First-Principles Nonequilibrium Green’s Function Approach to Energy Conversion in Nanoscale Optoelectronics

• DOI: 10.1021/acs.jctc.2c00547
• Publication Date: 2022-08-25T11:54:06Z
• Authors: Xiaoyan Wu; Rulin Wang; Hao Zou; Bowen Song; Shizheng Wen; Thomas Frauenheim; ChiYung Yam
• Keywords: 02 engineering and technology; 0210 nano-technology; 7. Clean energy

Understanding photon-electron conversion on the nanoscale is essential for future innovations in nano-optoelectronics. In this article, based nonequilibrium Green's function (NEGF) formalism, we develop a quantum-mechanical method modeling energy optoelectronic devices. The allows us to study photoinduced charge transport and electroluminescence processes realistic First, investigate properties of two-level model with two different treatments inelastic scatterings. We show regime where self-consistency between electron photon important correct description then applied single-molecule junctions density-functional tight-binding approach. predicted emission spectra are found be very good agreement experimental measurements. For nanostructured materials, further photoresponse two-dimensional graphene/graphite-C3N4 heterojunction photovoltaic device. simulations demonstrate clearly impact atomistic details nanodevices. This work provides practical theoretical framework that can design