Quantum Interference Effects in Resonant Raman Spectroscopy of Single- and Triple-Layer MoTe<sub>2</sub> from First-Principles.

Miranda, Henrique P C; Reichardt, Sven; Froehlicher, Guillaume; Molina-Sánchez, Alejandro; Berciaud, Stéphane; Wirtz, Ludger · Nano Lett · 2017

basic_science · Level V

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Abstract

We present a combined experimental and theoretical study of resonant Raman spectroscopy in single- and triple-layer MoTe<sub>2</sub>. Raman intensities are computed entirely from first-principles by calculating finite differences of the dielectric susceptibility. In our analysis, we investigate the role of quantum interference effects and the electron-phonon coupling. With this method, we explain the experimentally observed intensity inversion of the A<sub>1</sub><sup>'</sup> vibrational modes in triple-layer MoTe<sub>2</sub> with increasing laser photon energy. Finally, we show that a quantitative comparison with experimental data requires the proper inclusion of excitonic effects.