Resonant Coherent Raman Scattering from WSe2.

Abstract

Low-dimensional transition-metal dichalcogenides (TMDs) continue to comprise a subject of intense research because of their unique optical and electronic properties that may be harnessed in modern devices. Intense photoluminescence (PL) from few-/monolayer TMDs rendered PL-based micro- and nanospectroscopic characterization ideal in the quest to understand the correlation between structure and function in these materials. Nonlinear optical methods are by comparison far less utilized for this purpose. In this work, we describe an approach based on electronically resonant four-wave-mixing that allows spatio-spectral characterization of excitons in monolayer WSe2. Due to the coherent nature of the response that we exploit to trace exciton resonances, and recent demonstrations of electronic four-wave-mixing-based nanoimaging and nanospectroscopy, our present work is an important step toward characterizing TMDs on the nano-femto scale using light.