Twist-Angle-Dependent Ultrafast Charge Transfer in MoS2-Graphene van der Waals Heterostructures

Luo, Duan; Tang, Jian; Shen, Xiaozhe; Ji, Fuhao; Yang, Jie; Weathersby, Stephen; Kozina, Michael E.; Chen, Zhijiang; Xiao, Jun; Ye, Yusen; Cao, Ting; Zhang, Guangyu; Wang, Xijie; Lindenberg, Aaron M.

doi:10.1021/acs.nanolett.1c02356

Title: Twist-Angle-Dependent Ultrafast Charge Transfer in MoS₂-Graphene van der Waals Heterostructures

Journal Article · 16 September 2021 · Nano Letters

DOI: https://doi.org/10.1021/acs.nanolett.1c02356 · OSTI ID:1873515

^[1]; Tang, Jian ^[2]; Shen, Xiaozhe ^[3]; Ji, Fuhao ^[3]; Yang, Jie ^[3]; Weathersby, Stephen ^[3]; Kozina, Michael E. ^[3]; Chen, Zhijiang ^[3]; Xiao, Jun ^[1]; Ye, Yusen ^[4];

^[4]; Zhang, Guangyu ^[2]; Wang, Xijie ^[3];

^[1]

Stanford University, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Chinese Academy of Sciences (CAS), Beijing (China)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
University of Washington, Seattle, WA (United States)

Vertically stacked transition metal dichalcogenide-graphene heterostructures provide a platform for novel optoelectronic applications with high photoresponse speeds. Photoinduced nonequilibrium carrier and lattice dynamics in such heterostructures underlie these applications but have not been understood. In particular, the dependence of these photoresponses on the twist angle, a key tuning parameter, remains elusive. Here, using ultrafast electron diffraction, we report the simultaneous visualization of charge transfer and electron–phonon coupling in MoS₂-graphene heterostructures with different stacking configurations. We find that the charge transfer timescale from MoS₂ to graphene varies strongly with twist angle, becoming faster for smaller twist angles, and show that the relaxation timescale is significantly shorter in a heterostructure as compared to a monolayer. These findings illustrate that twist angle constitutes an additional tuning knob for interlayer charge transfer in heterobilayers and deepen our understanding of fundamental photophysical processes in heterostructures, of importance for future applications in optoelectronics and light harvesting.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Natural Science Foundation of China; Strategic Priority Research Program of Chinese Academy of Sciences

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1873515

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 19 Vol. 21; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Twist-Angle-Dependent Ultrafast Charge Transfer in MoS₂-Graphene van der Waals Heterostructures