John V. Foreman

Low dislocation densities and long carrier lifetimes in GaN thin films grown on a SiNx nanonetwork

Significant improvement of structural and optical qualities of GaN thin films on sapphire substrates was achieved by metal organic chemical vapor deposition with in situ SiNx nanonetwork. Transmission electron microscope (TEM) studies revealed that screw- and edge-type dislocations were reduced to 4.4×107 and 1.7×107cm−2, respectively, for a ∼5.5-μm-thick layer. Furthermore, room temperature carrier lifetimes of 2.22 and 2.49ns were measured by time-resolved photoluminescence (TRPL) for samples containing single and double SiNx network layers, respectively, representing a significant improvement over the previous studies. The consistent trends among the TEM, x-ray diffraction, and TRPL measurements suggest that in situ SiNx network reduces line defects effectively as well as the point-defect-related nonradiative centers.

Inhibition of Linear Absorption in Opaque Materials Using Phase-Locked Harmonic Generation

We theoretically predict and experimentally demonstrate inhibition of linear absorption for phase and group velocity mismatched second- and third-harmonic generation in strongly absorbing materials, GaAs, in particular, at frequencies above the absorption edge. A 100-fs pump pulse tuned to 1300 nm generates 650 and 435 nm second- and third-harmonic pulses that propagate across a 450-microm-thick GaAs substrate without being absorbed. We attribute this to a phase-locking mechanism that causes the pump to trap the harmonics and to impress on them its dispersive properties.

Effects of reabsorption and spatial trap distributions on the radiative quantum efficiencies of ZnO

Ultrafast time-resolved photoluminescence spectroscopy following one- and two-photon excitations of ZnO powder is used to gain unprecedented insight into the surprisingly high external quantum efficiency of its “green” defect emission band. The role of exciton diffusion, the effects of reabsorption, and the spatial distributions of radiative and nonradiative traps are comparatively elucidated for the ultraviolet excitonic and “green” defect emission bands in both unannealed nanometer-sized ZnO powders and annealed micrometersized ZnO:Zn powders. We find that the primary mechanism limiting quantum efficiency is surface recombination because of the high density of nonradiative surface traps in these powders. It is found that unannealed ZnO has a high density of bulk nonradiative traps as well, but the annealing process reduces the density of these bulk traps while simultaneously creating a high density of green-emitting defects near the particle surface. The data are discussed in the context of a simple rate equation model that accounts for the quantum efficiencies of both emission bands. The results indicate how defect engineering could improve the efficiency of ultraviolet-excited ZnO:Zn-based white light phosphors.

Ultraviolet surface-enhanced Raman scattering at the plasmonic band edge of a metallic grating

Surface-enhanced Raman Scattering (SERS) is studied in sub-wavelength metallic gratings on a substrate using a rigorous electromagnetic approach. In the ultraviolet SERS is limited by the metallic dampening, yet enhancements as large as 10(5) are predicted. It is shown that these enhancements are directly linked to the spectral position of the plasmonic band edge of the metal/substrate surface plasmon. A simple methodology is presented for selecting the grating pitch to produce optimal enhancement for a given laser frequency.

Sulfur-doped zinc oxide (ZnO) Nanostars: Synthesis and simulation of growth mechanism

AbstractWe present a bottom-up synthesis, spectroscopic characterization, and ab initio simulations of star-shaped hexagonal zinc oxide (ZnO) nanowires. The ZnO nanostructures were synthesized by a low-temperature hydrothermal growth method. The cross-section of the ZnO nanowires transformed from a hexagon to a hexagram when sulfur dopants from thiourea [SC(NH2)2] were added into the growth solution, but no transformation occurred when urea (OC(NH2)2) was added. Comparison of the X-ray photoemission and photoluminescence spectra of undoped and sulfur-doped ZnO confirmed that sulfur is responsible for the novel morphology. Large-scale theoretical calculations were conducted to understand the role of sulfur doping in the growth process. The ab initio simulations demonstrated that the addition of sulfur causes a local change in charge distribution that is stronger at the vertices than at the edges, leading to the observed transformation from hexagon to hexagram nanostructures.

The dependence of ZnO photoluminescence efficiency on excitation conditions and defect densities

The quantum efficiencies of both the band edge and deep-level defect emission from annealed ZnO powders were measured as a function of excitation fluence and wavelength from a tunable sub-picosecond source. A simple model of excitonic decay reproduces the observed excitation dependence of rate constants and associated trap densities for all radiative and nonradiative processes. The analysis explores how phosphor performance deteriorates as excitation fluence and energy increase, provides an all-optical approach for estimating the number density of defects responsible for deep-level emission, and yields new insights for designing efficient ZnO-based phosphors.

Taming the thermal emissivity of metals: A metamaterial approach

We demonstrate the possibility of realizing temporally coherent, wide-angle, thermal radiation sources based on the metamaterial properties of metallic gratings. In contrast to other approaches, we do not rely on the excitation of surface waves such as phonon-polaritons, plasmon-polaritons, or guided mode resonances along the grating, nor on the absorption resonances of extremely shallow metallic grating. Instead, we exploit the effective bulk properties of a thick metallic grating below the first diffraction order. We analytically model this physical mechanism of temporally coherent thermal emission based on localized bulk resonances in the grating. We validate our theoretical predictions with full-wave numerical simulations.

Thermal emission from a metamaterial wire medium slab

We investigate thermal emission from a metamaterial wire medium embedded in a dielectric host and highlight two different regimes for efficient emission, respectively characterized by broadband emission near the effective plasma frequency of the metamaterial, and by narrow-band resonant emission at the band-edge in the Bragg scattering regime. We discuss how to control the spectral position and relative strength of these two emission mechanisms by varying the geometrical parameters of the proposed metamaterial and its temperature.

Localized excitons mediate defect emission in ZnO powders

A series of continuous-wave spectroscopic measurements elucidates the mechanism responsible for the technologically important green emission from deep-level traps in ZnO:Zn powders. Analysis of low-temperature photoluminescence (PL) and PL excitation spectra for bound excitons compared to the temperature-dependent behavior of the green emission reveals a deep correlation between green PL and specific donor-bound excitons. Direct excitation of these bound excitons produces highly efficient green emission from near-surface defects. When normalized by the measured external quantum efficiency, the integrated PL for both excitonic and green emission features grows identically with excitation intensity, confirming the strong connection between green emission and excitons. The implications of these findings are used to circumscribe operational characteristics of doped ZnO-based white light phosphors whose quantum efficiency is almost twice as large when the bound excitons are directly excited.

Influence of temperature and photoexcitation density on the quantum efficiency of defect emission in ZnO powders

The effect of laser excitation power density on the efficiency of intrinsic defect emission in ZnO powders was characterized by varying the laser irradiance over three orders of magnitude and monitoring changes in the samples’ photoluminescence. The external quantum efficiency of the visible wavelength, broadband defect photoluminescence was found to depend not only on laser irradiance but also on temperature and prior annealing conditions. This material system is potentially useful as an ultraviolet-photoexcited, white light phosphor under low-power excitation (<0.2W∕cm2) at room temperature and below.