posted on 2017-01-04, 23:37authored byChathurangi Kumarasinghe
When electromagnetic
radiation is applied to a nanoparticle, scattering, absorption, and transmission of this radiation can take
place. The absorbed radiation (photons) will increase the kinetic and potential
energy of electrons inside the particle, pushing them into excited states. These
excited electrons with high energy are not in thermal equilibrium with the
lattice of the nanoparticle
and hence are referred to as hot electrons.
Hot electrons are
injected into the surrounding media if their energies are high enough to cross over the energy barrier at the interface
between the nanoparticles and the surroundings. This results in generation of a photocurrent, which is found useful in many opto electronic applications. Therefore,
hot electron generation and injection is a field of high scientific interest.
Localized surface
plasmons (LSPs) generated in metallic nanoparticles via optical excitation create an enhanced electric field inside the
nanoparticle, aiding the hot electron generation process. In smaller metallic nanoparticles, absorption is much more dominant than scattering and a larger proportion
of excited electrons
end up in higher energy levels, making them ideal for hot
electron injection related applications.
As the particle
dimensions are reduced to nanoscale and become comparable to the wavelength of the electron wave function, the energy
levels of electrons become highly discreet and geometrically dependent. The
efficiency and magnitude of the hot electron injection process depends on the energy
spectrum of the electrons, which is determined based on the shape and size of
the nanoparticle. In this thesis, the
shape and size dependent hot electron generation and injection behaviour of metallic nanoparticles, considering the
quantized motion of the conduction electrons, are studied. The results of this study are used to
design a hot electron based all-optical direction-switching device, which
is extremely useful in nanoscale electronic circuitry.
The shape and size
dependence of the electron energy levels cause the dielectric function of the nanoparticle to be geometry dependent as the
dimensions of the particle are reduced. When analysing hot electron
generation and other optical properties of nanoparticles, the dielectric function is a key
input. Therefore, it is important to obtain a realistic dielectric function based
on electron excitations at different frequencies, considering the shape as well as
the size of the particle by following a quantum-mechanical approach. Therefore, as a
final part of this research, the quantum confinement effects on the
frequency-dependent dielectric function of metallic nanoparticles and its influence on hot
electron generation are studied.
This thesis is
organized as follows. An introduction to hot electrons in nanoparticles and the objectives of this research are presented in Chapter
1, followed by a literature review of the mathematical techniques used to
model hot electron generation and injection in Chapter 2. Chapters 3 and 4 present
theoretical analyses of shape- and size-dependent hot electron behaviour and
design guidelines for nanorods and nanotubes, respectively. A design of a novel
all-optical hot electron based current-direction-switching device (CDSD) is presented
in Chapter 5, while Chapter 6 discusses the effects of quantum confinement
on the permittivity of a nanoparticle and how it effects hot electron generation.
Chapter 7 presents a summary of contributions and suggestions for future research.