Title: Probing Transition Metal Dichalcogenides via Strain-Tuned and Polarization-Resolved Optical Spectroscopy
Description: The strong light-matter interaction in the atomically thin transition metal dichalcogenides (TMDCs) has allowed the use of optical spectroscopy to investigate these materials in great depth. It has been shown that optoelectronic properties of ultrathin TMDCs are remarkably different from their bulk counterparts. Among them, this dissertation focuses on ultrathin MoTe2 (molybdenum ditelluride) and ReS2 (rhenium disulfide). We first introduce the fundamental properties of the two material systems, MoTe2 and ReS2, investigated in this dissertation. Specific experimental methods for optical spectroscopy of 2D materials, 2D sample preparation, and related optics calculations are presented. Absorption and photoluminescence measurements are applied to demonstrate that semiconducting MoTe2, an indirect band gap bulk material, acquires a direct band gap in the monolayer limit. Furthermore, strain-tuned optical spectroscopy on MoTe2 shows that tensile strain can significantly redshift its optical gap and partially suppress the intervalley exciton-phonon scattering.

This suppression results in a narrowing of the near-band excitonic transitions. We also discuss the effect of strain on the transport properties of MoTe2 due to this reduction in scattering. We investigate monolayer ReS2 as a TMDC system exhibiting strong in-plane anisotropy. These properties are explored by polarization-resolved spectroscopy. We show how the accessible optical properties vary with optical polarization. We find that the near-band excitons in ultrathin ReS2, absorb and emit light along specific polarizations. We also show that purely non-contact, optical techniques can determine the crystallographic orientation of ReS2.