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Title: Coupling-Assisted Renormalization of Excitons and Vibrations in Compressed MoSe2–WSe2 Heterostructure

Abstract

Vertical heterostructures (HSs) constructed with two-dimensional (2D) materials is expected to generate fascinating properties due to interlayer coupling between neighboring layers. However, interlayer coupling can be easily obscured by cross-contamination during transfer processes, rendering their experimental demonstration challenging. Here, we explore the coupling-assisted renormalization of excitons and vibrations in a mechanically fabricated MoSe2–WSe2 HS through high-pressure photoluminescence, Raman spectra, and density functional theory calculations. Accompanied by the interlayer coupling enhancement, the excitonic and vibrational renormalizations involving dimensionality and composition variations were achieved. A cycle of 2D–3D–2D excitonic evolution was disclosed and pressure-induced emergence of X exciton of MoSe2 in HS was found reflecting the band structure transition in the MoSe2–WSe2 HS. The Raman spectra reveals that the coupled A2" vibrations of WSe2 and MoSe2 in HS was stiffened and out-of-plane A1' vibrations of WSe2 and MoSe2 in HS got coherent upon pressure modulation. Here, this coupling-assisted renormalization in MoSe2–WSe2 HS can be extended to other 2D layered HSs, which indicates the possibility to design a flexible HS with controlled excitonic and vibrational system for light-emitting diodes, excitonic, and photovoltaic devices.

Authors:
 [1]; ORCiD logo [1];  [2];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. Jilin Univ., Changchun (China)
  2. Univ. of Texas, Austin, TX (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF); China Postdoctoral Science Foundation; National Natural Science Foundation of China (NSFC); National Basic Research Program of China
OSTI Identifier:
1434727
Grant/Contract Number:  
AC02-06CH11357; FG02-94ER14466; EAR-1634415; 2015M570265; 11574112; 11474127; 11274137; 2011CB808200
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 10; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; excitons; layered materials; oscillation; monolayers; energy

Citation Formats

Fu, Xinpeng, Li, Fangfei, Lin, Jung-Fu, Gong, Yuanbo, Huang, Xiaoli, Huang, Yanping, Gao, Hanxue, Zhou, Qiang, and Cui, Tian. Coupling-Assisted Renormalization of Excitons and Vibrations in Compressed MoSe2–WSe2 Heterostructure. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.8b01453.
Fu, Xinpeng, Li, Fangfei, Lin, Jung-Fu, Gong, Yuanbo, Huang, Xiaoli, Huang, Yanping, Gao, Hanxue, Zhou, Qiang, & Cui, Tian. Coupling-Assisted Renormalization of Excitons and Vibrations in Compressed MoSe2–WSe2 Heterostructure. United States. https://doi.org/10.1021/acs.jpcc.8b01453
Fu, Xinpeng, Li, Fangfei, Lin, Jung-Fu, Gong, Yuanbo, Huang, Xiaoli, Huang, Yanping, Gao, Hanxue, Zhou, Qiang, and Cui, Tian. Thu . "Coupling-Assisted Renormalization of Excitons and Vibrations in Compressed MoSe2–WSe2 Heterostructure". United States. https://doi.org/10.1021/acs.jpcc.8b01453. https://www.osti.gov/servlets/purl/1434727.
@article{osti_1434727,
title = {Coupling-Assisted Renormalization of Excitons and Vibrations in Compressed MoSe2–WSe2 Heterostructure},
author = {Fu, Xinpeng and Li, Fangfei and Lin, Jung-Fu and Gong, Yuanbo and Huang, Xiaoli and Huang, Yanping and Gao, Hanxue and Zhou, Qiang and Cui, Tian},
abstractNote = {Vertical heterostructures (HSs) constructed with two-dimensional (2D) materials is expected to generate fascinating properties due to interlayer coupling between neighboring layers. However, interlayer coupling can be easily obscured by cross-contamination during transfer processes, rendering their experimental demonstration challenging. Here, we explore the coupling-assisted renormalization of excitons and vibrations in a mechanically fabricated MoSe2–WSe2 HS through high-pressure photoluminescence, Raman spectra, and density functional theory calculations. Accompanied by the interlayer coupling enhancement, the excitonic and vibrational renormalizations involving dimensionality and composition variations were achieved. A cycle of 2D–3D–2D excitonic evolution was disclosed and pressure-induced emergence of X– exciton of MoSe2 in HS was found reflecting the band structure transition in the MoSe2–WSe2 HS. The Raman spectra reveals that the coupled A2" vibrations of WSe2 and MoSe2 in HS was stiffened and out-of-plane A1' vibrations of WSe2 and MoSe2 in HS got coherent upon pressure modulation. Here, this coupling-assisted renormalization in MoSe2–WSe2 HS can be extended to other 2D layered HSs, which indicates the possibility to design a flexible HS with controlled excitonic and vibrational system for light-emitting diodes, excitonic, and photovoltaic devices.},
doi = {10.1021/acs.jpcc.8b01453},
journal = {Journal of Physical Chemistry. C},
number = 10,
volume = 122,
place = {United States},
year = {Thu Feb 22 00:00:00 EST 2018},
month = {Thu Feb 22 00:00:00 EST 2018}
}

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Works referencing / citing this record:

Unusual Pressure‐Driven Phase Transformation and Band Renormalization in 2D vdW Hybrid Lead Halide Perovskites
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