Park, SoohyungWang, HaiyuanSchultz, ThorstenShin, DongguenOvsyannikov, RuslanZacharias, MariosMaksimov, DmitriiMeissner, MatthiasHasegawa, YuriYamaguchi, TakumaKera, SatoshiAljarb, AreejHakami, MariamLi, Lain-JongTung, VincentAmsalem, PatrickRossi, MarianaKoch, Norbert2021-06-052021-06-052021-06-052021-05-2510.1002/adma.202008677https://infoscience.epfl.ch/handle/20.500.14299/178671WOS:000653748100001Electronic charge rearrangement between components of a heterostructure is the fundamental principle to reach the electronic ground state. It is acknowledged that the density of state distribution of the components governs the amount of charge transfer, but a notable dependence on temperature is not yet considered, particularly for weakly interacting systems. Here, it is experimentally observed that the amount of ground-state charge transfer in a van der Waals heterostructure formed by monolayer MoS2 sandwiched between graphite and a molecular electron acceptor layer increases by a factor of 3 when going from 7 K to room temperature. State-of-the-art electronic structure calculations of the full heterostructure that accounts for nuclear thermal fluctuations reveal intracomponent electron-phonon coupling and intercomponent electronic coupling as the key factors determining the amount of charge transfer. This conclusion is rationalized by a model applicable to multicomponent van der Waals heterostructures.Chemistry, MultidisciplinaryChemistry, PhysicalNanoscience & NanotechnologyMaterials Science, MultidisciplinaryPhysics, AppliedPhysics, Condensed MatterChemistryScience & Technology - Other TopicsMaterials SciencePhysics2d semiconductorscharge transferelectron&#8211phonon couplingmolecular dopantsmos(2)photoelectron spectroscopyhybrid functionalsmonolayer mos2semiconductorsbandgapsurfaceimpactenergyatomtext::journal::journal article::research article