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The optical properties of the two-dimensional (2D) crystals are dominated bytightly bound electron-hole pairs (excitons) and lattice vibration modes(phonons). The exciton-phonon interaction is fundamentally important tounderstand the optical properties of 2D materials and thus help developemerging 2D crystal based optoelectronic devices. Here, we presented theexcitonic resonant Raman scattering (RRS) spectra of few-layer WS$_2$ excitedby 11 lasers lines covered all of A, B and C exciton transition energies atdifferent sample temperatures from 4 to 300 K. As a result, we are not onlyable to probe the forbidden phonon modes unobserved in ordinary Ramanscattering, but also can determine the bright and dark state fine structures of1s A exciton. In particular, we also observed the quantum interference betweenlow-energy discrete phonon and exciton continuum under resonant excitation. Ourworks pave a way to understand the exciton-phonon coupling and many-bodyeffects in 2D materials.

Observation of forbidden phonons and dark excitons by resonance Raman scattering in few-layer WS$_2$