Chelsea R. Haughn

Efficient exciton funneling in cascaded PbS quantum dot superstructures.

Benzenedithiol (BDT) and ethanedithiol (EDT) ligand-exchange treatments can be used to cross-link colloidal PbS quantum dots into nanocrystalline film structures with distinct optoelectronic properties. Such structures can provide a unique platform to study the energy transfer between layers of quantum dots with different sizes. In this report, efficient exciton funneling and recycling of surface state-bound excitons is observed in cascaded PbS quantum dot-based multilayered superstructures, where the excitons transfer from the larger band gap or donor layers to the smallest band gap or acceptor layers. In this system, both the BDT- and EDT-treated cascaded structures exhibit dramatically enhanced photoluminescence from the acceptor layers. As we show, the energy transfer mechanisms involved and their efficiencies are significantly different depending on the ligand-exchange treatment. In the future, we believe these efficient exciton recycling and funneling mechanisms could be used to improve significantly the photocurrent, charge-transport, and conversion efficiencies in low-cost nanocrystalline and hybrid solar cells and the emission efficiencies in hybrid light-emitting devices.

Electrical and optical properties of point defects in ZnO thin films

We show that the deposition of ZnO films under varying oxygen partial pressure and annealing conditions allows for the controllable formation of specific defects. Using x-ray diffraction and photoluminescence, we characterize the defects formed and show that these defects are responsible for changes in film carrier density, carrier type, sheet resistivity and mobility.

Impact of Different Surface Ligands on the Optical Properties of PbS Quantum Dot Solids

The engineering of quantum dot solids with low defect concentrations and efficient carrier transport through a ligand strategy is crucial to achieve efficient quantum dot (QD) optoelectronic devices. Here, we study the consequences of various surface ligand treatments on the light emission properties of PbS quantum dot films using 1,3-benzenedithiol (1,3-BDT), 1,2-ethanedithiol (EDT), mercaptocarboxylic acids (MPA) and ammonium sulfide ((NH4)2S). We first investigate the influence of different ligand treatments on the inter-dot separation, which mainly determines the conductivity of the QD films. Then, through a combination of photoluminescence and transient photoluminescence characterization, we demonstrate that the radiative and non-radiative recombination mechanisms in the quantum dot films depend critically on the length and chemical structure of the surface ligands.

Growth and characterization of TbAs:GaAs nanocomposites

Recently, there has been interest in semimetallic rare earth monopnictide nanoparticles epitaxially embedded in III-V semiconductors due to the drastic changes brought about in these materials’ electrical and thermal properties. The properties of terbium codeposited with gallium arsenide by molecular beam epitaxy are discussed here. These new materials were characterized by x-ray diffraction, Rutherford backscattering spectrometry, resistivity measurements, photoluminescence, time-domain thermoreflectance thermal conductivity measurements, optical absorption spectroscopy, and plan-view high-angle annular dark-field scanning transmission electron microscopy. Results revealed successful formation of randomly distributed nanoparticles with an average diameter of ∼1.5 nm, reduction of thermal conductivity by a factor of about 5, and consistency with theoretical predictions of mid-band-gap Fermi level pinning and behavior of past similar materials. The success of these TbAs:GaAs materials will lead the way for...

Quantification of trap state densities in GaAs heterostructures grown at varying rates using intensity-dependent time resolved photoluminescence

Time-resolved photoluminescence is an established technique for characterizing carrier lifetimes in semiconductors, but the dependence of lifetime on excitation fluence has been only qualitatively investigated. We develop a quantitative approach for fitting fluence-dependent PL decay data to a Shockely-Read-Hall model of carrier recombination in order to extract the trap state density. We demonstrate this approach by investigating growth rate-dependent trap densities in gallium arsenide-indium gallium phosphide double heterostructures. The techniques developed here can be applied for rapid, non-destructive quantification of trap state densities in a variety of materials.

Charge-transfer dynamics in multilayered PbS and PbSe quantum dot architectures

We demonstrate control of the charge transfer process in PbS and PbSe quantum dot assemblies. We first demonstrate efficient charge transfer from donor quantum dots to acceptor quantum dots in a multi-layer PbSe cascade structure. Then, we assemble type-I and type-II heterostructures using both PbS and PbSe quantum dots via careful control of the band alignment. In type-I structures, photo-generated carriers are transferred and localized in the smaller bandgap (acceptor) quantum dots, resulting in a significant luminescence enhancement. In contrast, a significant luminescence quenching and shorter emission lifetime confirms an efficient separation of photo-generated carriers in the type-II architecture.

Carrier transfer from InAs quantum dots to ErAs metal nanoparticles

Erbium arsenide (ErAs) is a semi-metallic material that self-assembles into nanoparticles when grown in GaAs via molecular beam epitaxy. We use steady-state and time-resolved photoluminescence to examine the mechanism of carrier transfer between indium arsenide (InAs) quantum dots and ErAs nanoparticles in a GaAs host. We probe the electronic structure of the ErAs metal nanoparticles (MNPs) and the optoelectronic properties of the nanocomposite and show that the carrier transfer rates are independent of pump intensity. This result suggests that the ErAs MNPs have a continuous density of states and effectively act as traps. The absence of a temperature dependence tells us that carrier transfer from the InAs quantum dots to ErAs MNPs is not phonon assisted. We show that the measured photoluminescence decay rates are consistent with a carrier tunneling model.

Analysis of high growth rate MOCVD structures by solar cell device measurements

Metal organic chemical vapor deposition (MOCVD) tools are integral to many technologies, including the growth of high-efficiency multijunction III-V solar cells. Veeco MOCVD has recently developed new tool designs that allow increased MOCVD growth rates that could drastically increase solar cell throughput and reduce manufacturing costs. It is important, however, to understand the trade-offs between increased throughput and decreased material quality and device performance. We fabricate multijunction III-V solar cells from materials grown by both standard and fast growth rate techniques. We analyze the open circuit voltage, short circuit current, fill factor, efficiency, and ideality factor of both types of devices. Comparison of these devices reveals that the existing fast growth protocols result in solar cells with similar performance to standard growth cells. The results suggest that increased growth rates can enable higher throughput fabrication of solar cells without significant performance sacrifices.

Colloidal Ag Nanoparticles Enhanced Polymer-LEDs by Exciton-Surface Plasmon Coupling

We report high performance enhancement in an all-solution processed polymer LED by incorporating large density of colloidal Ag nanoparticles. A 11-fold maximum luminance enhancement and a 20-fold maximum current efficiency enhancement are observed.