Temperature?Dependent Electronic Ground?State Charge Transfer in van der Waals Heterostructures

Electronic charge rearrangement between components of a heterostructure is the fundamental principle to reach electronic ground state. It acknowledged that density state distribution governs amount transfer, but notable dependence on temperature not yet considered, particularly for weakly interacting systems. Here, it experimentally observed ground-state transfer in van der Waals formed by monolayer MoS2 sandwiched graphite and molecular electron acceptor layer increases factor 3 when going from 7 K room temperature. State-of-the-art structure calculations full accounts nuclear thermal fluctuations reveal intracomponent electron–phonon coupling intercomponent as key factors determining transfer. This conclusion rationalized model applicable multicomponent heterostructures.