Optoelectronics of graphene-based Van der Waals heterostructures

Abstract

Research on van der Waals (vdW) materials (homo- or hetero-) is a rapidly emerging field in condensed matter physics. They are layered structures with strong chemical bonding within layers and relatively weak van der Waals force to combine layers together. This unique layer-bylayer nature makes it easy to exfoliate layers out and at the same time to re-assemble in arbitrary sequences with different combinations. The versatility, flexibility, and relatively low cost of production make the scientific community enthusiastic about their future. In this thesis, I investigate the fundamental physical processes of light-matter interactions in these layered structures, including graphene, boron nitride, transition metal dichalcogenides and heterostructures formed from these materials. My research involves state-of-the-art nanoscale fabrication and microscale photocurrent spectroscopy and imaging. In Chapter 1, 1 will briefly discuss basic physical properties of the vdW materials involved in this thesis and introduce the main nanofabrication and measurement techniques. Chapter 2-4 are about hot electron dynamics and electron-phonon coupling in intrinsic graphene systems, among which Chapter 2 is focusing on the generation mechanism of the photocurrent at the p-n interface, which is demonstrated to have a photothermoelectric origin. This indicates a weak electron-phonon coupling strength in graphene. Chapter 3 is a direct experimental follow-up of the work in Chapter 2 and reveals the dominant electron-phonon coupling mechanism at different temperature and doping regimes. In Chapter 4, I present the observation of anomalous geometric photocurrent patterns in various devices at the charge neutral point. The spatial pattern can be understood as a local photo-generated current near edges being collected by remote electrodes. The anomalous behavior as functions of change density and temperature indicates an interesting regime of energy and charge dynamics. In Chapter 5 and 6, 1 will show the photoresponse of graphene-BN heterostuctures. In graphene-BN stack directly on SiO₂, we observed strong photo-induced doping phenomenon, which can be understood as charge transfer from graphene across BN and eventually trapped at the interface between BN and SiO₂. By inserting another layer of graphene between BN and SiO₂ , we can measure an electrical current after photoexcitation due to such charge transfer. We further studied the competition between this vertical charge transfer and in-plane carrier-carrier scattering in different regimes. In Chapter 7, I will briefly summarize collaborated work with Prof. Dimitri Basov's group on near-field imaging of surface polariton in two-dimensional materials. This technique provides a complementary tool to examine the intriguing light-matter interaction (for large momentum excitations) in low-dimensional materials. Chapter 8 is the outlook, from my own point of view, what more can be done following this thesis.