Fundamental limits to local density of states in

absorptive system
by

Wenjie Yao
B.S., Peking University (2016)

Submitted to the Department of Electrical Engineering and Computer

Science
in partial fulfillment of the requirements for the degree of

Master of Science in Computer Science and Engineering

at the

MASSACHUSETTS INSTITUTE OF TECHNOLOGY

Feburary 2020

@ Massachusetts Institute of Technology 2020. All rights reserved.

Signature redacted
A uthor ................. ..........
Department of Electrical Engineering and Computer Science
/ IJanuary 16, 2020

Certified by.... Signature redacted..........

Steven G. Johnson
P fessor of Applied Mathematics and Physics
Thesis Supervisor

Signature redacted
A ccepted b . .....................
Leslie A. Kolodziejski
-Professor of Electrical Engineering and Computer Science
AR 13M Chair, Department Committee on Graduate Students
unnan::n To
2.......... .. ..... ..
..
 Fundamental limits to local density of states in absorptive
system
by

Wenjie Yao

Submitted to the Department of Electrical Engineering and Computer Science

on January 16, 2020, in partial fulfillment of the
requirements for the degree of
Master of Science in Computer Science and Engineering

Abstract
Fundamental limits to optical responses such as absorption, scattering and local den-
sity of states (LDOS) are proposed given intrinsic material losses by Owen, etc. The
absorption and scattering limits are validated in Owen's work while the LDOS of com-
mon structures fall short of the limits. To validate those theoretical limits in LDOS,
comprehensive studies are conducted in the metallic cavity structures, as typical res-
onant cavities will produce high LDOS. A novel shape optimization method based
on the adjoint method is presented in this work, several numerical methods (BEM,
CGAL, etc.) and optimization methods are implemented to enable more efficient
evaluation and reduce the computation costs.

Thesis Supervisor: Steven G. Johnson

Title: Professor of Applied Mathematics and Physics

3
4
Acknowledgments
The author thanks Mohammed Benzaouia and Owen Miller for insightful discussions.

5
 .....
6.... ......
Contents

1 Local Density of States and Limit 15

1.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
1.2 LDOS Expression . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
1.3 LD O S Lim it . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18

2 Optimization Methods 21
2.1 Adjoint Method and Shape Representation . . . . . . . . . . . . . . . 21
2.1.1 Introduction to Adjoint Method . . . . . . . . . . . . . . . . . 21
2.1.2 Adjoint Methods in LDOS Problem . . . . . . . . . . . . . . . 23
2.1.3 Shape Representation . . . . . . . . . . . . . . . . . . . . . . . 24
2.2 Stochastic Optimization Algorithm . . . . . . . . . . . . . . . . . . . 26

3 Numerical Methods 29
3.1 Electromagnetic Scattering Problem Solver . . . . . . . . . . . . . . . 29
3.1.1 Introduction to SCUFF-EM . . . . . . . . . . . . . . . . . . . 29
3.1.2 SCUFF-EM Validation-Mie Scattering . . . . . . . . . . . . . 31
3.1.3 SCUFF-EM Validation-Half Space LDOS . . . . . . . . . . . . 34
3.2 Geometry Mesh Generator . . . . . . . . . . . . . . . . . . . . . . . . 40
3.2.1 Introduction to GMSH and CGAL . . . . . . . . . . . . . . . 40
3.2.2 Level-set Function Geometry Presentation . . . . . . . . . . . 41
3.2.3 Custom Surface Mesh Generation . . . . . . . . . . . . . . . . 42

4 Results and Analysis 43

7
 4.1 Total LDOS Against Limit . . . . . . . . . . . . . . . . . . . . . . . . 43
4.1.1 Simple Geometries . . . . . . . . . . . . . . . . . . . . . . . . 44
4.1.2 Spherical Harmonics . . . . . . . . . . . . . . . . . . . . . . . 48
4.1.3 Resonant Sphere . . . . . . . . . . . . . . . . . . . . . . . . . 50
4.2 Polarized LDOS Against Limit . . . . . . . . . . . . . . . . . . . . . . 51
4.3 Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 53

A Custom Surface Mesh Criterion 55

8
List of Figures

3-1 Typical mesh file for sphere scattering problem. Characteristic length
lc = a /3 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32

3-2 Absorption and scattering cross-section per volume for gold sphere of
radius a = 200 nm (left) and dielectric sphere of radius a = 100 nm
(right). The absorbed and scattered cross-sections are denoted by blue
and red. The numerical results are depicted in dots and the Mie theory
results are depicted in lines. . . . . . . . . . . . . . . . . . . . . . . . 33

3-3 Relative deviation from the Mie theory for the scattering cross-section
per volume for dielectric sphere of radius a = 100 nm as a function of
N. The characteristic length is set to 1c = a/N. . . . . . . . . . . . . 33

3-4 Total LDOS above an Aluminum half space at different distance z as

a function of frequency w (In unit of w x 1014 rad/s). The numerical
results are depicted by dots and the analytical results are depicted by
lines. Different color denotes different emitter-metal separation z. . . 37

3-5 Total LDOS above an Aluminum half space at distance z = 1 nm as

a function of frequency w (In unit of w x 1014 rad/s). The numerical
results are depicted by dots and the analytical results are depicted by
lin es. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38

3-6 Electric and magnetic LDOS above a Aluminum half space at distance
z = 10 nm as a function of frequency w (In unit of w x 1014 rad/s).
The numerical results are depicted by dots and the analytical results
are depicted by lines. . . . . . . . . . . . . . . . . . . . . . . . . . . 39

9
4-1 Illustration of the simple geometry cavities. (a) Ellipsoid with tuning
parameter r1 = r 2 and fixing r3 = d, (b) Cuboid with tuning parame-

ters a = b and fixing c = d (c) Cylinder with tuning parameter r and

fixing h = d . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 43

4-2 LDOS optimization over three kinds of geometry in a silver cavity.

(a) Optimized LDOS for ellipsoid (blue line), cuboid (orange line) and
cylinder (green line) as a function of the wavelength against the the-
oretic limit (black line) at the minimum separation distance d = 10
nm. The inset shows the zoomed snapshot of the LDOS between 500

nm and 900 nm. (b) +Z and (c) +X view of the optimized cuboid at
the wavelength of 700 nm. (d) +Z and (e) +X view of the optimized
cylinder at the wavelength of 700 nm. . . . . . . . . . . . . . . . . . 44

4-3 LDOS optimization over three kinds of geometry in a silver cavity.

(a) Optimized LDOS for ellipsoid (blue line), cuboid (orange line) and
cylinder (green line) as a function of the wavelength against the theo-

retic limit (black line) at the minimum separation distance d = 50 nm.

(b) +Z and (c) +X view of the optimized cuboid at the wavelength
of 700 nm. (d) +Z and (e) +X view of the optimized cylinder at the
wavelength of 700 nm . . . . . . . . . . . . . . . . . . . . . . . . . . . 47

4-4 Optimized structure using spherical harmonics as base functions. The

wavelength and the separation distance are A = 500nm and d = 50

nm respectively. (a) +X, (b) +Y and (c) +Z view of the optimized

structure. ................................. .49

4-5 LDOS of the resonant sphere as a function of the wavelength. The

limit is calculated by setting the minimum separtion distance to be

the resonance radius ares. . . . . . . . . . . . . . . . . . . . . . . . . 50

10
4-6 LDOS optimization using polynomials in a silver cavity. Optimized
LDOS for polynomials (blue line) as a function of the wavelength
against the theoretic limit (black line) at the minimum separation dis-
tance (a) d = 10 nm and (b) d = 50 nm. (c) +Z and +X view of the
optimized geometry at the wavelength of 700 nm and d = 10 nm. (d)
+Z and +X view of the optimized geometry at the wavelength of 700
nm and d = 50 nm . . . . . . . . . . . . . . . . . . . . . . . . . . . . 52

11
12
List of Tables

2.1 Adam algorithm .............................. 27

4.1 /, factors for the three different geometry optimization at the minimum
separation d = 10 nm, the wavelength ranges from 400 nm to 900 nm. 45
4.2 K factors for the three different geometry optimization at the minimum
separation d = 50 nm, the wavelength ranges from 400 nm to 900 nm. 47

13
14
Chapter 1

Local Density of States and Limit

1.1 Introduction

The local density of states (LDOS) is a physical quantity that represents the density
of modes wighted by the relative energy density of each mode's electromagnetic field
at a given position [1]. Many macroscopic quantities can be derived from the LDOS,
a well-known example of a macroscopic quantity that follows immediately from the
knowledge of LDOS is the Casimir force [2, 3]. Other quantities such as shear force [4]
and heat transfer between two semi-infinite dielectrics [5] also relies on LDOS. How-
ever, most physical phenomena are related to electric dipole sources, the electric-field
LDOS is then the quantity which is usually calculated and considered to be the true
LDOS 16]. The (electric) LDOS is of fundamental interest for the understanding and
control of light-matter interaction in structured environments [7]-[9]. For example,
the spontaneous emission rate of atoms (key to fluorescence and lasing phenomena) is
proportional to the LDOS [10]-[12], and enhancement of the LDOS by a microcavity
is known as a Purcell effect [13]. A similar enhancement also occurs for nonlinear
optical effects [14].
In applications, metals have been extensively used for light-matter interaction be-
cause of its capability of confining light into sub-wavelength scales [15]-117]. However,
the optical response is limited by the metal losses [19]-[24]. Knowing the limits to
absorption, scattering and local density of states (LDOS) is of great importance for

15
the interaction optimization problem, otherwise one might continue to search for a
limit that can't be theoretically approached. In Ref. [18], fundamental limits to these
optical responses are proposed given intrinsic material losses. Unlike the bounds pro-
posed by other works [19]-[31], the limits in Ref. [18] do not depend on shape, size, or
topology, nor do they diverge for zero bandwidth. Given a material of susceptibility
X(w), the limits only depends on a material enhancement factor Ix(w)| 2 /ImX(w) and
on the incident-beam energy density (leading to a potential 1/d3 LDOS enhancement
for a metal-emitter separation d). This is a very simple but general limit that can
give us the physical insights.

In Ref. [18], examples of structures that approach the proposed absorption and
scattering limits at any frequency are provided, whereas common "antenna" structures
fall far short of the radiative LDOS bounds, suggesting the possibility for significant
further improvement. Because common structure is typically in the near field of the
emitter, it is difficult to design a resonant mode that exactly matches the rapidly
varying field profile of the emitter. One workaround will then be designing "cavity-
like" structures where resonances are much easier to achieve. Our work will focus
on optimizing structures to get highest LDOS possible and then compare to the
theoretical limits proposed in Ref. [18]

1.2 LDOS Expression

To start with, the local density of states (LDOS) is proportional to the imaginary
party of the dyadic green's function [61:

W
p(X0, w) = 2 ImTr[GEP(X0, X0, w) + GHM(X0, X0,W)

In many actual applications, only the electric responses are used and thus only
the electric part of the LDOS need to be considered [1]. We also focus on the electric
LDOS which comes from the electric part of the green's function GEP(X0, X0, W), it

16
can be expressed as

Pe (Xo, w) = 2 mTr[GEP(Xo, Xo, W) (1.2)

For simplicity, we will replace pc with p in the following context unless specified,
that is to say, all LDOS we will be discussing in the following is the electric part of
the LDOS.

The dyadic green's function can't be numerically computed directly, but it is

related to the electric field whose value could be obtained from numerical simulation.
The electric field E(xo, w) can be expressed by the green's function[6]:

E(xo, w) = ipow GEP(Xo, X, w) •j(x)dx. (13)

In the time harmonic case with only electric dipole at x 0 as the source, we have
3 (x _ xo), inserting this into Eq. (1.3) we hava
j(xo) = p(x=) -iWP6

W2
E(xo, w) = 2 GEP (Xo, Xo, w) . P. (1.4)
cC

Compare to the LDOS expression Eq. (1.2), we have

P(xo) = c 0 1 Im 8 (xo),
! - Es (1.5)

where Es, denotes the field from a dipole source at x0 polarized in the sj direction,
with an unit dipole moment Po = sj (thus |Po =- 1), and the sum over j accounts
for all possible orientations. This is a small modification to Eq. (8) in Owen's paper
[18], where we make the electric dipole to be unit dipole and the coefficient 60 to the
front.

Equation (1.5) will be the key expression we will be using to compute the LDOS
numerically. From the expression itself, we can see that by performing the scattered
electric field evaluation of three unit dipole excitation, the LDOS can be obtained
numerically. The remaining problem is how to calculate the scattered field from a

17
dipole excitation, which will be discussed in Chap. 2.

1.3 LDOS Limit

In Owen's paper, the total LDOS and the nonradiative LDOS can be expressed as[18]:

Ptot 27F16
ImEIV Finc,j -F 83 ,
(1.6)
P = 1+
P = 1+ 2ImEj F*, Fs. (1.7)
P0 k3 yVS

where po = w 2/2r 2 c3 is the free-space electric LDOS [32], k is the wave vector, X is
the susceptibility and F is a quantity defined as

E
F 4(). (1.8)
(ZoH)

According to Eqs. (1.6) and (1.7), the total LDOS is a linear function to the
scattered field response while the nonradiative part of the LDOS is a square function
to the scattered field response. Therefore, there must be a limit to the scattered field
response under the energy conservation constraint, which will then lead to a limit on
the LDOS. That is the key idea in Owen's paper: a linear function in the extinction
and a square function in the absorption will yield finite optimal polarization currents
and fields.

The optimal fields are obtained when the variational derivative to the quantity F
reaches zero, this gives us the limit on LDOS

Pt ; 1 + 2 ic,sj - X t(Imi) --l Xpi*,,, d3. (1.9)

Common metals (a material is said to behave as a "metal" if Rex(w) < -1 at a

given frequency w[18]) have homogeneous, isotropic, and nonmagnetic susceptibilities

18
at optical frequencies, which simplifies the susceptibility part in Eq. (1.9) as

ImX(w) (1.10)

and the integral over field can be evaluated as

ZJ c,,2 j |GEP (2

where | - ||F denotes the Frobenius norm [33].

Applying these two simplifications to Eq. (1.9) results

Ptot < 1+ 27 1x(w)| 2 [ GEpd 3 X (1.12)

Po ka Imx(w) JV

k1+ 2 [[(w)1 + + 1 ]d 3 x. (1.13)

47 Imy(w) IV (kr)6 (kr)4 kr)

Apparently, the limit of LDOS is dependent on the scattering geometry. To get a

universal limit, we need to force a minimum separation distance between the dipole
and the metal surface and determine the type of surface (an open surface or a closed
surface). In this work, we want to focus on the cavity-like surface as it yields higher
LDOS than an open surface. For a enclosure of minimum separation distance d, the
integral can be calculated as

< 1+ [
I-- +)+O(kL)]. (1.14)
Po - Imx(w) (kd)3 kd

As discussed in Owen's paper, the O(kL) term represents the largest interaction
distances over which polarization currents contribute to the LDOS. For small d, we
can neglect this term since 1 is the dominant term and is much larger than other
terms. This will lead to the final expression for the limit of LDOS

Ptot <1 + (w)1 2 1 1

Po Imx(w) (kd) 3 kd

Equation (1.15) is the central expression throughout our work, all simulation

19
results will be compared to the theoretical limit obtained with Eq. (1.15). One
thing to be noted is that for kd < 1 , the first two terms are smaller than 1 in Eq.
(1.14), then the O(kL) might play an important role to the limit. Another notice is
that this limit is about 8 times larger than the limit obtained in Owen's work (see
Eq. (34a) and (34b) in Ref. [18]), this comes from the different integration methods
used to calculate Eq. (1.13). These effects will be discussed in Chap. 4, and we will
leave it here for now.

20
Chapter 2

Optimization Methods

To find the largest LDOS given a minimum emitter-surface separation distance, two
factors are crucial, one is the information on the derivative and the other is the
optimization algorithm. In this chapter, we are going to explore the adjoint method
which is used to obtain the derivative and the Adam algorithm which is used for
stochastic optimization.

2.1 Adjoint Method and Shape Representation

2.1.1 Introduction to Adjoint Method

Adjoint method (also called adjoint state methods, adjoint model) is a numeri-
cal method for efficiently computing the derivative of function in an optimization
problem[34]-[38]. We will briefly review the key ideas in adjoint method in the fol-
lowing.

For a general optimization problem, we want to optimize an objective function

F(p, x) which depends on some design parameters p and a solution x to some equation
#(x, p) = 0 that depends on the design parameters p. For example, in the LDOS
optimization problem, x is the solution to the Maxwell's function, p is the geometry
control parameters and F is the LDOS at a given point. Therefore, the derivative we

21
want is
d- - F O= aF ±
+ aF
F ax . (2.1)
dp Op Ox Op

Generally, the objective function F is given, so it is easy to compute the partial

derivative OF/Op and OF/Ox. The complicated part is the partial derivative of the
solution Ox/Op. Traditionally, when we want a partial derivative to a parameter pi,
we need to change the parameter in a small amount 6pi and then re-evaluate the new
solution given the updated parameters. This is really time-costing especially when
the number of design parameters are large. The adjoint method, however, provides
a way to obtain all derivatives in only one more equation solving. To see how this
work, first we implement differentiation on the equation #(x, p) = 0 which yields

Oq#8x 0q (.2
+ = 0. (2.2)
axOP Op

Thus we have
Ox -( )O (2.3)
Op Ox Op

Inserting Eq. (2.3) into Eq. (2.1) we have

dF OF OF (#00)_lo#
dp -9p axOx Op
= F [F (o) 1] . (2.4)
Op ax ax ap

If we define the quantity of the bracket in Eq. (2.4) as A, then it can be obtained
by solving the adjoint equation

(2.5)
Ox A
(O90)T (F)T.
Ox

And finally we have

dF _ F 0q#
d - - A (2.6)
dp ap Op
Therefore, by only solving one adjoint problem Eq. (2.5) with a complexity similar
to the original problem solving #(x, p) = 0, we can obtain all parameter derivatives.

22
2.1.2 Adjoint Methods in LDOS Problem

In a general photonic design problem, the objective function is usually a function of

the electric E and magnetic H field, however, since the electric and magnetic fields are
both complex fields, the implementation of the adjoint method need to be carefully
treated. We will not present the detailed derivation here since it's already done by
others[39], the results will be directly used but a brief explanation will be provided.

From Ref. [39], the variation of F can be expressed as

F = 2Re fPind(x') - EA (x)d 3xI, (2.7)

where pind is the induced polarization which is proportional to E and EA is the ad-
joint field which is the solution of the same problem (same geometry) with a different
source (Of/oE, -(1/po)Of/OH).

To understand Eq. (2.7), first we start with Eq. (2.6). Since F(E, H) is only
a function of the fields, the partial derivative to the parameters OF/Op is then 0.
The solution x is the electric and magnetic fields and the constraint problem is the
Maxwell's equation
A(p)x = b, (2.8)

where A(p) is the operator of the Maxwell's function and b represents the source term.
Therefore, 0#/Ox = A(p) and the adjoint equation (2.5) becomes (the operator of
the Maxwell's equation is symmetric A(p)T = A(p))

A(p)A =( )T. (2.9)

It's now clear that A is exactly the adjoint field EA in Eq. (2.7). The second part
oq#/Op can be expressed as
=OA(p) x
_ (2.10)
Op a
which is proportional to the field, so it represents the induced polarization part pind

in Eq. (2.7).

23
 Suppose we have a surface b that separates two material ei and 62, the variation for
the object function F caused by a shape deformation 3Rs(x') in the normal direction
is then[39]

6F = 2Re j 6R,(x')[(e2-
(6 -1
E1)Eil (x') - E(x') + ()D-L(- DA(x')]dS (2.11)
12

(
Since the LDOS p is the imaginary part of some function, say p:

p _ =2i-ImQp) =m[ s-Esj (xo)]. (2.12)

7ro
3

For each direction j, the source of the adjoint field is then a electric dipole at xO with
the amplitude

p pp(x - xo)S- (2.13)

E5 O,8 Es, 217rw

while the conjugate adjoint field part -5 = 0.

This is a also a dipole at x = xO in the 9j direction, so the adjoint field is the

same as the original field up to a constant scalar:

60 Es
EA (x) = 2i27ro (2.14)

Inserting Eq. (2.14) to Eq. (2.11), we then have the variation for LDOS as

Jp = 601M JR, 6R(x'){( 2 - c1)[E, II(x')]2 + (- I )[D_ 1(x')] 2}dS (2.15)

2.1.3 Shape Representation

With Eq. (2.15) obtained, there's only one thing left to get the derivative of the
desired parameters, which is the shape representation R(p), in another words, how
to present the shape using the parameters. For simple geometries such as sphere,
ellipsoid, or cubic, it is easy to describe the shape using the corresponding character-
istic parameters. However, if we want an arbitrary shape in 3D, it would be best to

24
expand the shape in a set of spherical harmonic bases.

Since a minimum separation distance d is required during optimization (otherwise

LDOS will always goes to infinite as d goes to zero), the following shape function is
used for spherical harmonic optimization.

N
R(O, #) d+ p #2 (2.16)
n=O

where d is the minimum distance and pn(n = 0, 1, 2, --- ) is the expansion coefficients
and the parameters that we need to optimize. The real spherical harmonic function
Yn(0, #) is defined as

Y (0,) =
f 21(m)(pm(OS 0) cos(m#),
4r 1M) 1
m < 0
(2.17)
211 (1-m)! P" (cos 0) sin(m#$), m > 0

and the subscript n = 1(1 + 1) + m.

Note that for any shape function, the normal direction at a certain position can
be expressed as
n(1AfR 1 &R
n = (11 R o80 .R (2.18)
R sin 0 (9#

The normal deformation 6Rn for a spherical harmonics based shape with respect
to pn is then
6Rn 2[En pn Yn (0, #)Yn (0, #) -J 2.19)
1 ( )2 + (asin
)

Finally, combing Eq. (2.19) and (2.15) can give us the LDOS derivative with
respect to the desired parameters.

In some case which will be discussed in Chap. 4, we would want a shape repre-
sentation that is rotational symmetric, the function we will be using is

d + [En Pn (L')n]2, 0 < E

R(0, [ r) (2.20)
d + [1ZnPn(2 - 20)n] 2, Q > 7r

25
 Similarly, the normal deformation with respect to p, can be expressed as

2(E( (
V+(1 1
{)" (0)
)2
2
Pn»I
<.1
- 2

S+ Rn0,$)=R n 6N 20 n

2.2 Stochastic Optimization Algorithm

In the numerical optimization for LDOS, the accuracy of the obtained LDOS from
numerical evaluation depends on the mesh resolution of the surface. As a matter of
fact, the derivative of the LDOS is evaluated by numerical integral over the scattered
fields which are also numerical results. Therefore, the noise in the derivative of the
LDOS is even larger than the LDOS. To overcome the noisy objective function as
well as its derivative, efficient stochastic optimization techniques are required.

The stochastic optimization method we have implemented in our work is the Adam
algorithm. Adam, which stands for adaptive moment estimation, is an algorithm
for first-order gradient-based optimization of stochastic objective functions, based
on adaptive estimates of lower-order moments[40]. The pseduo-code of the Adam
algorithm is provided in Tab. 2.1. It finds the local minimum of the objective function
f(0), in the case of LDOS, the objective function is set to be -p. Some of Adam's
advantages are that the magnitudes of parameter updates are invariant to rescaling of
the gradient, its stepsizes are approximately bounded by the stepsize hyperparameter,
it does not require a stationary objective, it works with sparse gradients, and it
naturally performs a form of step size annealing.

26
 Table 2.1: Adam algorithm

Algorithm: gt indicates the element-wise square gt 0 gt. Good default settings

for the tested machine learning problems are a = 0.001, #1 = 0.9, 02 = 0.999 and
E =10-. All operations on vectors are element-wise. With #t and #t we denote #1
and #2 to the power t.
Require: a: Stepsize
Require: #1,#82 c [0, 1): Exponential decay rates for the moment estimates
Require: f(0): Stochastic objective function with parameters 0
Require: 0: Initial parameter vector
mo +- 0 (Initialize first moment vector)

vo <- 0 (Initialize second moment vector)

t +- 0 (Initialize timestep)
while Ot not converged do
t +- t+ 1
gt +- Voft(t_ 1 ) (Get gradients w.r.t. stochastic objective at timestep t)
mt <- #1 - mt1 + (1 - 31) - gt (Update biased first moment estimate)
Vt +- 32 - Vt1 + (1 - /2) - g2 (Update biased second raw moment estimate)
6Ilt <- mt/(1 - #3) (Compute bias-corrected first moment estimate)
ft+- vt/(1 - /3) (Compute bias-corrected second raw moment estimate)
Ot +- ,t - rnt/(v't+ 6) (Update parameters)
end while
return Ot (Resulting parameters)

27
28
Chapter 3

Numerical Methods

3.1 Electromagnetic Scattering Problem Solver

According to Eq. (1.5), the LDOS problem is basically three dipole scattering prob-
lem. Therefore, to get the LDOS at a specified point, we need an electromagnetic
scattering problem solver that can evaluate the scattered fields. For a surface scat-
tering problem, boundary-element method (BEM) based solvers are far more efficient
than finite-element method (FEM) or finite-difference frequency-domain (FDFD), as
the scattering problem only requires the surface information [41]. In this work, we
will be using a new BEM based open-source software SCUFF-EM to compute the
scattering problem.

3.1.1 Introduction to SCUFF-EM

SCUFF-EM, which stands for Surface Current/Field Formulation of ElectroMag-

netism, is a free, open-source software implementation of the BEM (or the "method of
moments") of electromagnetic scattering[42]. (More specifically, SCUFF-EM imple-
ments the EFIE and PMCHWT formulations of the BEM using RWG basis functions.)
Here is rough idea about what SCUFF-EM solver does: for a collection of ho-
mogeneous material objects (maybe gold or silicon spheres or cubes) embedded in
some medium (generally vacuum or a dielectric liquid), the solver irradiate the con-

29
figuration with some known electromagnetic disturbance (such as a plane wave), and
then seek to compute the electromagnetic fields scattered from the objects. In a
surface-integral-equation (SIE) method, the solver first computsthe surface currents
induced on the object surfaces by the incident field. (For perfectly conducting scat-
terers there's only electric surface currents (K); for general scatterers there are both
electric (K) and magnetic (N) surface currents.) Once the surface currents are solved,
they can be used to evaluate the scattered fields anywhere.

What we will be using throughout our simulation is the core library libscuff,
it stores the scattered fields as well as some key information on the surface, such as
electric and magnetic surface charges and currents, whose value can then be used to
compute the fields on surface by

o = n-D, (3.1)

K = nxH, (3.2)

r1 = n-B, (3.3)

N = nxE. (3.4)

For example, the parallel electrical field and perpendicular displacement can be
computed as

Eli = N, (3.5)

Di = -n. (3.6)

To check the validity of SCUFF-EM, we implement the numerical evaluations on

two benchmark problems: Mie scattering and LDOS of a half space. All relative
electric permittivities are obtained using interpolations from the data in Ref. [43]
throughout all numerical evaluations.

30
3.1.2 SCUFF-EM Validation-Mie Scattering

According to Mie theory [44], the scattering, absorption, and extinction cross-sections
can all be expressed in terms of the an and bn coefficients,

27r 00

-e = - (2n + 1)Re(an + bn), (3.7)

n=1

- (2n + 1)( an| 2 + b|2 ), (3.8)

n=1

O-a e - Us-. (3.9)

The coefficients an and bn can be computed as

an b(ma)2bn(a) - mrn~(na)'(a) (3.10)

_ (ma)4((a) - mn(m)('(a) ('3.1
bn = ~n(OO(e -O(a n( (3.11)
m' (ma)(n(a) - $n(ma)('(a)

where a = ka = 27ra/A is called the size parameter, m is the index of refraction, a is

the particle radii, and @ and ri are related to spherical Bessel functions. They are
characteristic of spherical geometry and arise when solving the wave equation. The
prime indicates the first derivative with respect to r.

We implement SCUFF-EM on two cases: solid gold sphere with radius a = 200
nm and solid dielectric sphere with relative electric permittivity e = 12 and radius
a = 100 nm. To perform the numerical evaluation, we first need to create a mesh
file using GMSH (details will be discussed in the following section). The mesh size
is determined by the characteristic length 1c per physical point in GMSH. For the
sphere geometry, we can simply set all points' characteristic lengths to be 1c = a/3,
where the radius a is of unit pm which is 0.2 for gold sphere and 0.1 for dielectric
sphere. A typical mesh file is shown in Fig. 3-1.

31
Figure 3-1: Typical mesh file for sphere scattering problem. Characteristic length
1c = a/3

The absorbed (Pa) and scattered power (P,) can be obtained from SCUFF-EM
outputs. Plane waves are incident fields of general interests, the cross-section is
defined as the ratio of the power and incident electric or magnetic intensities (Plane
waves have equal electric and magnetic energy densities and constant intensities):

P 1
o-= , inc = cUE,inc = 1ocEin 2 . (3.12)
linc 2

Therefore, the absorbed and scattered cross-section per volume can then be com-
puted as:

o-' 3Zo
V
V = 27ra3|Eo|12
2aIo1P a, (3.13)
-' 3Zo
3
V = o P. (3.14)
V 27ra3|Eol2

where Zo = 377Q is the vacuum impedance and Eo is the incident electric field
amplitude specified in the inputs.

32
 Gold Sphere of radius 200ran Constant e=12 Sphere of radius 100nm
0.014
• Scattered
0.012 0.008. - Absorbed Mie
- Scattered Me
0.010-
0.006

-
0.008- •Absorbed
- Scattered
-Absorbed Me 0.004
0.006- ---Scattered Mie

-
0.004-
0.002-
0.002
-

0.000- 0.000

-
400 500 600 700 800 900 1000 1100 1200 400 500 600 700 300 900 10 1100 1200
Nnm) Xnm)

Figure 3-2: Absorption and scattering cross-section per volume for gold sphere of
radius a = 200 nm (left) and dielectric sphere of radius a = 100 nm (right). The
absorbed and scattered cross-sections are denoted by blue and red. The numerical
results are depicted in dots and the Mie theory results are depicted in lines.

- Scattered
12-

10-

iF
4

4-

0-
2 4 6 8 10
N

Figure 3-3: Relative deviation from the Mie theory for the scattering cross-section
per volume for dielectric sphere of radius a = 100 nm as a function of N. The
characteristic length is set to ic = a/N.

The numerical results of SCUFF-EM for the gold and dielectric sphere are shown in
Fig. 3-2. For the gold sphere, the absorbed and scattered cross-section from SCUFF-
EM results match very well with the Mie theory results with a little deviation. For the

33
dielectric sphere, the absorbed cross-section is theoretically zero since we assumed a
lossless material, the SCUFF-EM also gives zero absorbed power. The scattered cross-
section, however, deviates a little from the Mie theory. In fact, these discrepancies
mainly comes from the resolution. We performed the same calculation using different
characteristic lengths at A = 600 nm for the dielectric sphere, the relative deviation
as a function of characteristic lengths are shown in Fig. 3-3.

The characteristic lengths vary from ic = a to 1c = a/10, we can see from Fig. 3-3
that the SCUFF-EM result does converge to the Mie theory. For N > 6, the relative
difference Ao/a is smaller than 1%. However, finer meshes cost more memory and
time. The used memory goes up to 2 Gigabytes for N = 10 and it takes about 10
minutes to compute just one point (The CPU type is 3.5 GHz 6-Core Intel Xeon E5).
There's a tradeoff between the accuracy and the costs. Nonetheless, we can conclude
that SCUFF-EM gives valid absorbed and scattered power with enough resolution.

3.1.3 SCUFF-EM Validation-Half Space LDOS

In this part, we are going to check the accuracy of the core library libscuf f using the
built-in command-line function scuf f -idos. What scuf f -idos actually computes
is the scattering part of the dyadic Green's functions (DGFs) of the geometry in
question. For a given (angular frequency, evaluation point) pair (w, x), these are 3 x 3
matrices giving the scattered fields at x due to point sources at x, with all fields and
sources having time dependence e-iwt. The LDOS is obtained from the imaginary
part of the traces of the DGFs. Therefore, the total LDOS should be the scattering
part obtained from scuf f -idos plus the total vacuum LDOS p,.

w2
PV 3 (3.15)
723

34
The benchmark problem here is the LDOS above a half metallic (Aluminum) space,
the analytical solution for the electric and magnetic LDOS are [61

pE(Z W) PV {[ + 2 Re(r 2e
2
ipwz/c) + Re(r 2e 2i2pz/c)(2K 2 _ 1)

+ I [Im(r1 2 ) + (2K 2 - 1)Im(r 2 )]e Plwz/J (3.16)

pM 4w) P [2 + Re(r 2e 2 Poz/c) + Re(rI 2 2 xwz/c)(2K 2 _ 1)

+ [Im(rP2 ) + (22 - 1)m(r2)] 2jpiz/c(3.17)

2
where p = V/1 -K if K < 1 and p i/ - 1 if K > 1. r1 2 and r 2 are the Fresnel

reflection factors between media 1 and 2 in s and p polarizations, respectively, for a

parallel wave vector wr/c [45].

2
i-K/1 - K2 _- / K
2= 1- 2 (3.18)
s/1 ~f - K2 +/ - 2

8 EV/1 - K2 _C _K2
-/
r2 1-K 2 C-K 2 (3.19)

Aluminum is a metal whose dielectric constant is well described by a Drude model

for near-uv, visible, and near-ir frequencies:

W2 = -(3.20)
W(o +i)

with w = 1.747 x 1016 rad/s and y 7.696 x 1013 rad/s.

There's a little trick implementing the scuff -idos on the infinite half space.
In scuff -ldos, the electric and magnetic DGFs for a given source point (and any
number of destination points) collectively describe the results of 6 scattering problems

(with incident fields produced by electric and magnetic dipoles oriented in each of the
3 cartesian directions), and-for compact geometries-could be computed simply by

assembling 6 right-hand-side vectors, solving the BEM system for the corresponding

surface currents, and computing the scattered fields at all desired destination points.

However, the situation is more complicated for infinitely extended geometries.

35
Such geometries can only be described in SCUFF-EM by a unit-cell geometry together
with a basis of vectors for a (one- or two-dimensional) lattice L. By restricting our
attention to scattering problems in which the incident fields (and thus all fields and
currents) satisfies the Bloch-periodicity condition

f(x+ L) = e BJ(s), for all L C L (3.21)

for some Bloch wavevector kB, we can get away with solving only for the surface
currents within the unit cell, the currents everywhere else being then fixed by the
Bloch periodicity. This is the basic magic trick that allows infinite geometries to be
modeled on finite computers.

Of course, the restriction to scattering problems involving only Bloch-periodic

incident fields is in fact highly restrictive; indeed, it excludes the particular problem
we must solve to compute DGFs and LDOS, in which the incident field emanates
from a point source at 'S and is certainly not Bloch-periodic. But here we can avail
to the linearity of Maxwell's equations and the magic of Fourier analysis. Instead of
solving a scattering problem involving the field of a point source at Ys, we consider
the field of an infinite phased array of point sources, located at points {s + L} with
phases eik'E, for all L E L. This is a Bloch-periodic field, so we can take it as the
incident field in a SCUFF-EM scattering problem, and the resulting scattered fields
at iD define the Bloch-periodic scattering DGFs g(w; kB; XD, Xs). To recover the
non-periodic DGF g from 9, we now imagine solving and summing the results of
many scattering problems involving our infinite array of point sources phased with
many different Bloch vectors kB, chosen cleverly to ensure that the contributions of
the single point source at X's add constructively, while the contributions of all other
point sources in the array add destructively and cancel. The formal expression of this
procedure is a sort of inverse Fourier transform relating g to the average of 9(kB)
over the Brillouin zone (BZ) of the reciprocal lattice:

(w;iD,~S(w B XD, 3.22)

(s3B
JBZ
6VBZ

36
or, evaluating the integral approximately by numerical cubature,

__#;rD, S m Bm D (3.23)
VBZ

where {kBm, Wm} are the points and weights in a cubature rule for integration over
the Brillouin zone. Thus, getting the LDOS at a single point in a periodic geometry
requires summing the results of many scattering calculations at various Bloch vectors
kBm lying in the Brillouin zone of the reciprocal lattice.
In the scuff -idos computation, we first generate a square lattice with lattice
constant L = 0.01pm, the resolution is set to be 8 points per side. The Brillouin-zone
integration option is set to be -- BZIMethod Polar2 -- BZIOrder 0002. This uses
polar cubature with change of variables and selects an adaptive integration algorithm
for the radial integral, which determines the number and location of the sample points
automatically to achieve user-specified relative and absolute error tolerances. [471.

Aluminum LDOS pe+pm

101.

1010-

106-

104 - z=10nm
-- z=-1000nm
100 101 102

Figure 3-4: Total LDOS above an Aluminum half space at different distance z as
a function of frequency w (In unit of w x 1014 rad/s). The numerical results are
depicted by dots and the analytical results are depicted by lines. Different color
denotes different emitter-metal separation z.

37
 The total LDOS (pto = Pe + Pm) from scuf f -ldos are shown in Fig. 3-4 in com-
parison with the theoretical integration values. We first note that the LDOS increases
drastically when the distance to the material is reduced. At a large distance from the
material, one retrieves the vacuum density of states. Note that at a given distance,
it is always possible to find a sufficiently high frequency for which the corresponding
wavelength is small compared to the distance so that a far-field situation is retrieved.
When the distance to the material is reduced, additional modes are present: these are
the evanescent modes that are confined close to the interface and that cannot be seen
in the far field. Moreover, aluminum exhibits a resonance around w,/V2. Below this
frequency, the material supports resonant surface waves "surface-plasmon polaritons".
Additional modes are therefore seen in the near field. This produces an increase of
the LDOS close to the interface. The enhancement is particularly important at the
resonant frequency that corresponds to Re(c) = -1. Finally, Fig. 3-4 shows that it
is possible to have a LDOS smaller than that of vacuum at some particular distances
and frequencies.

Aluminum LDOS pe+pm

- z=lnm
1010

109

107

100 101 102

Figure 3-5: Total LDOS above an Aluminum half space at distance z = 1 nm as a

function of frequency w (In unit of W x 1014 rad/s). The numerical results are depicted
by dots and the analytical results are depicted by lines.

38
 The numerical results from scuff -ldos matched very well with the analytical
solution for z =10, 100 and 1000 nm, however, it deviates dramatically from the
analytical solution. The reason behind it is still the resolution. Our lattice constant
is L = 10 nm with 8 points per side, then the mesh size is around 1.2 nm. This mesh
size is too big for a distance z =1 nm and results deviation from the theory. To get a
more accurate numerical results, we need to shrink the lattice size to L = 1 nm. We
plot the modified values in Fig. 3-5. Although there's still some small deviations, it
matched already very well with the analytical solution. To increase the accuracy, we
need to further increase the resolution. Unfortunately, the computation time for Fig.
3-5 already takes about 2 days, we are not able to do a finer mesh at present, but we
will continue to check the validity in the future.

Aluminum LDOS
- pe

107.

106

105

100 101 102

Figure 3-6: Electric and magnetic LDOS above a Aluminum half space at distance
z = 10 nm as a function of frequency w (In unit of w x 10" rad/s). The numerical
results are depicted by dots and the analytical results are depicted by lines.

In application, pE is the quantity that is usually calculated and considered to be

the true LDOS. We also need to verify the validity of the electric LDOS (pe) and the
magnetic LDOS (pm). We consider the distance z = 10 nm case, the electric and
magnetic LDOS are plotted in Fig. 3-6. The numerical values match very well for
large frequencies but differs a little bit at small frequency regions. We also notice

39
that the analytical solutions have some "ripples" in some range (as well as in Fig.
3-4), this comes from the errors when we implement the numerical integration of Eq.
(3.16) and (3.17), the integration step we choose is 10-3 and the upper bound for the
infinity integration is chosen to be 104, a more accurate value requires smaller steps
and bigger upper bounds, but again, the time cost will be too large.
To conclude, SCUFF-EM gives valid results regarding scattering or LDOS calcu-
lations. Better resolution is needed for higher accuracy. There's a tradeoff between
the accuracy and the memory and time costs, user should balance between them and
carefully choose the parameters that suit the problem best.

3.2 Geometry Mesh Generator

To implement BEM, one critical thing is to create an appropriate surface mesh.
Two surface mesh generating software will be discussed in the following: CGAL and
GMSH. Both are powerful mesh generators with its own strengths.

3.2.1 Introduction to GMSH and CGAL

Gmsh is a three-dimensional finite element mesh generator with a build-in CAD

engine and post-processor. Its design goal is to provide a fast, light and user-friendly
meshing tool with parametric input and advanced visualization capabilities[49]. It's
good at quickly describing simple and/or "repetitive" geometries with the built-in
scripting language, parametrizing geometries, importing geometries from other CAD
software in standard exchange formats, generating ID, 2D and 3D simplicial (i.e.,
using line segments, triangles and tetrahedra) finite element meshes with fine control
over the element size, creating simple extruded geometries and meshes, visualizing
and export computational results in a great variety of ways.
It is so powerful and even perfect when it comes to simple geometries, but its
weak point is also very obvious: cannot generate meshes with high complexity such as
implicit function controlled shape. Therefore, we will use GMSH for simple geometries
and CGAL for complex geometries.

40
 CGAL is a software project that provides easy access to efficient and reliable
geometric algorithms in the form of a C++ library. CGAL is used in various ar-
eas needing geometric computation, such as geographic information systems, com-
puter aided design, molecular biology, medical imaging, computer graphics, and
robotics.Specifically, we will be using the 3D surface mesh generation package[50]-

[52]. This package provides a function template to compute a triangular mesh ap-
proximating a surface. The meshing algorithm requires to know the surface to be
meshed only through an oracle able to tell whether a given segment, line or ray in-
tersects the surface or not and to compute an intersection point if any. This feature
makes the package generic enough to be applied in a wide variety of situations. For
instance, it can be used to mesh implicit surfaces described as the zero level set of
some function. The meshing algorithm is based on the notion of the restricted De-
launay triangulation. Basically the algorithm computes a set of sample points on
the surface, and extract an interpolating surface mesh from the three dimensional
triangulation of these sample points. Points are iteratively added to the sample, as
in a Delaunay refinement process, until some size and shape criteria on the elements
of the surface mesh are satisfied.

3.2.2 Level-set Function Geometry Presentation

For a surface optimization problem, we need a parameterized shape that can be arbi-
trary shape. The way to do it is the implementation of level-set function methods[531-
[55]. The boundary is defined as the zero level set of a level set function D, such that
D = 0 at points on the boundary. Away from the boundary, it is numerically conve-
nient to set 4 equal to a signed distance function; that is, at every point 4 equals
the distance to the closest boundary point. Moreover, points inside the boundary are
taken to be the negative of the distance, enabling one to keep track of which material
is where.
In 3D Cartesian coordinates, a level-set function can be written as

1(x, y, z) = V/x 2 + y 2 + z 2 - R(x, y, z) (3.24)

41
where R(x, y, z) or R(r, 0, <) in spherical coordinates are the shape function of the
object.
In CGAL, we can set the implicit function to be <b = 0 to get the desired shape.

3.2.3 Custom Surface Mesh Generation

Another important thing about the mesh generation is that we want a mesh that
can have different resolution at different region. For example, we always want higher
resolution at sharp corners or edges. This is easy to achieve with GMSH since you
can assign every geometric point with a characteristic length, which will then affect
the mesh size around that point. However, things become a little bit complicated
with CGAL, especially when it comes to a level-set function defined geometry.
In level-set functions, there are no more such fixed "geometric" point, every point
might be moving, we can only assign different fixed-region with specific resolution. In
our work, we would want to focus on the region with small emitter-surface separation
d, thus we need higher resolution within a range close to d. The implementation is
achieved by creating a custom surface mesh criterion in the CGAL 3D surface mesh
generation module. A detailed code is attached in the Appendix A.

42
Chapter 4

Results and Analysis

4.1 Total LDOS Against Limit

a) b)M c)

Metal Metal

Ellipsoid Cuboid Cylinder

Figure 4-1: Illustration of the simple geometry cavities. (a) Ellipsoid with tuning
parameter r1 = r 2 and fixing r 3 = d, (b) Cuboid with tuning parameters a = b and
fixing c = d (c) Cylinder with tuning parameter r and fixing h = d
.

In this section, we are going to compare the optimized total electric LDOS given a
minimum separation distance d to the theoretical limit obtained from Eq. (1.15). We
will first start with some simple geometries and observe their performances. Then we
are going to discuss the optimized results using spherical harmonics optimization. At
certain conditions, we could have a resonant sphere resulting a large LDOS, which

43
will be discussed in the last part.

4.1.1 Simple Geometries

Optimization over three typical geometries are conducted: an ellipsoid cavity, a cuboid
cavity and a cylinder cavity, as illustrated in Fig. 4-1. Silver is selected as the metal
since its electric permittivity behaves better than other metal in the optical frequency
range[43]. The LDOS is evaluated at the center of those geometries.

a) b) C)

107

d) e)
&

Figure 4-2: LDOS optimization over three kinds of geometry in a silver cavity. (a)
Optimized LDOS for ellipsoid (blue line), cuboid (orange line) and cylinder (green
line) as a function of the wavelength against the theoretic limit (black line) at the
minimum separation distance d = 10 nm. The inset shows the zoomed snapshot of
the LDOS between 500 nm and 900 nm. (b) +Z and (c) +HX view of the optimized
cuboid at the wavelength of 700 nm. (d) ±Z and (e) +X view of the optimized
cylinder at the wavelength of 700 nm.

As discussed in Chap. 2, the limit of Eq. (1.15) is only valid for small separation
dmin, therefore we will start with the smallest separation to be d = 10 nm. In the
simulation, the minimum separation is guaranteed by setting one parameter to be
d and other parameters subject to a box constraint. For example, in the case of
ellipsoid, we set one semi-major axis ra = d and constrain the variation range of r 1

44
and r2 to be [d, 10A]. The upper bound 10A is chosen to avoid overly large parameters
sometimes caused by a large derivative, 10A is a reasonable upper bound based on our
simulation experiences. Furthermore, it is found that for different local optimum, the
more symmetric geometry yields a larger total LDOS. This can be interpreted that
the total LDOS is a sum over three dipoles orienting at three orthogonal directions, an
asymmetric geometry will result a lower LDOS for the unoptimized dipole directions.
Therefore, we can further simplify the optimization problem by applying symmetries.
For the ellipsoid, we have the tuning parameter r1 = r2 and r3 = d; for the cuboid,
the tuning parameters are a = b and c = d; for the cylinder, the minimum separation
distance is chosen as h = d as we found that "pan-cake" shape yields a larger LDOS.
The optimized LDOS as a function of the wavelength at the minimum distance
d = 10 nm for three kinds of geometries are given in Fig. 4-2(a), the wavelength
varies from 400 nm to 900 nm as a typical range for optical frequencies[43]. The
results show that the optimized LDOS is far from the limit. Among the three kinds
of geometries, the ellipsoid gives the lowest LDOS while the cuboid and cylinder share
similar LDOS at long wavelength range. From the inset of Fig. 4-2(a), however, we
could see that the cylinder gives slightly better LDOS than cuboid. To quantify the
performance of the optimization more clearly, we define a new factor K that indicates
how much the optimized LDOS is away from the limit:

K1 fAend Plimit (4.1)

Aend - Astart JXstart Poptimized

Geometry Type Ellipsoid Cuboid Cylinder

K 819 796 689

Table 4.1: K factors for the three different geometry optimization at the minimum
separation d = 10 nm, the wavelength ranges from 400 nm to 900 nm.

It is defined as the average ratio of the LDOS limit and the optimized LDOS
in the considered wavelength region, a smaller K would indicate a better optimized

45
LDOS that is approaching the limit. The factors , for the three different geometry
optimization at the minimum separation d = 10 nm are given in Tab. 4.1. The
cylinder gives a smallest r, of 689, however, this number is still too large since we
want a number close to 1 (which means the limit is actually reached). Two factors
contributes to the large K, one is the overestimate of the limit in the current case and
the other is the separation distance too small.

First, let's look at the optimized structure at the wavelength of 700 nm ( chosen
as the middle of 400 and 900, but other wavelengths also present similar features). As
displayed in Fig. 4-2(b)-(e) (cuboid and cylinder are chosen because of their higher
LDOS), the optimized structures are like "pan-cakes", so the emitter at the center is
more like in between two half-space plane rather than surrounded by metal surfaces.
This will to an overestimate of the limit of Eq. (1.15), since it is evaluated assuming
that all surrounding points are at the minimum separation distance d. In Ref. [18],
the limit to a half-space with separation d is

Po< 1 + ( + 2 (4.2)
PO- 8 Imx(w) (kd)3 kd

This is about 8 times smaller than the limited evaluated by Eq. (1.15). For two
half-space plane surrounding the emitter, the limit doubles so the actual limit of the
pan-cake shape structures should be about 4 times smaller than the current limit,
which means the factor r, should approximately divide by 4. Nevertheless, a factor of
4 can't make much difference to a number of 689. There's something intrinsic here
that prevents from getting a high LDOS, that is the ultra-small separation distance.
As we have said before, we want a closed cavity rather than a open surface because
we want to have some sort of "resonance" that enhances the LDOS. In the ultra-
small separation distance kd « 1, it's more difficult for "resonance" to occur, thus
the LDOS performance is not much different to an open surface, and the optimized
structures would be like two half-space planes which resembles more "open" surface
features.

On the other hand, the limit requires a small separation such that the O(kL) term

46
in Eq. (1.14) can be neglected. Since L represents the largest interaction distance, in
metal materials, the electromagnetic waves damp fast at optical frequencies[56], thus
the O(kL) term is about the order of 101. When kd < 0.5, we have 1/(kd) 3 +1/(kd) >
10, this means a minimum separation of d < A/47r would be already good enough.
Taking A = 700 nm gives us d < 55.7 nm, now we do another round of the same
optimization but at a different separation distance of d = 50 nm.

aI b)c)
- Elipsoid
-- Cuboid
- Cylidner
104

d) e)
102.

10' ---

-
400 500 800 700 800 "0
1nm)

Figure 4-3: LDOS optimization over three kinds of geometry in a silver cavity. (a)
Optimized LDOS for ellipsoid (blue line), cuboid (orange line) and cylinder (green
line) as a function of the wavelength against the theoretic limit (black line) at the
minimum separation distance d = 50 nm. (b) +Z and (c) +X view of the optimized
cuboid at the wavelength of 700 nm. (d) +Z and (e) +X view of the optimized
cylinder at the wavelength of 700 nm.

Geometry Type Ellipsoid Cuboid Cylinder

49 38 36

Table 4.2: K factors for the three different geometry optimization at the minimum
separation d = 50 nm, the wavelength ranges from 400 nm to 900 nm.

The behavior of the three kinds of geometry are similar to the d = 10 nm case,
see in Fig. 4-3. The cylinder still performs the best and very close to the cuboid,

47
ellipsoid performs the worst. However, those optimized LDOS are now much closer
to the limit. As shown in Tab. 4.2, the factor K drops dramatically from around 700
to around 40. Although there is still a long way to go from 40 to 1, it is already
a very big improvement, and it proves our theory and the limit should be easier to
reach at larger separation distance. This could also be understood by looking at
the optimized geometry, see in Fig. 4-3(b)-(e). The optimized structures are now
less flat compared to the previous ones, the larger separation distance enables better
"resonance". Meanwhile, since smaller A plays a similar role to larger separation, we
can see from Fig. 4-3(a) that it is closer to the limit in the short wavelength range.

4.1.2 Spherical Harmonics

The case for the spherical harmonics based geometry optimization is far more compli-
cated than the simple geometries. First, there are far more parameters to consider, so
the optimization time cost is far more expensive. For example, if we want to include 5
set of spherical harmonics (1 = 0, 1, 2, 3, 4), there will be 16 parameters, it would take
days or week to run one optimization to get a converged result. Second, the large
quantity of optimization parameters of spherical harmonics will cause too many local
optimums to occur. In our early stage of spherical harmonics optimization, we often
run into such local optimums with random initial guess, those local optimums are
not much different from the simple geometry optimums despite that we have spent
lots of time trying different initial guesses. To speed up the optimization process, we
noticed from our simulations that a symmetry usually results higher LDOS, therefore
we implement an inversion symmetry on our optimization.
For spherical harmonics, we have the parity property

Y'(-r) = (-1)1Y'(r). (4.3)

For spherical harmonics with even or odd 1, they share same parity. Therefore,
we can optimize the spherical harmonics using two set of function bases, one is even
1 (0, 2, 4, - --) and the other is odd 1 (1, 3, 5, -- -). Consider the number of parameters

48
to be optimized, we chose one set to be l=(0,2,4) and the other one l=(1,3). The
wavelength and the separation distance are chosen to be A = 500nm and d = 50 nm
respectively. The best LDOS we get is p/po = 89.3, which is only about 7 times
smaller than the theoretic limit Plimit/po = 675. Compared with the cylinder results
of p/po = 52, the performance is about 1.7 times better. In general, this number
if about 1.5 for all optimized geometries we found. The corresponding optimized
geometry at 700 nm is shown in Fig. 4-4.

a) b) C)

Figure 4-4: Optimized structure using spherical harmonics as base functions. The
wavelength and the separation distance are A = 500nm and d = 50 nm respectively.
(a) +X, (b) +Y and (c) +Z view of the optimized structure.

For the LDOS in the optimized structure, it is found that the polarized LDOS
components (the LDOS of one dipole excitation) are p., py, p, = (44.8, 0.2, 4 4 .3 )po,

this result actually illuminates a way of optimization. As shown in Fig. 4-4, the
structure has a C3 symmetry in the x - z plane, which results the x and z polarized
LDOS are almost identical. This indicates that more symmetry yields higher LDOS
which is consistent with other simulation results. Besides, the separation distance in
the x and z axises are d while the separation distance in y direction is much larger,
this means that to get a higher LDOS in one direction, the separation distance in
that direction must be the minimum separation distance d.

49
4.1.3 Resonant Sphere

To obtain the largest total LDOS, we need the three polarized LDOS to be identical,
which means the shape function must be mutation invariant to x, y and z. Besides,
the separation distance on each axis must also be the minimum separation distance d.
The most simple geometry that meets all those requirements is the sphere. However,
the resonance can only be achieved at certain combinations of d and A[57]-[58].
For a void sphere, the electromagnetic surface modes satisfy:

Cm(E)H(kma)[kdaJ(kda)]' = cAJ(kda)[kmaHi(kma)]' (4.4)

where a corresponds to the void radius, 1 is the (integer) index denoting the angular
momentum, km = Vk and kd =/ik are wave vectors in metal and void. J and

H are spherical Bessel and Hankel functions of the first kind. Since the excitation
source in the LDOS problem is a dipole, only 1 = 1 mode will be excited. Therefore
for each wavelength, there's only one resonant sphere with radius d = are,.

- Umit
- Resonant Sphere

102.
&a

400 500 60 700 80 90

A(nm)

Figure 4-5: LDOS of the resonant sphere as a function of the wavelength. The limit
is calculated by setting the minimum separtion distance to be the resonance radius
ares.

50
 Using Eq. (4.4), we can directly computes the resonance radius ares and then
evaluates the corresponding LDOS, the results are shown in Fig. 4-5. We can see
that the LDOS of the resonant sphere is very close to the theoretical limit, with a
average deviation factor of s = 1.17. This is a pretty good result that verifies the
limit at least at the resonance combinations of d and A.
However, it is also noticed that the LDOS actually exceeds the theoretic limit
obtain with Eq. (1.15) in short wavelength ranges. The reason is that the resonance
radius is too large compared to the wavelength. For example, at the wavelength of
700 nm, the resonance radius is 273 nm, this would lead to kd = 2.45 and 1/(kd) 3

+
1/(kd) = 0.47. As a matter of fact, 1/(kd) 3 + 1/(kd) < 1 for all resonant spheres,
thus the O(kL) term in Eq. (1.13) will have a notable influence to the limit, causing
the actual limit higher than Eq. (1.15).

4.2 Polarized LDOS Against Limit

As the optimization of the total LDOS requires the geometry to have mutation invari-
ant symmetry on three axis and a minimum separation distance constraint on three
axis, this greatly reduces the number of geometry choices and the chance to achieve
"resonance". Therefore, we now change the subject of optimization from the total
LDOS to the polarized LDOS.
The polarized LDOS is defined as the LDOS produced by only one dipole direction:

p(xo) - Im[sj - E, (xo)], (4.5)

this differs from Eq. (1.5) in that the summation over three dipole is deleted.
Since the three dipole directions are identical in the integral in Eq. (1.13), the
new limit for polarized LDOS limit is then

ptot 1 X (w)|2 1 1
< 1 +[- + ].(4.6)
Po - 3 ImX(w) (kd) 3 kd

which is about 1/3 of the total LDOS limit.

51
 As for the optimization, we can now implement a rotational symmetry around one
axis as well as a mirror symmetry. The shape functions are chosen to be

n]"2, < W_
R(0, = d+d+[E
d) 2
Pn[(I)n]
- 2
(4.7)

,
d+ [Enpn(2 - )"|2 92

Here we use the polynomials as the base function for R(6, #) as the polynomials are
simple and typically a order of n = 5 would be already good enough to approximate
an arbitrary function.

a) d- . n b) d-50 nm

1L04

20.

202.

900 400 500 000 700 60o 90

C) 400 00 70 800
d) -nm)

F ~ ~(*

Figure 4-6: LDOS optimization using polynomials in a silver cavity. Optimized LDOS
for polynomials (blue line) as a function of the wavelength against the theoretic limit
(black line) at the minimum separation distance (a) d = 10 nm and (b) d = 50 nm.
(c) +Z and +X view of the optimized geometry at the wavelength of 700 nm and
d = 10 nm. (d) +Z and +X view of the optimized geometry at the wavelength of 700
nm and d = 50 nm.

The optimized LDOS as a function of wavelength is shown in Fig. 4-6. The other

52
parameters are chosen in comparison with the result in the first section. The average
derivation factor K is 65 and 8 for d = 10 nm and 50 nm respectively. Compared to
the cylinder result of 689 and 36 in the first section, this is really a great improvement.
Especially at the wavelength of A = 450 nm, the optimized LDOS 31.4 is only about
3 times smaller than the theoretical limit of 100. Meanwhile, from the optimized
structures shown in Fig. 4-6(c)(d), we can see that the limit which assumes all
surrounding points at a minimum separation is overestimated. As discussed in the
first section, there should be a factor of 4 decrease to the K factor if the geometry is
pancake-like. In the current case, we can numerically evaluate the limit integral of
the specific shape, which gives a general decrease of factor 3 in the K. Therefore, the
limit is nearly reached when all factors are taking into consideration.

4.3 Conclusion
The total LDOS optimization is conducted on the spherical harmonic shapes and
three simple geometries: ellipsoid, cuboid and cylinder. The cylinder has the smallest
average deviation of K = 36, 689 for d = 50, 10 nm respectively. The spherical
harmonics performs slightly better than the cylinder with general decrease of about
1.5 in the factor K. The resonant sphere has the smallest average deviation factor
K = 1.17 that is almost approaching the limit, though the large separation distance
d will cause the effect of O(kL) in Eq. (1.13) to become notable. The polarized
LDOS optimization is conducted on the rotational polynomials, the average deviation
K is 8 and 65 for d = 50, 10 nm respectively. The limit of the polarized LDOS
is approximately reached when considering the shape-dependent limit in the short
wavelength range.
To conclude, the LDOS limit of Eq. (1.15) is generally an overestimate of the
actual optimized LDOS that can be achieved. However, it is still a valid limit in
a sense that it can be reached at certain circumstances. Besides, the limit is more
difficult to reach the limit in the long wavelength range or in the short minimum
separation distance range.

53
54
Appendix A

Custom Surface Mesh Criterion

#include <CGAL/ license /Surfacemesher . h>

#include <CGAL/Surfacemesher/Standard_ criteria. h>

#include <iostream>
namespace CGAL {
template <class Tr>
class Surface_ mesh_ custom_ criteria_3

{
typedef Surface_ mesher:: Refine _criterion <Tr> Criterion;
typedef Surfacemesher:: Standard_ criteria<Criterion> Criteria;
public:
typedef Tr Triangulation;
typedef typename Tr:: Geom traits::FT FT;
typedef typename Criteria :: Quality Quality;
typedef _mefyehacusTrimteri3(cont
typename Tr:: Facet Facet; FT;agebud
typedef typename Tr:: Point Point;
Surface
const FT radius bound1,
const FT distance_bound1,
const FT radiusbound2,
const FT distancebound2, double dmin)
curvature size criterion1 (distance_ bound1),
uniform _ size_ criterioni (radiusboundl ),
curvature- size_ criterion2 (distance_ bound2)

uniform size criterion2 (radiusbound2),

55
 aspect_ ratio_ criterion (angle_bound),

Dmin(dmin)

{
criterion _vector1 . reserve (4);
criterion _vectori .pushback (&aspect _ratio_ criterion);

criterion _vector1 .pushback (&uniform _size_ criterion );

criterion _vector1 .pushback (&curvature_ size -criterionI);
criterial .set cri teria(criterion vector );
criterion _vector2 . reserve (4);
criterion _ vector2 .pushback (&aspect _ ratio _ criterion);

criterion _vector2 .pushback (&uniform_ sizecriterion2);

criterion vector2 .pushback (&curvature _ size_ criterion2);

criteria2 .set cri teria (criterion vector2 );

}
bool isbad (const Facet& f, Quality& q) const {
Point p1 = f . first ->vertex (( f. second+1)&3)->point (;
Point p2 = f . first ->vertex ((f. second+2)&3)->point (;
Point p3 = f. first ->vertex ((f. second+3)&3)->point ();
double dtemp = sqrt ((pl.x()+p2.x(+p3.x ())
*(pl . x(+p2 .x(+p3 .x ())+(pl. y(+p2.- y(+p3. y)*
(pl. y(+p2. y()+p3. y ())+(p1. z ()+p2. z ()+p3. z )*(p1. z ()+p2. z ()+p3. z ))/3;
if (dtemp<Dmin)
return criterial is_bad(f, q);
else

return criteria2.is_bad(f, q);}

private:

Surfacemesher :: Curvature_ size_ criterion<Tr> curvature _size_ criterion 1

Surface _mesher :: Curvature_ size_ criterion<Tr> curvature _ size _ criterion2

Surfacemesher :: Uniform_ size_ criterion<Tr> uniform _size_ criterionI;

Surface mesher :: Uniform_ size_ criterion<Tr> uniform size _ criterion2 ;

Surfacemesher :: Aspect _ratio_ criterion<Tr> aspect_ ratio_ criterion;
std :: vector<Criterion*> criterion _vectorI , criterion vector2
Criteria criterial , criteria2
double Dmin;

56
Bibliography

[1] A. Oskooi and S. G. Johnson, "Electromagnetic wave source conditions," in "Ad-

vances in FDTD Computational Electrodynamics: Photonics and Nanotechnol-
ogy," A. Taflove, A. Oskooi, and S. G. Johnson, eds. (Artech, 2013), chap. 4, pp.
65-100.

[2] N.G. Van Kampen, B.R.A. Nijboer, and K. Schram, "On the macroscopic theory
of van der Waals forces," Phys. Lett. A 26, 307 (1968).

[3] E. Gerlach, Phys. Rev. B "Equivalence of van der Waals forces between solids
and the surface-plasmon interaction," 4, 393 (1971).

[4] J.-B. Pendry, "Shearing the vacuum-quantum friction," J. Phys.: Condens. Mat-
ter, 9, 10301 (1997).

[5] J.P. Mulet, K. Joulain, R. Carminati, and J.-J. Greffet, "Enhanced radiative
heat transfer at nanometric distances," Microscale Thermophys. Eng. 6, 209-222
(2002).

[6] K. Joulain, R. Carminati, J.-P. Mulet, and J.-J. Greffet, "Definition and mea-
surement of the local density of electromagnetic states close to an interface,"
Phys. Rev. B 68, 245405 (2003).

[7] R. R. Chance A. Prock and R. Silbey, "Molecular Fluorescence and Energy Trans-
fer Near Interfaces," Adv. Chem. Phys. 37, 1 (1978)

[8] P. Berman, ed., Cavity Quantum Electrodynamics, Academic, 1994.

57
 [9] L. Novotny and B. Hecht, Principles of Nano-Optics, Cambridge University,
2006.

[10] Wijnands, F., J. B. Pendry, F. J. Garcia-Vidal, P. M. Bell, P. J. Roberts, and L.

M. Moreno, "Green's functions for Maxwell's equations: Application to sponta-
neous emission," Opt. Quan. Elect., 29, 199-216 (1997).

[11] Xu, Y., R. K. Lee, and A. Yariv, "Quantum analysis and the classical analysis
of spontaneous emission in a microcavity," Phys. Rev. A, 61, 033807 (2000).

[12] Sakoda, K., Optical Properties of Photonic Crystals, Berlin, Germany: Springer,
2001.

[13] Purcell, E. M., "Spontaneous emission probabilities at radio frequencies," Phys.

Rev., 69, 681 (1946).

114] Hamam, R. E., M. Ibanescu, E. J. Reed, P. Bermel, S. G. Johnson, E. Ippen, J. D.

Joannopoulos, and M. Soljacic, "Purcell effect in nonlinear photonic structures:
A coupled mode theory analysis," Opt. Express, 16, 12523-12537 (2008).

[15] E. Ozbay, "Plasmonics: merging photonics and electronics at nanoscale dimen-

sions," Science 311, 189-193 (2006).

[16] S. A. Maier, "Plasmonics: Fundamentals and Applications", Springer Science

Business Media, 2007 &
.

[171 A. Boltasseva and H.A.Atwater, "Low-loss plasmonic metamaterials," Science

331,290-291(2011).

[18] 0. D. Miller, A. G. Polimeridis, M. T. H.Reid, C. W.Hsu, B. G. DeLacy, J. D.

Joannopoulos, M. Soljacic, and S. G. Johnson, "Fundamental limits to optical
response in absorptive systems," Opt. Express 24, 3329-3364 (2016).

[19] M. D. Arnold and M. G. Blaber, "Optical performance and metallic absorption

in nanoplasmonic systems," Opt. Express 17, 3835-3847 (2009).

58
[20] A. Raman, W. Shin, and S. Fan, "Upper bound on the modal material loss rate
in plasmonic and metamaterial systems," Phys. Rev. Lett. 110, 183901 (2013).

[21] E. M. Purcell, "On the absorption and emission of light by interstellar grains,"
Astrophys. J. 158, 433-440 (1969).

[22] C. Sohl, M. Gustafsson, and G. Kristensson, "Physical limitations on metama-

terials: restrictions on scattering and absorption over a frequency interval," J.
Phys. D. Appl. Phys. 40, 7146-7151 (2007).

[231 C. Sohl, M. Gustafsson, and G. Kristensson, "Physical limitations on broadband

scattering by heterogeneous obstacles," J. Phys. A Math. Theor. 40, 11165-11182
(2007).

[24] M. Gustafsson, C. Sohl, and G. Kristensson, "Physical limitations on antennas of

arbitrary shape," Proc. R. Soc. A Math. Phys. Eng. Sci. 463, 2589-2607 (2007).

[25] D.-H. Kwon and D. M. Pozar, "Optimal characteristics of an arbitrary receive

antenna," IEEE Trans. Antennas Propag. 57, 3720-3727 (2009).

[26] I. Liberal, Y. Ra'di, R. Gonzalo, I. Ederra, S. A. Tretyakov, and R. W. Ziolkowski,

"Least upper bounds of the powers extracted and scattered by bi-anisotropic
particles," IEEE Trans. Antennas Propag. 62, 4726-4735 (2014).

[27] H. A. Wheeler, "Fundamental limitations of small antennas," Proc. IRE 35,

1479-1484 (1947).

[28] L. J. Chu, "Physical limitations of omni-directional antennas," J. Appl. Phys.

19, 1163-1175 (1948).

[29] J. S. McLean, "A re-examination of the fundamental limits on the radiation Q of

electrically small antennas," IEEE Trans. Antennas Propag. 44, 672-676 (1996).

[30] F. Wang and Y. R. Shen, "General properties of local plasmons in metal nanos-
tructures," Phys. Rev. Lett. 97, 206806 (2006).

59
[31] J.-P. Hugonin, M. Besbes, and P. Ben-Abdallah, "Fundamental limits for light
absorption and scattering induced by cooperative electromagnetic interactions,"
Phys. Rev. B 91, 180202 (2015).

[321 K. Joulain, J.-P. Mulet, F. Marquier, R. Carminati, and J.-J. Greffet, "Surface
electromagnetic waves thermally excited: radiative heat transfer, coherence prop-
erties and casimir forces revisited in the near field," Surf. Sci. Rep. 57, 59-112
(2005).

[33] L. N. Trefethen and D. Bau, Numerical Linear Algebra (Society for Industrial
and Applied Mathematics, 1997).

[341 R. M. Errico, ?What is an adjoint model?,? Bulletin Am. Meteorological Soc.

78, 2577-2591 (1997).

[35] Y. Cao, S. Li, L. Petzold, and R. Serban, "Adjoint sensitivity analysis for differ-
entialalgebraic equations: The adjoint DAE system and its numerical solution,?
SIAM J. Sci. Comput., 24, 1076-1089 (2003).

[36] G. Strang, Computational Science and Engineering. Wellesley, MA: Wellesley-

Cambridge Press, 2007.

[37] S. G. Johnson, "Notes on Adjoint Methods for 18.335", 2012

[38] R.-E. Plessix, "A review of the adjoint-state method for computing the gradient
of a functional with geophysical applications", Geophysical Journal International
167, 495-503, (2006).

[39] 0. D. Miller, "Photonic Design: From Fundamental Solar Cell Physics to Com-
putational Inverse Design", PhD Thesis in Electric Engineering, UC Berkeley,
2012

[40] Diederik P. Kingma, Jimmy Ba, "Adam: A Method for Stochastic Optimization,"
arXiv:1412.6980

60
[41] P. K. Banerjee, R. Butterfield, Boundary element methods in engineering science,
McGraw-Hill Book Co. (UK), 1981.

[42] H. Reid, S. G. Johnson, "Efficient Computation of Power, Force, and Torque in

BEM Scattering Calculations," ArXiv e-prints, 1307.2966 (2013).

[43] E. D. Palik, Handbook of Optical Constants of Solids, (Elsevier Science,1998).

[44] G. Mie, Gustav. "Beitrige zur Optik truber Medien, speziell kolloidaler
Metall6sungen". Annalen der Physik. 330 (3): 377-445 (1908)

[45] C. Henkel, K. Joulain, R. Carminati, and J.-J. Greffet, "Spatial coherence of

thermal near fields," Opt. Commun. 186, 57 (2000).

[46] C. F. Bohren and D. R. Huffman, "Absorption and Scattering of Light by Small

Particles" (John Wiley & Sons, 1983).

[47] https://homerreid.github.io/scuff-em-documentation/reference/BrillouinZonelntegration

[48] J. A. Scholl, A. L. Koh, and J. A. Dionne, "Quantum plasmon resonances of

individual metallic nanoparticles," Nature 483, 421-427 (2012).

[49] C. Geuzaine and J. F. Remacle. "Gmsh: a three-dimensional finite element mesh

generator with built-in pre- and post-processing facilities," Int. J. Numer. Meth.
Eng. 79(11), 1309-1331 (2009).

[50] J. D. Boissonnat and S. Oudot. "Provably good sampling and meshing of sur-
faces," Graphical Models 67, 405?451 (2005).

[51] M.Phillips. G. Manual, Version 1.6.1 for Unix Workstations. The Geometry Cen-
ter, University of Minnesota, 1996.

[52] L. Rineau and M. Yvinec. "A generic software design for Delaunay refinement
meshing," Comput. Geom. Theory Appl. 38, 100?110 (2007).

61
[53] S. Osher and J. A. Sethian, "Fronts Propagating with Curvature Dependent
Speed: Algorithms Based on Hamilton-Jacobi Formulations," Jour. Comp. Phys.,
79, 12-49 (1988).

[54] S. Osher and R. Fedkiw, Level Set Methods and Dynamic Implicit Surfaces.
SpringerVerlag New York, Inc., 2003

[55] J. A. Sethian, Level set methods and fast marching methods: evolving interfaces
in computational geometry, fluid mechanics, computer vision, and materials sci-
ence, Cambridge University Press, 1999

[56] M. P. Givens,"Optical Properties of Metals," Solid State Physics 6, 313-352

(1958).

[57] M. E. Abdelsalam S. Cintra, S. Mahajan, A. E. Russell, and P. N. Bartlett,

"Localized and delocalized plasmons in metallic nanovoids" Phys. Rev. B 74,
245415 (2006).

[58] A. D. Boardman, Electromagnetic Surface Modes, Wiley-Interscience, 1982

62