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

Title: Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields

Abstract

In semiconductor physics, many essential optoelectronic material parameters can be experimentally revealed via optical spectroscopy in sufficiently large magnetic fields. For monolayer transition-metal dichalcogenide semiconductors, this field scale is substantial—tens of teslas or more—due to heavy carrier masses and huge exciton binding energies. Here we report absorption spectroscopy of monolayer MoS2, MoSe2, MoTe2, and WS2 in very high magnetic fields to 91 T. We follow the diamagnetic shifts and valley Zeeman splittings of not only the exciton’s 1s ground state but also its excited 2s,3s,…,ns Rydberg states. This provides a direct experimental measure of the effective (reduced) exciton masses and dielectric properties. Exciton binding energies, exciton radii, and free-particle bandgaps are also determined. The measured exciton masses are heavier than theoretically predicted, especially for Mo-based monolayers. These results provide essential and quantitative parameters for the rational design of opto-electronic van der Waals heterostructures incorporating 2D semiconductors.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [2];  [3];  [3];  [3]; ORCiD logo [3];  [3]; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. National Institute for Materials Science, Ibaraki (Japan)
  3. Univ. de Toulouse, Toulouse (France)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1565907
Report Number(s):
LA-UR-19-23579
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; High Magnetic Field Science

Citation Formats

Goryca, Mateusz Marek, Li, Jing, Stier, Andreas V., Taniguchi, Takashi, Watanabe, K., Courtade, Emmanuel, Shree, S., Robert, Cedric, Urbaszek, B., Marie, X., and Crooker, Scott A. Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields. United States: N. p., 2019. Web. doi:10.1038/s41467-019-12180-y.
Goryca, Mateusz Marek, Li, Jing, Stier, Andreas V., Taniguchi, Takashi, Watanabe, K., Courtade, Emmanuel, Shree, S., Robert, Cedric, Urbaszek, B., Marie, X., & Crooker, Scott A. Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields. United States. doi:10.1038/s41467-019-12180-y.
Goryca, Mateusz Marek, Li, Jing, Stier, Andreas V., Taniguchi, Takashi, Watanabe, K., Courtade, Emmanuel, Shree, S., Robert, Cedric, Urbaszek, B., Marie, X., and Crooker, Scott A. Fri . "Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields". United States. doi:10.1038/s41467-019-12180-y. https://www.osti.gov/servlets/purl/1565907.
@article{osti_1565907,
title = {Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields},
author = {Goryca, Mateusz Marek and Li, Jing and Stier, Andreas V. and Taniguchi, Takashi and Watanabe, K. and Courtade, Emmanuel and Shree, S. and Robert, Cedric and Urbaszek, B. and Marie, X. and Crooker, Scott A.},
abstractNote = {In semiconductor physics, many essential optoelectronic material parameters can be experimentally revealed via optical spectroscopy in sufficiently large magnetic fields. For monolayer transition-metal dichalcogenide semiconductors, this field scale is substantial—tens of teslas or more—due to heavy carrier masses and huge exciton binding energies. Here we report absorption spectroscopy of monolayer MoS2, MoSe2, MoTe2, and WS2 in very high magnetic fields to 91 T. We follow the diamagnetic shifts and valley Zeeman splittings of not only the exciton’s 1s ground state but also its excited 2s,3s,…,ns Rydberg states. This provides a direct experimental measure of the effective (reduced) exciton masses and dielectric properties. Exciton binding energies, exciton radii, and free-particle bandgaps are also determined. The measured exciton masses are heavier than theoretically predicted, especially for Mo-based monolayers. These results provide essential and quantitative parameters for the rational design of opto-electronic van der Waals heterostructures incorporating 2D semiconductors.},
doi = {10.1038/s41467-019-12180-y},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 2 works
Citation information provided by
Web of Science

Figures / Tables:

Table 1 Table 1: Fundamental optoelectronic material parameters of monolayer TMD semiconductors

Save / Share:

Works referenced in this record:

Exciton spectra in thin crystals: the diamagnetic effect
journal, June 1967


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


Excitonic Valley Effects in Monolayer WS 2 under High Magnetic Fields
journal, November 2016


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


Breaking of Valley Degeneracy by Magnetic Field in Monolayer MoSe 2
journal, January 2015


Large effective mass and interaction-enhanced Zeeman splitting of K -valley electrons in MoSe 2
journal, May 2018


Hydrogenic energy levels in two dimensions at arbitrary magnetic fields
journal, June 1986


Normal Modes in Hexagonal Boron Nitride
journal, June 1966


Magnetic brightening and control of dark excitons in monolayer WSe2
journal, June 2017

  • Zhang, Xiao-Xiao; Cao, Ting; Lu, Zhengguang
  • Nature Nanotechnology, Vol. 12, Issue 9
  • DOI: 10.1038/nnano.2017.105

Emerging Photoluminescence in Monolayer MoS2
journal, April 2010

  • Splendiani, Andrea; Sun, Liang; Zhang, Yuanbo
  • Nano Letters, Vol. 10, Issue 4, p. 1271-1275
  • DOI: 10.1021/nl903868w

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

Magnetostriction and magnetic texture to 100.75 Tesla in frustrated SrCu2(BO3)2
journal, July 2012

  • Jaime, M.; Daou, R.; Crooker, S. A.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 31
  • DOI: 10.1073/pnas.1200743109

Brightening of dark excitons in monolayers of semiconducting transition metal dichalcogenides
journal, January 2017


In-Plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules
journal, July 2017


Substrate interactions with suspended and supported monolayer Mo S 2 : Angle-resolved photoemission spectroscopy
journal, March 2015


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


Interband Optical Transitions in Extremely Anisotropic Semiconductors. II. Coexistence of Exciton and the Landau Levels
journal, January 1967

  • Akimoto, Okikazu; Hasegawa, Hiroshi
  • Journal of the Physical Society of Japan, Vol. 22, Issue 1
  • DOI: 10.1143/JPSJ.22.181

Valley- and spin-polarized Landau levels in monolayer WSe2
journal, October 2016


Magneto-polarons in monolayer transition-metal dichalcogenides
journal, June 2018

  • Chen, Qiao; Wang, Weiyang; Peeters, F. M.
  • Journal of Applied Physics, Vol. 123, Issue 21
  • DOI: 10.1063/1.5025907

Single-layer MoS2
journal, April 1986


Diamagnetic shift in In x Ga 1 x As/GaAs strained quantum wells
journal, February 1991


Three-band tight-binding model for monolayers of group-VIB transition metal dichalcogenides
journal, August 2013


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


XX. Properties of slow electrons in polar materials
journal, March 1950

  • Fröhlich, H.; Pelzer, H.; Zienau, S.
  • The London, Edinburgh, and Dublin Philosophical Magazine and Journal of Science, Vol. 41, Issue 314
  • DOI: 10.1080/14786445008521794

Atomically Thin MoS2 A New Direct-Gap Semiconductor
journal, September 2010


Magnetoexcitons in large area CVD-grown monolayer MoS 2 and MoSe 2 on sapphire
journal, April 2016


Exciton diamagnetic shift in semiconductor nanostructures
journal, April 1998


Spin- and valley-dependent magneto-optical properties of MoS 2
journal, September 2013


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

Exciton diamagnetic shifts and valley Zeeman effects in monolayer WS2 and MoS2 to 65 Tesla
journal, February 2016

  • Stier, Andreas V.; McCreary, Kathleen M.; Jonker, Berend T.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms10643

Effects of confinement and environment on the electronic structure and exciton binding energy of MoS 2 from first principles
journal, December 2012


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


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

Observation of interlayer excitons in MoSe 2 single crystals
journal, June 2018


Polaronic correction to the exciton effective mass
journal, June 1987


Magnetooptics of Exciton Rydberg States in a Monolayer Semiconductor
journal, February 2018


Excitons, trions, and biexcitons in transition-metal dichalcogenides: Magnetic-field dependence
journal, May 2018


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


Electronic structure of a single MoS2 monolayer
journal, May 2012


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


Luminescent Emission of Excited Rydberg Excitons from Monolayer WSe 2
journal, March 2019


Coulomb interaction in monolayer transition-metal dichalcogenides
journal, September 2018


Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers
journal, July 2017

  • Ajayi, Obafunso A.; Ardelean, Jenny V.; Shepard, Gabriella D.
  • 2D Materials, Vol. 4, Issue 3
  • DOI: 10.1088/2053-1583/aa6aa1

Splitting between bright and dark excitons in transition metal dichalcogenide monolayers
journal, March 2016


Robust optical emission polarization in MoS 2 monolayers through selective valley excitation
journal, August 2012


Valley Zeeman Splitting and Valley Polarization of Neutral and Charged Excitons in Monolayer MoTe 2 at High Magnetic Fields
journal, May 2016


Direct observation of the transition from indirect to direct bandgap in atomically thin epitaxial MoSe2
journal, December 2013


Intervalley polaron in atomically thin transition metal dichalcogenides
journal, July 2019


Emergence of Interfacial Polarons from Electron–Phonon Coupling in Graphene/h-BN van der Waals Heterostructures
journal, January 2018


Van der Waals heterostructures
journal, July 2013

  • Geim, A. K.; Grigorieva, I. V.
  • Nature, Vol. 499, Issue 7459, p. 419-425
  • DOI: 10.1038/nature12385

Interactions and Magnetotransport through Spin-Valley Coupled Landau Levels in Monolayer MoS 2
journal, December 2018


Spatial extent of the excited exciton states in WS 2 monolayers from diamagnetic shifts
journal, August 2018


Binding energies of exciton complexes in transition metal dichalcogenide monolayers and effect of dielectric environment
journal, November 2015


Spin-resolved photoemission study of epitaxially grown MoSe 2 and WSe 2 thin films
journal, September 2016


Electronics and optoelectronics of two-dimensional transition metal dichalcogenides
journal, November 2012

  • Wang, Qing Hua; Kalantar-Zadeh, Kourosh; Kis, Andras
  • Nature Nanotechnology, Vol. 7, Issue 11, p. 699-712
  • DOI: 10.1038/nnano.2012.193

Magneto-optics in GaAs- Ga 1 x Al x As quantum wells
journal, September 1986


Monolayer MoS2 Bandgap Modulation by Dielectric Environments and Tunable Bandgap Transistors
journal, July 2016

  • Ryou, Junga; Kim, Yong-Sung; Kc, Santosh
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep29184

Band Structures of Transition-Metal-Dichalcogenide Layer Compounds
journal, October 1973


Orbital, spin and valley contributions to Zeeman splitting of excitonic resonances in MoSe 2 , WSe 2 and WS 2 Monolayers
journal, October 2018


Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides
journal, March 2016


Corrigendum: k.p theory for two-dimensional transition metal dichalcogenide semiconductors (2015 2D Mater. 2 022001)
journal, November 2015


Valley-splitting and valley-dependent inter-Landau-level optical transitions in monolayer MoS 2 quantum Hall systems
journal, July 2014


Direct exciton emission from atomically thin transition metal dichalcogenide heterostructures near the lifetime limit
journal, September 2017


Large Excitonic Reflectivity of Monolayer MoSe 2 Encapsulated in Hexagonal Boron Nitride
journal, January 2018


Realization of an Electrically Tunable Narrow-Bandwidth Atomically Thin Mirror Using Monolayer MoSe 2
journal, January 2018


Optical spectroscopy of excited exciton states in MoS 2 monolayers in van der Waals heterostructures
journal, January 2018


Valley Splitting and Polarization by the Zeeman Effect in Monolayer MoSe 2
journal, December 2014


The Dielectric Impact of Layer Distances on Exciton and Trion Binding Energies in van der Waals Heterostructures
journal, March 2018


Magneto-optics in transition metal diselenide monolayers
journal, June 2015


Excitons in van der Waals heterostructures: The important role of dielectric screening
journal, December 2015


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


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

Quasiparticle band structures and optical properties of strained monolayer MoS 2 and WS 2
journal, April 2013


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


Quasiparticle band structure calculation of monolayer, bilayer, and bulk MoS 2
journal, May 2012


Electronic and thermoelectric properties of few-layer transition metal dichalcogenides
journal, March 2014

  • Wickramaratne, Darshana; Zahid, Ferdows; Lake, Roger K.
  • The Journal of Chemical Physics, Vol. 140, Issue 12
  • DOI: 10.1063/1.4869142

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

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


High-quality, large-area MoSe 2 and MoSe 2 /Bi 2 Se 3 heterostructures on AlN(0001)/Si(111) substrates by molecular beam epitaxy
journal, January 2015

  • Xenogiannopoulou, E.; Tsipas, P.; Aretouli, K. E.
  • Nanoscale, Vol. 7, Issue 17
  • DOI: 10.1039/C4NR06874B

    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.