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

Soohyung Park, Haiyuan Wang, Thorsten Schultz, Dongguen Shin, Ruslan Ovsyannikov, Marios Zacharias, Dmitrii Maksimov, Matthias Meissner, Yuri Hasegawa, Takuma Yamaguchi, Satoshi Kera, Areej Aljarb, Marim A. Hakami, Lain-Jong Li, Vincent Tung, Patrick Amsalem, Mariana Rossi, Norbert Koch

Research output: Contribution to journalArticlepeer-review

15 Scopus citations


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.
Original languageEnglish (US)
Pages (from-to)2008677
JournalAdvanced Materials
StatePublished - May 25 2021

Bibliographical note

KAUST Repository Item: Exported on 2021-05-27
Acknowledgements: This 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.

ASJC Scopus subject areas

  • Mechanics of Materials
  • General Materials Science
  • Mechanical Engineering


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