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Optical dynamics in van der Waals heterobilayers is of fundamental scientificand practical interest. Based on a time-dependent adiabatic GW approach, wediscover a new many-electron (excitonic) channel for converting photoexcitedintralayer to interlayer excitations and the associated ultrafast opticalresponses in heterobilayers, which is conceptually different from theconventional single-particle picture. We find strong electron-hole interactionsdrive the dynamics and enhance the pump-probe optical responses by an order ofmagnitude with a rise time of ~300 fs in MoSe$_2$/WSe$_2$ heterobilayers, inagreement with experiment.

Excitonic interactions and mechanism for ultrafast interlayer photoexcited response in van der Waals heterostructures