Characterization of Excitonic Nature in Raman Spectra Using Circularly Polarized Light.

Zhao, Yan; Zhang, Shishu; Shi, Yuping; Zhang, Yanfeng; Saito, Riichiro; Zhang, Jin; Tong, Lianming · ACS Nano · 2020

basic_science · Level V

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Abstract

We propose a technique of Raman spectroscopy to characterize the excitonic nature and to evaluate the relative contribution of the two kinds of electron/exciton-phonon interactions that are observed in two-dimensional transition-metal dichalcogenides (TMDCs). In the TMDCs, the electron/exciton-phonon interactions mainly originate from the deformation potential (DP) or the Fröhlich interaction (FI) which give the mutually different Raman tensors. Using a circularly polarized light, the relative proportion of the DP and the FI can be defined by the ratio of helicity-polarized intensity that is observed by MoS<sub>2</sub>. By this analysis, we show that the excitonic FI interaction gradually increases with decreasing temperature, contributes equally to DP at ∼230 K, and dominates at lower temperatures. The excitonic effect in the Raman spectra is confirmed by modulating the dielectric environment for the exciton and by changing the laser power.