skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Theory of optical absorption by interlayer excitons in transition metal dichalcogenide heterobilayers

Abstract

In this paper, we present a theory of optical absorption by interlayer excitons in a heterobilayer formed from transition metal dichalcogenides. The theory accounts for the presence of small relative rotations that produce a momentum shift between electron and hole bands located in different layers, and a moire pattern in real space. Because of the momentum shift, the optically active interlayer excitons are located at the moire Brillouin zone's corners, instead of at its center, and would have elliptical optical selection rules if the individual layers were translationally invariant. We show that the exciton moire potential energy restores circular optical selection rules by coupling excitons with different center of mass momenta. A variety of interlayer excitons with both senses of circular optical activity, and energies that are tunable by twist angle, are present at each valley. The lowest energy exciton states are generally localized near the exciton potential energy minima. Finally, we discuss the possibility of using the moire pattern to achieve scalable two-dimensional arrays of nearly identical quantum dots.

Authors:
 [1];  [2];  [2]
+ Show Author Affiliations
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  2. Univ. of Texas, Austin, TX (United States). Department of Physics
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; U.S. Army Research Laboratory - U.S. Army Research Office (ARO); Welch Foundation; USDOE
OSTI Identifier:
1419946
Alternate Identifier(s):
OSTI ID: 1417696
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 97; Journal Issue: 3; Journal ID: ISSN 2469-9950
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

Wu, Fengcheng, Lovorn, Timothy, and MacDonald, A. H. Theory of optical absorption by interlayer excitons in transition metal dichalcogenide heterobilayers. United States: N. p., 2018. Web. doi:10.1103/PhysRevB.97.035306.
Copy to clipboard
Wu, Fengcheng, Lovorn, Timothy, & MacDonald, A. H. Theory of optical absorption by interlayer excitons in transition metal dichalcogenide heterobilayers. United States. doi:10.1103/PhysRevB.97.035306.
Copy to clipboard
Wu, Fengcheng, Lovorn, Timothy, and MacDonald, A. H. Mon . "Theory of optical absorption by interlayer excitons in transition metal dichalcogenide heterobilayers". United States. doi:10.1103/PhysRevB.97.035306. https://www.osti.gov/servlets/purl/1419946.
Copy to clipboard
@article{osti_1419946,
title = {Theory of optical absorption by interlayer excitons in transition metal dichalcogenide heterobilayers},
author = {Wu, Fengcheng and Lovorn, Timothy and MacDonald, A. H.},
abstractNote = {In this paper, we present a theory of optical absorption by interlayer excitons in a heterobilayer formed from transition metal dichalcogenides. The theory accounts for the presence of small relative rotations that produce a momentum shift between electron and hole bands located in different layers, and a moire pattern in real space. Because of the momentum shift, the optically active interlayer excitons are located at the moire Brillouin zone's corners, instead of at its center, and would have elliptical optical selection rules if the individual layers were translationally invariant. We show that the exciton moire potential energy restores circular optical selection rules by coupling excitons with different center of mass momenta. A variety of interlayer excitons with both senses of circular optical activity, and energies that are tunable by twist angle, are present at each valley. The lowest energy exciton states are generally localized near the exciton potential energy minima. Finally, we discuss the possibility of using the moire pattern to achieve scalable two-dimensional arrays of nearly identical quantum dots.},
doi = {10.1103/PhysRevB.97.035306},
journal = {Physical Review B},
issn = {2469-9950},
number = 3,
volume = 97,
place = {United States},
year = {2018},
month = {1}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI:  10.1103/PhysRevB.97.035306
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 23 works
Citation information provided by
Web of Science

Figures / Tables:

FIG. 1 FIG. 1: (a) Illustration of AA stacking with a small twist angle θ and an in-plane displacement r0. The blue and red hexagons mark the Wigner-Seitz cells of the two layers. (b) The corresponding illustration of AB stacking. AA and AB stacking are distinguished by a rotation of of themore » top layer (MoX2) by π around the metal (Mo) axis. (c) Unit cell of the bilayer when θ = 0. The vectors r0,n in this figure are high symmetry points as discussed in the main text. (d) Brillouin zone and the first shell reciprocal lattice vectors for the bilayer with θ = 0. (e) Brillouin zones associated with the top and bottom layers in a twisted bilayer.« less
All figures and tables (6 total)
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Coupled Spin and Valley Physics in Monolayers of MoS 2 and Other Group-VI Dichalcogenides
journal, May 2012

Exciton fine structure and spin decoherence in monolayers of transition metal dichalcogenides
journal, May 2014

An updated version of wannier90: A tool for obtaining maximally-localised Wannier functions
journal, August 2014

  • Mostofi, Arash A.; Yates, Jonathan R.; Pizzi, Giovanni
  • Computer Physics Communications, Vol. 185, Issue 8
  • DOI: 10.1016/j.cpc.2014.05.003

Tunable moiré bands and strong correlations in small-twist-angle bilayer graphene
journal, March 2017

  • Kim, Kyounghwan; DaSilva, Ashley; Huang, Shengqiang
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 13
  • DOI: 10.1073/pnas.1620140114

Spin and pseudospins in layered transition metal dichalcogenides
journal, April 2014

  • Xu, Xiaodong; Yao, Wang; Xiao, Di
  • Nature Physics, Vol. 10, Issue 5
  • DOI: 10.1038/nphys2942

Two-Step Growth of Two-Dimensional WSe 2 /MoSe 2 Heterostructures
journal, August 2015

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

  • Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
  • Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
  • DOI: 10.1088/0953-8984/21/39/395502

Boson localization and the superfluid-insulator transition
journal, July 1989

  • Fisher, Matthew P. A.; Weichman, Peter B.; Grinstein, G.
  • Physical Review B, Vol. 40, Issue 1
  • DOI: 10.1103/PhysRevB.40.546

Valley-polarized exciton dynamics in a 2D semiconductor heterostructure
journal, February 2016

Valley-selective optical Stark effect in monolayer WS2
journal, December 2014

  • Sie, Edbert J.; McIver, James W.; Lee, Yi-Hsien
  • Nature Materials, Vol. 14, Issue 3
  • DOI: 10.1038/nmat4156

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

Large, valley-exclusive Bloch-Siegert shift in monolayer WS 2
journal, March 2017

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

Moiré assisted fractional quantum Hall state spectroscopy
journal, December 2016

Anomalous Light Cones and Valley Optical Selection Rules of Interlayer Excitons in Twisted Heterobilayers
journal, October 2015

The valley Hall effect in MoS2 transistors
journal, June 2014

Evolution of interlayer coupling in twisted molybdenum disulfide bilayers
journal, September 2014

  • Liu, Kaihui; Zhang, Liming; Cao, Ting
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5966

Valley-selective circular dichroism of monolayer molybdenum disulphide
journal, January 2012

  • Cao, Ting; Wang, Gang; Han, Wenpeng
  • Nature Communications, Vol. 3, Issue 1
  • DOI: 10.1038/ncomms1882

Tunable Exciton Funnel Using Moiré Superlattice in Twisted van der Waals Bilayer
journal, August 2014

  • Wu, Menghao; Qian, Xiaofeng; Li, Ju
  • Nano Letters, Vol. 14, Issue 9
  • DOI: 10.1021/nl502414t

Dirac cones and Dirac saddle points of bright excitons in monolayer transition metal dichalcogenides
journal, May 2014

  • Yu, Hongyi; Liu, Gui-Bin; Gong, Pu
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4876

Theory of two-dimensional spatially indirect equilibrium exciton condensates
journal, October 2015

Topological Exciton Bands in Moiré Heterojunctions
journal, April 2017

Interlayer couplings, Moiré patterns, and 2D electronic superlattices in MoS 2 /WSe 2 hetero-bilayers
journal, January 2017

Moiré excitons: From programmable quantum emitter arrays to spin-orbit–coupled artificial lattices
journal, November 2017

Tightly Bound Excitons in Monolayer WSe 2
journal, July 2014

Gaps induced by inversion symmetry breaking and second-generation Dirac cones in graphene/hexagonal boron nitride
journal, August 2016

  • Wang, Eryin; Lu, Xiaobo; Ding, Shijie
  • Nature Physics, Vol. 12, Issue 12
  • DOI: 10.1038/nphys3856

Hofstadter’s butterfly and the fractal quantum Hall effect in moiré superlattices
journal, May 2013

Directional interlayer spin-valley transfer in two-dimensional heterostructures
journal, December 2016

  • Schaibley, John R.; Rivera, Pasqual; Yu, Hongyi
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms13747

Vertical and in-plane heterostructures from WS2/MoS2 monolayers
journal, September 2014

  • Gong, Yongji; Lin, Junhao; Wang, Xingli
  • Nature Materials, Vol. 13, Issue 12, p. 1135-1142
  • DOI: 10.1038/nmat4091

Cloning of Dirac fermions in graphene superlattices
journal, May 2013

  • Ponomarenko, L. A.; Gorbachev, R. V.; Yu, G. L.
  • Nature, Vol. 497, Issue 7451
  • DOI: 10.1038/nature12187

Ising pairing in superconducting NbSe2 atomic layers
journal, November 2015

  • Xi, Xiaoxiang; Wang, Zefang; Zhao, Weiwei
  • Nature Physics, Vol. 12, Issue 2
  • DOI: 10.1038/nphys3538

High-temperature superfluidity with indirect excitons in van der Waals heterostructures
journal, July 2014

  • Fogler, M. M.; Butov, L. V.; Novoselov, K. S.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5555

Exciton band structure of monolayer MoS 2
journal, February 2015

Ultrafast charge transfer in atomically thin MoS2/WS2 heterostructures
journal, August 2014

  • Hong, Xiaoping; Kim, Jonghwan; Shi, Su-Fei
  • Nature Nanotechnology, Vol. 9, Issue 9
  • DOI: 10.1038/nnano.2014.167

Moire bands in twisted double-layer graphene
journal, July 2011

  • Bistritzer, R.; MacDonald, A. H.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 30
  • DOI: 10.1073/pnas.1108174108

Ab initio theory of moiré superlattice bands in layered two-dimensional materials
journal, May 2014

Edge conduction in monolayer WTe2
journal, April 2017

  • Fei, Zaiyao; Palomaki, Tauno; Wu, Sanfeng
  • Nature Physics, Vol. 13, Issue 7
  • DOI: 10.1038/nphys4091

Massive Dirac Fermions and Hofstadter Butterfly in a van der Waals Heterostructure
journal, May 2013

Ultrafast generation of pseudo-magnetic field for valley excitons in WSe 2 monolayers
journal, December 2014

Topological mosaics in moiré superlattices of van der Waals heterobilayers
journal, November 2016

  • Tong, Qingjun; Yu, Hongyi; Zhu, Qizhong
  • Nature Physics, Vol. 13, Issue 4
  • DOI: 10.1038/nphys3968

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

Spectroscopic Signatures for Interlayer Coupling in MoS 2 –WSe 2 van der Waals Stacking
journal, August 2014

  • Chiu, Ming-Hui; Li, Ming-Yang; Zhang, Wengjing
  • ACS Nano, Vol. 8, Issue 9
  • DOI: 10.1021/nn504229z

Control of valley polarization in monolayer MoS2 by optical helicity
journal, June 2012

Valley polarization in MoS2 monolayers by optical pumping
journal, June 2012

  • Zeng, Hualing; Dai, Junfeng; Yao, Wang
  • Nature Nanotechnology, Vol. 7, Issue 8
  • DOI: 10.1038/nnano.2012.95

Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures
journal, February 2015

  • Rivera, Pasqual; Schaibley, John R.; Jones, Aaron M.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms7242

Determination of band offsets, hybridization, and exciton binding in 2D semiconductor heterostructures
journal, February 2017

  • Wilson, Neil R.; Nguyen, Paul V.; Seyler, Kyle
  • Science Advances, Vol. 3, Issue 2
  • DOI: 10.1126/sciadv.1601832

Emergence of superlattice Dirac points in graphene on hexagonal boron nitride
journal, March 2012

  • Yankowitz, Matthew; Xue, Jiamin; Cormode, Daniel
  • Nature Physics, Vol. 8, Issue 5
  • DOI: 10.1038/nphys2272
    [ × clear filter / sort ]

    Figures / Tables found in this record:

    FIG. 1 (p. 3)figure
    FIG. 2 (p. 4)figure
    FIG. 3 (p. 5)figure
    FIG. 4 (p. 6)figure
    FIG. 5 (p. 7)figure
    FIG. 6 (p. 8)figure
      [ × clear filter / sort ]
      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

      Similar records in OSTI.GOV collections: