Temperature-Dependent Electronic Ground-State Charge Transfer in van der Waals Heterostructures
Hakami, Marim A.
KAUST DepartmentMaterial Science and Engineering Program
Physical Science and Engineering (PSE) Division
Physical Sciences and Engineering King Abdullah University of Science and Technology Thuwal 23955-6900 Saudi Arabia
Permanent link to this recordhttp://hdl.handle.net/10754/668184
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AbstractElectronic 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.
CitationPark, S., Wang, H., Schultz, T., Shin, D., Ovsyannikov, R., Zacharias, M., … Koch, N. (2021). Temperature-Dependent Electronic Ground-State Charge Transfer in van der Waals Heterostructures. Advanced Materials, 2008677. doi:10.1002/adma.202008677
SponsorsThis work was funded by the Deutsche Forschungsgemeinschaft (DFG)—Projektnummer 182087777—SFB 951, AM 419/1-1, and by the JSPS KAKENHI under Grant No. JP18H03904. Further support by the National Research Foundation (NRF) of Korea under Grant No. 2018M3D1A1058793 and Technology Innovation Program (20012502), funded by the Korean Ministry of Trade, industry and Energy, is acknowledged. The authors thank the IMS and HZB for allocating synchrotron radiation beam time (UVSOR, BL7U and Bessy II, PM4). H.W. thanks Karen Fidanyan for assistance with the phonon calculations.
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