Optics and Optoelectronics of Two-dimensional Semiconducting Monolayers and Heterostructures
Ross, Jason Solomon
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Until recently, the physics of truly two-dimensional (2D) excitons could only be explored theoretically. Following the discovery of graphene, many 2D materials were quickly identified and isolated, one system being the semiconducting Group VI-B transition metal dichalcogenides (TMDs). These semiconductors are the first air-stable materials that are atomically thin (three atomics thick), and yet can be produced in arbitrarily large lateral sheets. They have a direct band gap in which confinement leads to large spatial overlap of electrons and holes resulting in strongly coupled excitonic transitions that dominate light-matter interactions. The direct band-gap of monolayer TMDs occurs at the corners of the hexagonal Brillouin zone, referred to as the K valleys. Entirely unique to these materials, excitons in adjacent K valleys selectively couple to light of opposite circular polarization, i.e. the K (K’) valley is selective to right (left) circularly polarized photons. This property offers the possible realization of novel devices that will manipulate the valley index, known as valleytronics. Further, creating a stacked heterostructure (HS) of two TMD monolayers of different molecular species can exhibit type-II band alignment leading to the first atomically sharp built-in p-n junction and a bright interlayer exciton with long lifetimes. Being flat 2D sheets, it is easy to couple these materials to nearby systems such as microfabricated electrodes and photonic crystal cavities allowing for unique modulation and device schemes. Here, I employ both optical and electronic techniques to study the unique physics of 2D excitons in TMDs as well as demonstrate some of their first optoelectronic and valleytronic devices. The most notable achievement is perhaps the first demonstrations of both atomically thin and 2D heterostructure light emitting diodes and photovoltaic devices. Other breakthroughs include the first demonstration of exciton charging tunability in a 2D system, the first valleytronic demonstration via electrical control of the degree of valley polarization, and resonant excitation investigations of the interlayer exciton’s role in absorption and emission in heterostructures. This work paves the way for future studies of 2D semiconducting systems and utilizing them in important new devices ranging from LEDs to photovoltaics to photonically coupled nanosystems such as a 2D nanolaser.