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

Abstract

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.

Authors:
ORCiD logo [1];  [2];  [3];  [3];  [3];  [3];  [3];  [3];  [1];  [4]; ORCiD logo [4];  [2];  [3]; ORCiD logo [1]
  1. Stanford University, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Chinese Academy of Sciences (CAS), Beijing (China)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. University of Washington, Seattle, WA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Natural Science Foundation of China (NSFC); Strategic Priority Research Program of Chinese Academy of Sciences
OSTI Identifier:
1873515
Grant/Contract Number:  
AC02-76SF00515; 61888102; 11834017; XDB30000000
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 21; Journal Issue: 19; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; van der Waals heterostructures; charge transfer; electron−phonon coupling; structural dynamics; ultrafast electron diffraction

Citation Formats

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, and Lindenberg, Aaron M. Twist-Angle-Dependent Ultrafast Charge Transfer in MoS2-Graphene van der Waals Heterostructures. United States: N. p., 2021. Web. doi:10.1021/acs.nanolett.1c02356.
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. Twist-Angle-Dependent Ultrafast Charge Transfer in MoS2-Graphene van der Waals Heterostructures. United States. https://doi.org/10.1021/acs.nanolett.1c02356
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, and Lindenberg, Aaron M. Thu . "Twist-Angle-Dependent Ultrafast Charge Transfer in MoS2-Graphene van der Waals Heterostructures". United States. https://doi.org/10.1021/acs.nanolett.1c02356. https://www.osti.gov/servlets/purl/1873515.
@article{osti_1873515,
title = {Twist-Angle-Dependent Ultrafast Charge Transfer in MoS2-Graphene van der Waals Heterostructures},
author = {Luo, Duan and Tang, Jian and Shen, Xiaozhe and Ji, Fuhao and Yang, Jie and Weathersby, Stephen and Kozina, Michael E. and Chen, Zhijiang and Xiao, Jun and Ye, Yusen and Cao, Ting and Zhang, Guangyu and Wang, Xijie and Lindenberg, Aaron M.},
abstractNote = {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.},
doi = {10.1021/acs.nanolett.1c02356},
journal = {Nano Letters},
number = 19,
volume = 21,
place = {United States},
year = {Thu Sep 16 00:00:00 EDT 2021},
month = {Thu Sep 16 00:00:00 EDT 2021}
}

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