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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 Laboratory (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. https://doi.org/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. https://doi.org/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 = {Fri Sep 13 00:00:00 EDT 2019},
month = {Fri Sep 13 00:00:00 EDT 2019}
}

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Cited by: 127 works
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Figures / Tables:

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

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Works referencing / citing this record:

Rydberg series of dark excitons and the conduction band spin-orbit splitting in monolayer WSe2
journal, August 2021


Energy Spectrum of Two-Dimensional Excitons in a Nonuniform Dielectric Medium
journal, September 2019


Coherent dynamics and mapping of excitons in single-layer MoSe$_2$ and WSe$_2$ at the homogeneous limit
text, January 2020


Spontaneous Valley Polarization of Interacting Carriers in a Monolayer Semiconductor
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High optical quality of MoS 2 monolayers grown by chemical vapor deposition
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Tunable quantum confinement of neutral excitons using electric fields and exciton-charge interactions
preprint, January 2021


Controlling exciton many-body states by the electric-field effect in monolayer MoS$_2$
text, January 2020


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