Professor Robert Taylor

Abstract:

We have characterized the carrier dynamics of the excitonic emission emerging from a monolayer of graphene grown on a Cu(111) surface. Excitonic emission from the graphene, with strong and sharp peaks both with a full-width at half-maximum of 2.7 meV, was observed near ~3.16 and ~3.18 eV at 4.2 K. The carrier recombination parameters were studied by measuring both temperature-dependent and time-resolved photoluminescence. The intensity variation with temperature of these two peaks shows an opposing trend. The time-resolved emission was modelled using coupled differential equations and the decay time was found to be dominated by carrier trapping and Auger recombination as the temperature increased.

Abstract:

Crystallographic point defects (PDs) can dramatically decrease the efficiency of optoelectronic semiconductor devices, many of which are based on quantum well (QW) heterostructures. However, spatially resolving individual nonradiative PDs buried in such QWs has so far not been demonstrated. Here, using high-resolution cathodoluminescence (CL) and a specific sample design, we spatially resolve, image, and analyze nonradiative PDs in InGaN/GaN QWs at the nanoscale. We identify two different types of PDs by their contrasting behavior with temperature and measure their densities from 10¹⁴ cm^–3 to as high as 10¹⁶ cm^–3. Our CL images clearly illustrate the interplay between PDs and carrier dynamics in the well: increasing PD concentration severely limits carrier diffusion lengths, while a higher carrier density suppresses the nonradiative behavior of PDs. The results in this study are readily interpreted directly from CL images and represent a significant advancement in nanoscale PD analysis.

Abstract:

Current industrial production of ammonia from the Haber-Bosch process and its transport concomitantly produces a large quantity of CO2. Herein, we successfully synthesize inorganic-structure-based catalysts with [Fe-S2-Mo] motifs with a connecting structure similar to that of FeMoco (a cofactor of nitrogenase) by placing iron atoms on a single molecular layer of MoS2 at various loadings. This type of new catalytic material functionally mimics the nitrogenase to convert N2 to ammonia and hydrogen in water without adding any sacrificial agent under visible-light illumination. Using the elevated temperature boosts the ammonia yield and the energy efficiency by one order of magnitude. The solar-to-NH3 energy-conversion efficiency can be up to 0.24% at 270°C, which is the highest efficiency among all reported photocatalytic systems. This method of ammonia production and the photocatalytic materials may open up an exciting possibility for the decentralization of ammonia production for fertilizer provision to local farmlands using solar illumination.