Electronic Origin of Optically-Induced Sub-Picosecond Lattice Dynamics in MoSe Monolayer.

Atomically thin layers of transition metal dichalcogenide (TMDC) semiconductors exhibit outstanding electronic and optical properties, with numerous applications such as valleytronics. While unusually rapid and efficient transfer of photoexcitation energy to atomic vibrations was found in recent experiments, its electronic origin remains unknown. Here, we study the lattice dynamics induced by electronic excitation in a model TMDC monolayer, MoSe, using nonadiabatic quantum molecular dynamics simulations.

Photo-induced lattice contraction in layered materials.

Structural and electronic changes induced by optical excitation is a promising technique for functionalization of 2D crystals. Characterizing the effect of excited electronic states on the in-plane covalent bonding network as well as the relatively weaker out-of-plane dispersion interactions is necessary to tune photo-response in these highly anisotropic crystal structures. In-plane atom dynamics was measured using pump-probe experiments and characterized using ab initio simulations, but the effect of electronic excitation on weak out-of-plane van der Waals bonds is less well-studied.