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Title: Evolution of interlayer coupling in twisted molybdenum disulfide bilayers

Abstract

Van der Waals (vdW) coupling is emerging as a powerful method to engineer and tailor physical properties of atomically thin two-dimensional (2D) materials. In graphene/graphene and graphene/boron-nitride structures it leads to interesting physical phenomena ranging from new van Hove singularities and Fermi velocity renormalization to unconventional quantum Hall effects and Hofstadter's butterfly pattern. 2D transition metal dichalcogenides (TMDCs), another system of predominantly vdW-coupled atomically thin layers can also exhibit interesting but different coupling phenomena because TMDCs can be direct or indirect bandgap semiconductors. Here, we present the first study on the evolution of interlayer coupling with twist angles in as-grown MoS 2 bilayers. We find that an indirect bandgap emerges in bilayers with any stacking configuration, but the bandgap size varies appreciably with the twist angle: it shows the largest redshift for AA- and AB-stacked bilayers, and a significantly smaller but constant redshift for all other twist angles. The vibration frequency of the out-of-plane phonon in MoS 2 shows similar twist angle dependence. Furthermore, our observations, together with ab initio calculations, reveal that this evolution of interlayer coupling originates from the repulsive steric effects, which leads to different interlayer separations between the two MoS 2 layers in different stacking configurations.

Authors:
 [1];  [2];  [3];  [2];  [3];  [4];  [3];  [3];  [3];  [3]
  1. Univ. of California, Berkeley, CA (United States); Peking Univ., Beijing (China)
  2. Univ. of California, Berkeley, CA (United States)
  3. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1494115
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 5; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Liu, Kaihui, Zhang, Liming, Cao, Ting, Jin, Chenhao, Qiu, Diana, Zhou, Qin, Zettl, Alex, Yang, Peidong, Louie, Steve G., and Wang, Feng. Evolution of interlayer coupling in twisted molybdenum disulfide bilayers. United States: N. p., 2014. Web. doi:10.1038/ncomms5966.
Liu, Kaihui, Zhang, Liming, Cao, Ting, Jin, Chenhao, Qiu, Diana, Zhou, Qin, Zettl, Alex, Yang, Peidong, Louie, Steve G., & Wang, Feng. Evolution of interlayer coupling in twisted molybdenum disulfide bilayers. United States. doi:10.1038/ncomms5966.
Liu, Kaihui, Zhang, Liming, Cao, Ting, Jin, Chenhao, Qiu, Diana, Zhou, Qin, Zettl, Alex, Yang, Peidong, Louie, Steve G., and Wang, Feng. Thu . "Evolution of interlayer coupling in twisted molybdenum disulfide bilayers". United States. doi:10.1038/ncomms5966. https://www.osti.gov/servlets/purl/1494115.
@article{osti_1494115,
title = {Evolution of interlayer coupling in twisted molybdenum disulfide bilayers},
author = {Liu, Kaihui and Zhang, Liming and Cao, Ting and Jin, Chenhao and Qiu, Diana and Zhou, Qin and Zettl, Alex and Yang, Peidong and Louie, Steve G. and Wang, Feng},
abstractNote = {Van der Waals (vdW) coupling is emerging as a powerful method to engineer and tailor physical properties of atomically thin two-dimensional (2D) materials. In graphene/graphene and graphene/boron-nitride structures it leads to interesting physical phenomena ranging from new van Hove singularities and Fermi velocity renormalization to unconventional quantum Hall effects and Hofstadter's butterfly pattern. 2D transition metal dichalcogenides (TMDCs), another system of predominantly vdW-coupled atomically thin layers can also exhibit interesting but different coupling phenomena because TMDCs can be direct or indirect bandgap semiconductors. Here, we present the first study on the evolution of interlayer coupling with twist angles in as-grown MoS2 bilayers. We find that an indirect bandgap emerges in bilayers with any stacking configuration, but the bandgap size varies appreciably with the twist angle: it shows the largest redshift for AA- and AB-stacked bilayers, and a significantly smaller but constant redshift for all other twist angles. The vibration frequency of the out-of-plane phonon in MoS2 shows similar twist angle dependence. Furthermore, our observations, together with ab initio calculations, reveal that this evolution of interlayer coupling originates from the repulsive steric effects, which leads to different interlayer separations between the two MoS2 layers in different stacking configurations.},
doi = {10.1038/ncomms5966},
journal = {Nature Communications},
issn = {2041-1723},
number = 1,
volume = 5,
place = {United States},
year = {2014},
month = {9}
}

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