sensing due to the added de20nm and inner radius of (a) 13nm, (b) 16nm, and (c) 19nm, and for
different core displacements. The enhancement is at the point with grees of freedom resulting from symmetry braking.
angle 0 on the surface of the nanoegg
Insuring the best performance of such nanoparticles with added tunability requires efficient design
methodologies for nanoparticle based sensors and
field enhancement as a function of the displacement systems, which in turn requires efficient modeling
of the dielectric core and the aspect ratio (ratio of techniques. In this paper we presented an analytical
the core radius to shell radius). The nanoegg we formulation, which is efficient and accurate, for
used consists of a gold shell and a silica core. Figure nanoeggs in the quasistatic regime. The formulation
(1) shows the field enhancement for a nanoegg with is based on solving Laplaces equation in spherical
269

coordinates utilizing translation theorems of spherical harmonics. The translation theorems are key to
achieve simple and analytically solvable formulation
for the potential function. We demonstrated how
our formulation can be used to study the resonant
properties of nanoeggs.
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