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Title: Rigid Band Shifts in Two-Dimensional Semiconductors through External Dielectric Screening

Abstract

In this work, we investigate the effects of external dielectric screening on the electronic dispersion and the band gap in the atomically thin, quasi-two-dimensional (2D) semiconductor WS 2 using angle-resolved photoemission and optical spectroscopies, along with first-principles calculations. We find the main effect of increased external dielectric screening to be a reduction of the quasiparticle band gap, with rigid shifts to the bands themselves. Specifically, the band gap of monolayer WS 2 is decreased by about 140 meV on a graphite substrate as compared to a hexagonal boron nitride substrate, while the electronic dispersion of WS 2 remains unchanged within our experimental precision of 17 meV. These essentially rigid shifts of the valence and conduction bands result from the special spatial structure of the changes in the Coulomb potential induced by the dielectric environment of the monolayer.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [4];  [5]; ORCiD logo [5];  [5];  [6]; ORCiD logo [6];  [5];  [4]; ORCiD logo [1]
  1. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry (TMF); Univ. of California, Berkeley, CA (United States)
  3. Radboud Univ., Nijmegen (Netherlands)
  4. Univ. of Bremen (Germany)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  6. National Inst. for Materials Science, Tsukuba, Ibaraki (Japan)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF); German Research Foundation (DFG); Ministry of Education, Culture, Sports, Science and Technology (MEXT) (Japan); Japan Society for the Promotion of Science (JSPS); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1596965
Report Number(s):
[arXiv: 1907.05535v1]
[Journal ID: ISSN 0031-9007; PRLTAO]
Grant/Contract Number:  
[AC02-76SF00515; AC02-05CH11231; GBMF4545; DMR-1708457; GRK-2247; JPMJCR15F3]
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
[ Journal Volume: 123; Journal Issue: 20]; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE

Citation Formats

Waldecker, Lutz, Raja, Archana, Rösner, Malte, Steinke, Christina, Bostwick, Aaron, Koch, Roland J., Jozwiak, Chris, Taniguchi, Takashi, Watanabe, Kenji, Rotenberg, Eli, Wehling, Tim O., and Heinz, Tony F. Rigid Band Shifts in Two-Dimensional Semiconductors through External Dielectric Screening. United States: N. p., 2019. Web. doi:10.1103/PhysRevLett.123.206403.
Waldecker, Lutz, Raja, Archana, Rösner, Malte, Steinke, Christina, Bostwick, Aaron, Koch, Roland J., Jozwiak, Chris, Taniguchi, Takashi, Watanabe, Kenji, Rotenberg, Eli, Wehling, Tim O., & Heinz, Tony F. Rigid Band Shifts in Two-Dimensional Semiconductors through External Dielectric Screening. United States. doi:10.1103/PhysRevLett.123.206403.
Waldecker, Lutz, Raja, Archana, Rösner, Malte, Steinke, Christina, Bostwick, Aaron, Koch, Roland J., Jozwiak, Chris, Taniguchi, Takashi, Watanabe, Kenji, Rotenberg, Eli, Wehling, Tim O., and Heinz, Tony F. Wed . "Rigid Band Shifts in Two-Dimensional Semiconductors through External Dielectric Screening". United States. doi:10.1103/PhysRevLett.123.206403.
@article{osti_1596965,
title = {Rigid Band Shifts in Two-Dimensional Semiconductors through External Dielectric Screening},
author = {Waldecker, Lutz and Raja, Archana and Rösner, Malte and Steinke, Christina and Bostwick, Aaron and Koch, Roland J. and Jozwiak, Chris and Taniguchi, Takashi and Watanabe, Kenji and Rotenberg, Eli and Wehling, Tim O. and Heinz, Tony F.},
abstractNote = {In this work, we investigate the effects of external dielectric screening on the electronic dispersion and the band gap in the atomically thin, quasi-two-dimensional (2D) semiconductor WS2 using angle-resolved photoemission and optical spectroscopies, along with first-principles calculations. We find the main effect of increased external dielectric screening to be a reduction of the quasiparticle band gap, with rigid shifts to the bands themselves. Specifically, the band gap of monolayer WS2 is decreased by about 140 meV on a graphite substrate as compared to a hexagonal boron nitride substrate, while the electronic dispersion of WS2 remains unchanged within our experimental precision of 17 meV. These essentially rigid shifts of the valence and conduction bands result from the special spatial structure of the changes in the Coulomb potential induced by the dielectric environment of the monolayer.},
doi = {10.1103/PhysRevLett.123.206403},
journal = {Physical Review Letters},
number = [20],
volume = [123],
place = {United States},
year = {2019},
month = {11}
}

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Works referenced in this record:

Large excitonic effects in monolayers of molybdenum and tungsten dichalcogenides
journal, September 2012


Theory of neutral and charged excitons in monolayer transition metal dichalcogenides
journal, July 2013

  • Berkelbach, Timothy C.; Hybertsen, Mark S.; Reichman, David R.
  • Physical Review B, Vol. 88, Issue 4
  • DOI: 10.1103/PhysRevB.88.045318

Optical Spectrum of MoS 2 : Many-Body Effects and Diversity of Exciton States
journal, November 2013


Tightly Bound Excitons in Monolayer WSe 2
journal, July 2014


Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS 2
journal, August 2014


Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
journal, August 2014

  • Ugeda, Miguel M.; Bradley, Aaron J.; Shi, Su-Fei
  • Nature Materials, Vol. 13, Issue 12
  • DOI: 10.1038/nmat4061

Probing excitonic dark states in single-layer tungsten disulphide
journal, August 2014

  • Ye, Ziliang; Cao, Ting; O’Brien, Kevin
  • Nature, Vol. 513, Issue 7517
  • DOI: 10.1038/nature13734

Colloquium : Excitons in atomically thin transition metal dichalcogenides
journal, April 2018


Two-Dimensional Heterojunctions from Nonlocal Manipulations of the Interactions
journal, March 2016


Probing the Influence of Dielectric Environment on Excitons in Monolayer WSe 2 : Insight from High Magnetic Fields
journal, October 2016


Coulomb engineering of the bandgap and excitons in two-dimensional materials
journal, May 2017

  • Raja, Archana; Chaves, Andrey; Yu, Jaeeun
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15251

Direct determination of monolayer MoS 2 and WSe 2 exciton binding energies on insulating and metallic substrates
journal, January 2018


A dielectric-defined lateral heterojunction in a monolayer semiconductor
journal, February 2019


Environmentally sensitive theory of electronic and optical transitions in atomically thin semiconductors
journal, January 2018


Dielectric disorder in two-dimensional materials
journal, August 2019


Tightly bound trions in monolayer MoS2
journal, December 2012

  • Mak, Kin Fai; He, Keliang; Lee, Changgu
  • Nature Materials, Vol. 12, Issue 3
  • DOI: 10.1038/nmat3505

The Computational 2D Materials Database: high-throughput modeling and discovery of atomically thin crystals
journal, September 2018


Wannier function approach to realistic Coulomb interactions in layered materials and heterostructures
journal, August 2015


Electronic excitations from a perturbative LDA + G d W approach
journal, November 2010


Band structure engineering in van der Waals heterostructures via dielectric screening: the GΔW method
journal, March 2017


Dielectric Genome of van der Waals Heterostructures
journal, June 2015


Giant spin-orbit-induced spin splitting in two-dimensional transition-metal dichalcogenide semiconductors
journal, October 2011


Nanoscale mapping of quasiparticle band alignment
journal, July 2019


Dielectric screening in two-dimensional insulators: Implications for excitonic and impurity states in graphane
journal, August 2011


Renormalization of Molecular Electronic Levels at Metal-Molecule Interfaces
journal, November 2006


Plasmons in graphite and stage-1 graphite intercalation compounds
journal, May 1997


Giant spin-splitting and gap renormalization driven by trions in single-layer WS2/h-BN heterostructures
journal, January 2018


Bandgap Engineering of Strained Monolayer and Bilayer MoS2
journal, July 2013

  • Conley, Hiram J.; Wang, Bin; Ziegler, Jed I.
  • Nano Letters, Vol. 13, Issue 8, p. 3626-3630
  • DOI: 10.1021/nl4014748