Quantum Interference Effects in Resonant Raman Spectroscopy of Single- and Triple-Layer MoTe₂ from First-Principles

We present a combined experimental and theoretical study of resonant Raman spectroscopy in single- and triple-layer MoTe 2 . 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 1 ′ vibrational modes in triple-layer MoTe 2 with increasing laser photon energy. Finally, we show that a quantitative comparison with experimental data requires the proper inclusion of excitonic effects.