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Title: Photocarrier generation from interlayer charge-transfer transitions in WS 2-graphene heterostructures

Abstract

Efficient interfacial carrier generation in van der Waals heterostructures is critical for their electronic and optoelectronic applications. We demonstrate broadband photocarrier generation in WS 2-graphene heterostructures by imaging interlayer coupling–dependent charge generation using ultrafast transient absorption microscopy. Interlayer charge-transfer (CT) transitions and hot carrier injection from graphene allow carrier generation by excitation as low as 0.8 eV below the WS 2 bandgap. The experimentally determined interlayer CT transition energies are consistent with those predicted from the first-principles band structure calculation. CT interactions also lead to additional carrier generation in the visible spectral range in the heterostructures compared to that in the single-layer WS 2 alone. The lifetime of the charge-separated states is measured to be ~1 ps. These results suggest that interlayer interactions make graphene–two-dimensional semiconductor heterostructures very attractive for photovoltaic and photodetector applications because of the combined benefits of high carrier mobility and enhanced broadband photocarrier generation.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Purdue Univ., West Lafayette, IN (United States)
  2. Universität Leipzig (Germany); Jacobs University Bremen (Germany)
Publication Date:
Research Org.:
Purdue Univ., West Lafayette, IN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1499923
Grant/Contract Number:  
SC0016356
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 4; Journal Issue: 2; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Yuan, Long, Chung, Ting-Fung, Kuc, Agnieszka, Wan, Yan, Xu, Yang, Chen, Yong P., Heine, Thomas, and Huang, Libai. Photocarrier generation from interlayer charge-transfer transitions in WS2-graphene heterostructures. United States: N. p., 2018. Web. doi:10.1126/sciadv.1700324.
Yuan, Long, Chung, Ting-Fung, Kuc, Agnieszka, Wan, Yan, Xu, Yang, Chen, Yong P., Heine, Thomas, & Huang, Libai. Photocarrier generation from interlayer charge-transfer transitions in WS2-graphene heterostructures. United States. doi:10.1126/sciadv.1700324.
Yuan, Long, Chung, Ting-Fung, Kuc, Agnieszka, Wan, Yan, Xu, Yang, Chen, Yong P., Heine, Thomas, and Huang, Libai. Fri . "Photocarrier generation from interlayer charge-transfer transitions in WS2-graphene heterostructures". United States. doi:10.1126/sciadv.1700324. https://www.osti.gov/servlets/purl/1499923.
@article{osti_1499923,
title = {Photocarrier generation from interlayer charge-transfer transitions in WS2-graphene heterostructures},
author = {Yuan, Long and Chung, Ting-Fung and Kuc, Agnieszka and Wan, Yan and Xu, Yang and Chen, Yong P. and Heine, Thomas and Huang, Libai},
abstractNote = {Efficient interfacial carrier generation in van der Waals heterostructures is critical for their electronic and optoelectronic applications. We demonstrate broadband photocarrier generation in WS2-graphene heterostructures by imaging interlayer coupling–dependent charge generation using ultrafast transient absorption microscopy. Interlayer charge-transfer (CT) transitions and hot carrier injection from graphene allow carrier generation by excitation as low as 0.8 eV below the WS2 bandgap. The experimentally determined interlayer CT transition energies are consistent with those predicted from the first-principles band structure calculation. CT interactions also lead to additional carrier generation in the visible spectral range in the heterostructures compared to that in the single-layer WS2 alone. The lifetime of the charge-separated states is measured to be ~1 ps. These results suggest that interlayer interactions make graphene–two-dimensional semiconductor heterostructures very attractive for photovoltaic and photodetector applications because of the combined benefits of high carrier mobility and enhanced broadband photocarrier generation.},
doi = {10.1126/sciadv.1700324},
journal = {Science Advances},
number = 2,
volume = 4,
place = {United States},
year = {2018},
month = {2}
}

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