charge transfer; electrochemical gating; operando terahertz spectroscopy; photogating; van der Waals heterostructures; Charge flow; Electrical control; Interfacial charge; Operando; Two-dimensional; Van der Waal; Van der waal heterostructure; Bioengineering; Chemistry (all); Materials Science (all); Condensed Matter Physics; Mechanical Engineering; General Materials Science; General Chemistry
Abstract :
[en] Bond-free integration of two-dimensional (2D) materials yields van der Waals (vdW) heterostructures with exotic optical and electronic properties. Manipulating the splitting and recombination of photogenerated electron-hole pairs across the vdW interface is essential for optoelectronic applications. Previous studies have unveiled the critical role of defects in trapping photogenerated charge carriers to modulate the photoconductive gain for photodetection. However, the nature and role of defects in tuning interfacial charge carrier dynamics have remained elusive. Here, we investigate the nonequilibrium charge dynamics at the graphene-WS2 vdW interface under electrochemical gating by operando optical-pump terahertz-probe spectroscopy. We report full control over charge separation states and thus photogating field direction by electrically tuning the defect occupancy. Our results show that electron occupancy of the two in-gap states, presumably originating from sulfur vacancies, can account for the observed rich interfacial charge transfer dynamics and electrically tunable photogating fields, providing microscopic insights for optimizing optoelectronic devices.
Disciplines :
Chemistry
Author, co-author :
Fu, Shuai ; Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany
Jia, Xiaoyu; Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany
Hassan, Aliaa S; Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany
Zhang, Heng ; Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany
Zheng, Wenhao; Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany
Gao, Lei; Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany ; School of Physics and Key Laboratory of MEMS of the Ministry of Education, Southeast University, Nanjing 211189, China
Di Virgilio, Lucia; Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany
Krasel, Sven; Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany
Beljonne, David ; Université de Mons - UMONS > Faculté des Science > Service de Chimie des matériaux nouveaux
Tielrooij, Klaas-Jan ; Catalan Institute of Nanoscience and Nanotechnology (ICN2), BIST & CSIC, Campus UAB, Bellaterra, Barcelona 08193, Spain
Bonn, Mischa ; Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany
Wang, Hai I ; Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany
Language :
English
Title :
Reversible Electrical Control of Interfacial Charge Flow across van der Waals Interfaces.
R400 - Institut de Recherche en Science et Ingénierie des Matériaux Complexys
Funders :
Deutsche Forschungsgemeinschaft Johannes Gutenberg-Universit?t Mainz Horizon 2020 Framework Programme China Scholarship Council
Funding text :
We thank Jaco Geuchies, Yongkang Wang, Chao Zhu, Maksim Grechko, Heejae Kim, Sheng Qu, Jiabao Yang, Min Liu, Shuai Chen, Yunji Lee, Pushpendra Kumar, Arjan Houtepen and Samir Al-Hilfi for fruitful discussions. S.F. and L.G. acknowledge the fellowship support from China Scholarship Council (CSC). X.J. acknowledges the financial support by DFG through the Excellence Initiative by the Graduate School of Excellence Materials Science in Mainz (MAINZ) (GSC 266) and support from the Max Planck Graduate Center mit der Johannes Gutenberg-Universität Mainz (MPGC). K.J.T. acknowledges funding from the European Union’s Horizon 2020 research and innovation programme under Grant Agreement No. 804349 (ERC StG CUHL) and financial support through the MAINZ Visiting Professorship.Open access funded by Max Planck Society.
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