Two-dimensional coherent spectroscopy of monolayer transition metal dichalcogenides
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Two-dimensional semiconductors have long been studied for their unique optical and electronic properties, but with the work of Novoselov and Geim on van der Waals materials, two-dimensional semiconductors have seen a surge of renewed interest. This dissertation focuses on monolayer transition metal dichalcogenides (TMDCs), a class of two-dimensional materials that can easily be fabricated by mechanical exfoliation, much like graphene. In their bulk form, these materials have indirect band gaps, but transition to direct gap semiconductors in the monolayer limit. The band-edge optical response of TMDCs, like WSe₂ and MoS₂, is dominated by exciton absorption occurring at the ±K-points of the Brillouin zone. Because of the unique electronic structure of these materials, these two points form distinct valleys in the band structure which can be exploited to produce valley polarization. Exciton quantum dynamics are characterized by two fundamental parameters, one of which is the dephasing rate, γ, which describes quantum dissipation arising from the interaction of the excitons with their environment (i.e. other excitons, impurities, etc…). This dissertation focuses on measuring the fundamental property of dephasing time (which is inversely proportional to the dephasing rate and homogeneous linewidth) in monolayer WSe₂ through the use of two-dimensional coherent spectroscopy. Our measurements have revealed a homogeneous linewidth consistent with dephasing times in the sub-picosecond regime. We also characterize the role of exciton-exciton and exciton-phonon interactions, on the homogeneous linewidth, through excitation density and temperature dependent studies. These studies have revealed strong many-body effects and nonradiative population relaxation as the primary dephasing mechanisms. Microscopic calculations show that in perfect crystalline samples of monolayer TMDCs, the radiative lifetimes are also in the sub-picosecond regime due to the large oscillator strengths inherent in these materials. This result is consistent with the short dephasing times found experimentally.