期刊
ADVANCED MATERIALS
卷 33, 期 29, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202008677
关键词
2D semiconductors; charge transfer; electron– phonon coupling; molecular dopants; MoS; (2); photoelectron spectroscopy
类别
资金
- Deutsche Forschungsgemeinschaft (DFG) [182087777-SFB 951, AM 419/1-1]
- JSPS KAKENHI [JP18H03904]
- National Research Foundation (NRF) of Korea [2018M3D1A1058793]
- Technology Innovation Program - Korean Ministry of Trade, industry and Energy [20012502]
- Projekt DEAL
- Korea Evaluation Institute of Industrial Technology (KEIT) [20012502] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
- National Research Foundation of Korea [2018M3D1A1058793] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
The study explores the electronic charge rearrangement principle in heterostructures and the impact of temperature on the amount of charge transfer. It is observed that the ground-state charge transfer increases by a factor of 3 when going from low temperature to room temperature in a specific heterostructure setup. Further electronic structure calculations and modeling identify electron-phonon coupling and electronic coupling as key factors determining the charge transfer quantity.
Electronic 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.
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