Photon-Electron Interactions in Graphene-Based Heterojunctions.

摘要

Graphene, a single layer of carbon atoms arranged in honeycomb lattice, has been one of the most attractive materials for fundamental and applied research in the past decade. Its unique electronic, optical, thermal, chemical and mechanical properties have lead to the discovery of new physics and many promising applications. In particular, research on photon-electron interaction in graphene-based heterojunctions has revealed a new route to design photoactive devices.;In this thesis, I present our work on the synthesis of graphene by chemical vapor deposition (CVD) and the study of graphene-based optoelectronic devices. In addition to the conventional synthesis of graphene on copper (Cu) foils, we also present the CVD synthesis of graphene on a new substrate: palladium (Pd). Especially, we performed detailed study of the nucleation, evolution and morphology of graphene growth on Pd substrate. It helps us to understand the growth reaction mechanism and achieve controllable synthesis of graphene from single layer to multiple layers with different morphologies. We then studied the broadband and ultrasensitive photocurrent and photovoltage response of graphene/silicon (Si) Schottky diodes. For the same architecture, we identified a new photoconductive mode with ultra high photoconductive gain, namely "quantum carrier reinvestment (QCR)". A gain exceeding 107 A/W was demonstrated. The underlying physics of photon-electron interactions in these junctions were studied by a combination of optical characterization tools including Raman spectroscopy, UV-Vis spectroscopy and scanning optical microscopy. The results obtained have been discussed in the framework of the unique electronic band structure, density states, and mobility of graphene, along with the manner in witch photoexcited carrier behave under various externally tuned parameters. We also systematically studied the optimization of performance of graphene/Si and thin transparent graphite/Si junction solar cells and demonstrated power conversion efficiency as high as 7.5%. Furthermore, other types of graphene/semiconductor junctions, e.g., graphene/ZnO and graphene/MoS2, were also studied. The solution processed graphene/ZnO heterojunctions have great potential for low-cost ultra violet photodetectors. The graphene/MoS2 is a new class of heterojunctions grown by van der Waals epitaxy, serving as a bridge connecting graphene and other 2D materials beyond graphene.