Reversible Electrical Control of Interfacial Charge Flow across van der Waals Interfaces

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....

ver descrição completa

Detalhes bibliográficos
Autores: Fu, Shuai|||0000-0003-4038-2384, Jia, Xiaoyu, Hassan, Aliaa S., Zhang, Heng|||0000-0002-5175-7367, Zheng, Wenhao, Gao, Lei, Di Virgilio, Lucia, Krasel, Sven|||0000-0003-1123-6556, Beljonne, David|||0000-0002-2989-3557, Tielrooij, Klaas-Jan|||0000-0002-0055-6231, Bonn, Mischa|||0000-0001-6851-8453, Wang, Hai I.|||0000-0003-0940-3984
Formato: artículo
Fecha de publicación:2023
País:España
Recursos:Universitat Autònoma de Barcelona
Repositorio:Dipòsit Digital de Documents de la UAB
Idioma:inglés
OAI Identifier:oai:ddd.uab.cat:281379
Acesso em linha:https://ddd.uab.cat/record/281379
https://dx.doi.org/urn:doi:10.1021/acs.nanolett.2c04795
Access Level:acceso abierto
Palavra-chave:Van der Waals heterostructures
Charge transfer
Photogating
Electrochemical gating
Operando terahertz spectroscopy
Descrição
Resumo: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-WS 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.