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Original Title: A Second Order Approximation for the Quasistatic Properties of a Nanoegg

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FrA1-1.4

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

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

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)

2

m

2

+Aout

1 r1 cos1 + A2 r1 3(3cos1 1)

d = B1d r2 cos2 + B2d r22 cos(3cos22 1)

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)

(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)

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

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

(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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