Zinc oxide quantum dot nanostructures

Zinc oxide (ZnO) is one of the most intensely studied wide band gap semiconductors due to its many desirable properties. This project established new techniques for investigating the hydrodynamic properties of ZnO nanoparticles, their assembly into useful photonic structures, and their multiphoton absorption coefficients for excitation with visible or infrared light rather than ultraviolet light. The methods developed are also applicable to a wide range of nanoparticle samples.

Simulations of the effect of waveguide cross-section on quantum dot – plasmon coupling

Quantum dot - plasmon waveguide systems are of interest for the active control of plasmon propagation, and consequently, the development of active nanophotonic devices such as nano-sized optical transistors. This paper is concerned with how varying aspect ratio of the waveguide crosssection affects the quantum dot - plasmon coupling. We compare a stripe waveguide with an equivalent nanowire, illustrating that both waveguides have a similar coupling strength to a nearby quantum dot for small waveguide cross-section, thereby indicating that stripe lithographic waveguides have strong potential use in quantum dot –plasmon waveguide systems. We also demonstrate that changing the aspect ratio of both stripe and wire waveguides can increase the spontaneous emission rate of the quantum dot into the plasmon mode, by up to a factor of five. The results of this paper will contribute to the optimisation of quantum dot - plasmon waveguide systems and help pave the way for the development of active nanophotonics devices.

Simulations of the spontaneous emission of a quantum dot near a gap plasmon waveguide

In this paper we modeled a quantum dot at near proximity to a gap plasmon waveguide to study the quantum dot-plasmon interactions. Assuming that the waveguide is single mode, this paper is concerned about the dependence of spontaneous emission rate of the quantum dot on waveguide dimensions such as width and height. We compare coupling efficiency of a gap waveguide with symmetric configuration and asymmetric configuration illustrating that symmetric waveguide has a better coupling efficiency to the quantum dot. We also demonstrate that optimally placed quantum dot near a symmetric waveguide with 50 nm x 50 nm cross section can capture 80% of the spontaneous emission into a guided plasmon mode.

Self-organized quantum dot arrays : kinetic mapping of adatom capture

Deterministic synthesis of self-organized quantum dot arrays for renewable energy, biomedical, and optoelectronic applications requires control over adatom capture zones, which are presently mapped using unphysical geometric tessellation. In contrast, the proposed kinetic mapping is based on simulated two-dimensional adatom fluxes in the array and includes the effects of nucleation, dissolution, coalescence, and process parameters such as surface temperature and deposition rate. This approach is generic and can be used to control the nanoarray development in various practical applications. © 2009 American Institute of Physics.

Deterministic control of plasma-assembled self-organized Ge/Si quantum dot arrays

Self-assembly of size-uniform and spatially ordered quantum dot (QD) arrays is one of the major challenges in the development of the new generation of semiconducting nanoelectronic and photonic devices. Assembly of Ge QD (in the ∼5-20 nm size range) arrays from randomly generated position and size-nonuniform nanodot patterns on plasma-exposed Si (100) surfaces is studied using hybrid multiscale numerical simulations. It is shown, by properly manipulating the incoming ion/neutral flux from the plasma and the surface temperature, the uniformity of the nanodot size within the array can be improved by 34%-53%, with the best improvement achieved at low surface temperatures and high external incoming fluxes, which are intrinsic to plasma-aided processes. Using a plasma-based process also leads to an improvement (∼22% at 700 K surface temperature and 0.1 MLs incoming flux from the plasma) of the spatial order of a randomly sampled nanodot ensemble, which self-organizes to position the dots equidistantly to their neighbors within the array. Remarkable improvements in QD ordering and size uniformity can be achieved at high growth rates (a few nms) and a surface temperature as low as 600 K, which broadens the range of suitable substrates to temperature-sensitive ultrathin nanofilms and polymers. The results of this study are generic, can also be applied to nonplasma-based techniques, and as such contributes to the development of deterministic strategies of nanoassembly of self-ordered arrays of size-uniform QDs, in the size range where nanodot ordering cannot be achieved by presently available pattern delineation techniques.

Ge/Si quantum dot formation from non-uniform cluster fluxes

The controlled growth of ultra-small Ge/Si quantum dot (QD) nuclei (≈1 nm) suitable for the synthesis of uniform nanopatterns with high surface coverage, is simulated using atom-only and size non-uniform cluster fluxes. It is found that seed nuclei of more uniform sizes are formed when clusters of non-uniform size are deposited. This counter-intuitive result is explained via adatom-nanocluster interactions on Si(100) surfaces. Our results are supported by experimental data on the geometric characteristics of QD patterns synthesized by nanocluster deposition. This is followed by a description of the role of plasmas as non-uniform cluster sources and the impact on surface dynamics. The technique challenges conventional growth modes and is promising for deterministic synthesis of nanodot arrays.

Numerical simulation of self-organized nano-islands in plasma-based assembly of quantum dot arrays

This work presents the details of the numerical model used in simulation of self-organization of nano-islands on solid surfaces in plasma-assisted assembly of quantum dot structures. The model includes the near-substrate non-neutral layer (plasma sheath) and a nanostructured solid deposition surface and accounts for the incoming flux of and energy of ions from the plasma, surface temperature-controlled adatom migration about the surface, adatom collisions with other adatoms and nano-islands, adatom inflow to the growing nano-islands from the plasma and from the two-dimensional vapour on the surface, and particle evaporation to the ambient space and the two-dimensional vapour. The differences in surface concentrations of adatoms in different areas within the quantum dot pattern significantly affect the self-organization of the nano-islands. The model allows one to formulate the conditions when certain islands grow, and certain ones shrink or even dissolve and relate them to the process control parameters. Surface coverage by selforganized quantum dots obtained from numerical simulation appears to be in reasonable agreement with the available experimental results.

High efficiency quantum dot-sensitised solar cells by material science and device architecture

This thesis studied cadmium sulfide and cadmium selenide quantum dots and their performance as light absorbers in quantum dot-sensitised solar cells. This research has made contributions to the understanding of size dependent photodegradation, passivation and particle growth mechanism of cadmium sulfide quantum dots using SILAR method and the role of ZnSe shell coatings on solar cell performance improvement.

Enhanced electron lifetime of CdSe/CdS quantum dot (QD) sensitized solar cells using ZnSe core–shell structure with efficient regeneration of quantum Ddots

Research on development of efficient passivation materials for high performance and stable quantum dot sensitized solar cells (QDSCs) is highly important. While ZnS is one of the most widely used passivation material in QDSCs, an alternative material based on ZnSe which was deposited on CdS/CdSe/TiO2 photoanode to form a semi-core/shell structure has been found to be more efficient in terms of reducing electron recombination in QDSCs in this work. It has been found that the solar cell efficiency was improved from 1.86% for ZnSe0 (without coating) to 3.99% using 2 layers of ZnSe coating (ZnSe2) deposited by successive ionic layer adsorption and reaction (SILAR) method. The short circuit current density (Jsc) increased nearly 1-fold (from 7.25 mA/cm2 to13.4 mA/cm2), and the open circuit voltage (Voc) was enhanced by 100 mV using ZnSe2 passivation layer compared to ZnSe0. Studies on the light harvesting efficiency (ηLHE) and the absorbed photon-to-current conversion efficiency (APCE) have revealed that the ZnSe coating layer caused the enhanced ηLHE at wavelength beyond 500 nm and a significant increase of the APCE over the spectrum 400−550 nm. A nearly 100% APCE was obtained with ZnSe2, indicating the excellent charge injection and collection process in the device. The investigation on charge transport and recombination of the device has indicated that the enhanced electron collection efficiency and reduced electron recombination should be responsible for the improved Jsc and Voc of the QDSCs. The effective electron lifetime of the device with ZnSe2 was nearly 6 times higher than ZnSe0 while the electron diffusion coefficient was largely unaffected by the coating. Study on the regeneration of QDs after photoinduced excitation has indicated that the hole transport from QDs to the reduced species (S2−) in electrolyte was very efficient even when the QDs were coated with a thick ZnSe shell (three layers). For comparison, ZnS coated CdS/CdSe sensitized solar cell with optimum shell thickness was also fabricated, which generated a lower energy conversion efficiency (η = 3.43%) than the ZnSe based QDSC counterpart due to a lower Voc and FF. This study suggests that ZnSe may be a more efficient passivation layer than ZnS, which is attributed to the type II energy band alignment of the core (CdS/CdSe quantum dots) and passivation shell (ZnSe) structure, leading to more efficient electron−hole separation and slower electron recombination.

Optimizing the quantum dot: Plasmon interaction in a nano gap waveguide

Spontaneous emission (SE) of a Quantum emitter depends mainly on the transmission strength between the upper and lower energy levels as well as the Local Density of States (LDOS)[1]. When a QD is placed in near a plasmon waveguide, LDOS of the QD is increased due to addition of the non-radiative decay and a plasmonic decay channel to free space emission[2-4]. The slow velocity and dramatic concentration of the electric field of the plasmon can capture majority of the SE into guided plasmon mode (Гpl ). This paper focused on studying the effect of waveguide height on the efficiency of coupling QD decay into plasmon mode using a numerical model based on finite elemental method (FEM). Symmetric gap waveguide considered in this paper support single mode and QD as a dipole emitter. 2D simulation models are done to find normalized Гpl and 3D models are used to find probability of SE decaying into plasmon mode ( β) including all three decay channels. It is found out that changing gap height can increase QD-plasmon coupling, by up to a factor of 5 and optimally placed QD up to a factor of 8. To make the paper more realistic we briefly studied the effect of sharpness of the waveguide edge on SE emission into guided plasmon mode. Preliminary nano gap waveguide fabrication and testing are already underway. Authors expect to compare the theoretical results with experimental outcomes in the future

A novel fluorescent probe involving a graphene quantum dot-enzyme hybrid system for the analysis of hydroquinone in the presence of toxic resorcinol and catechol

An efficient method for the analysis of hydroquinone at trace levels in water samples has been developed in the form of a fluorescent probe based on graphene quantum dots (GQDs). The analytical variable, fluorescence quenching, was generated from the formation of benzoquinone intermediates, which formed during the catalytic oxidation of hydroquinone by horseradish peroxidase (HRP). In general, the reaction mechanism involved hydroquinone, as an electron acceptor, which affected the surface state of GQDs via an electron transfer effect. The water-soluble GQDs were directly prepared by the pyrolysis of citric acid and with the use of the mentioned hybrid enzyme system, the detection limit for hydroquinone was as low as 8.4 × 10−8 M. Furthermore, this analysis was almost unaffected by other phenol and quinine compounds, such as phenol, resorcinol and other quinines, and therefore, the developed GQD method produced satisfactory results for the analysis of hydroquinone in several different lake water samples.

Coupling of energy from quantum emitters to the plasmonic mode of V groove waveguides: A numerical study

This work is a theoretical investigation into the coupling of a single excited quantum emitter to the plasmon mode of a V groove waveguide. The V groove waveguide consists of a triangular channel milled in gold and the emitter is modeled as a dipole emitter, and could represent a quantum dot, nitrogen vacancy in diamond, or similar. In this work the dependence of coupling efficiency of emitter to plasmon mode is determined for various geometrical parameters of the emitter-waveguide system. Using the finite element method, the effect on coupling efficiency of the emitter position and orientation, groove angle, groove depth, and tip radius, is studied in detail. We demonstrate that all parameters, with the exception of groove depth, have a significant impact on the attainable coupling efficiency. Understanding the effect of various geometrical parameters on the coupling between emitters and the plasmonic mode of the waveguide is essential for the design and optimization of quantum dot–V groove devices.

Effect of elemental composition and size on electron confinement in self-assembled SiC quantum dots : a combinatorial approach

A high level of control over quantum dot (QD) properties such as size and composition during fabrication is required to precisely tune the eventual electronic properties of the QD. Nanoscale synthesis efforts and theoretical studies of electronic properties are traditionally treated quite separately. In this paper, a combinatorial approach has been taken to relate the process synthesis parameters and the electron confinement properties of the QDs. First, hybrid numerical calculations with different influx parameters for Si1-x Cx QDs were carried out to simulate the changes in carbon content x and size. Second, the ionization energy theory was applied to understand the electronic properties of Si1-x Cx QDs. Third, stoichiometric (x=0.5) silicon carbide QDs were grown by means of inductively coupled plasma-assisted rf magnetron sputtering. Finally, the effect of QD size and elemental composition were then incorporated in the ionization energy theory to explain the evolution of the Si1-x Cx photoluminescence spectra. These results are important for the development of deterministic synthesis approaches of self-assembled nanoscale quantum confinement structures.

Surface fluxes of Si and C adatoms at initial growth stages of SiC quantum dots

Self-assembly of highly stoichiometric SiC quantum dots still remains a major challenge for the gas/plasma-based nanodot synthesis. By means of a multiscale hybrid numerical simulation of the initial stage (0.1-2.5 s into the process) of deposition of SiCSi (100) quantum dot nuclei, it is shown that equal Si and kst atom deposition fluxes result in strong nonstoichiometric nanodot composition due to very different surface fluxes of Si and C adatoms to the quantum dots. At this stage, the surface fluxes of Si and C adatoms to SiC nanodots can be effectively controlled by manipulating the SiC atom influx ratio and the Si (100) surface temperature. It is demonstrated that at a surface temperature of 800 K the surface fluxes can be equalized after only 0.05 s into the process; however, it takes more then 1 s at a surface temperature of 600 K. Based on the results of this study, effective strategies to maintain a stoichiometric ([Si] [C] =1:1) elemental ratio during the initial stages of deposition of SiCSi (100) quantum dot nuclei in a neutral/ionized gas-based process are proposed.