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Title: Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

Abstract

Atomically thin transition metal dichalcogenides are direct-gap semiconductors with strong light–matter and Coulomb interactions. The latter accounts for tightly bound excitons, which dominate their optical properties. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in the optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. We investigate the microscopic origin of the excitonic coherence lifetime in two representative materials (WS 2 and MoSe 2) through a study combining microscopic theory with spectroscopic measurements. We also show that the excitonic coherence lifetime is determined by phonon-induced intravalley scattering and intervalley scattering into dark excitonic states. Particularly, we identify exciton relaxation processes involving phonon emission into lower-lying dark states that are operative at all temperatures, in WS 2.

Authors:
 [1];  [1];  [2];  [3];  [3];  [4];  [3];  [5];  [6];  [1]
  1. Technical Univ. of Berlin (Germany). Inst. for Theoretical Physics
  2. Columbia Univ., New York, NY (United States). Dept. of Chemistry; Stanford Univ., CA (United States). Dept. of Applied Physics
  3. Univ. of Regensburg (Germany). Inst. for Experimental and Applied Physics
  4. Stanford Univ., CA (United States). Dept. of Applied Physics; SLAC National Accelerator Lab., Menlo Park, CA (United States); Columbia Univ., New York, NY (United States). Dept. of Physics and Electrical Engineering
  5. Univ. of Regensburg (Germany). Inst. for Experimental and Applied Physics; Columbia Univ., New York, NY (United States). Dept. of Physics and Electrical Engineering
  6. Chalmers Univ. of Technology, Gothenburg (Sweden). Dept. of Physics
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1348911
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; electronic properties and materials; optical physics; two-dimensional materials

Citation Formats

Selig, Malte, Berghäuser, Gunnar, Raja, Archana, Nagler, Philipp, Schüller, Christian, Heinz, Tony F., Korn, Tobias, Chernikov, Alexey, Malic, Ermin, and Knorr, Andreas. Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides. United States: N. p., 2016. Web. doi:10.1038/ncomms13279.
Selig, Malte, Berghäuser, Gunnar, Raja, Archana, Nagler, Philipp, Schüller, Christian, Heinz, Tony F., Korn, Tobias, Chernikov, Alexey, Malic, Ermin, & Knorr, Andreas. Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides. United States. doi:10.1038/ncomms13279.
Selig, Malte, Berghäuser, Gunnar, Raja, Archana, Nagler, Philipp, Schüller, Christian, Heinz, Tony F., Korn, Tobias, Chernikov, Alexey, Malic, Ermin, and Knorr, Andreas. Mon . "Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides". United States. doi:10.1038/ncomms13279. https://www.osti.gov/servlets/purl/1348911.
@article{osti_1348911,
title = {Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides},
author = {Selig, Malte and Berghäuser, Gunnar and Raja, Archana and Nagler, Philipp and Schüller, Christian and Heinz, Tony F. and Korn, Tobias and Chernikov, Alexey and Malic, Ermin and Knorr, Andreas},
abstractNote = {Atomically thin transition metal dichalcogenides are direct-gap semiconductors with strong light–matter and Coulomb interactions. The latter accounts for tightly bound excitons, which dominate their optical properties. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in the optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. We investigate the microscopic origin of the excitonic coherence lifetime in two representative materials (WS2 and MoSe2) through a study combining microscopic theory with spectroscopic measurements. We also show that the excitonic coherence lifetime is determined by phonon-induced intravalley scattering and intervalley scattering into dark excitonic states. Particularly, we identify exciton relaxation processes involving phonon emission into lower-lying dark states that are operative at all temperatures, in WS2.},
doi = {10.1038/ncomms13279},
journal = {Nature Communications},
issn = {2041-1723},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {11}
}

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Cited by: 34 works
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    Works referencing / citing this record:

    Evidence for line width and carrier screening effects on excitonic valley relaxation in 2D semiconductors
    journal, July 2018


    The role of momentum-dark excitons in the elementary optical response of bilayer WSe2
    journal, July 2018


    Two-dimensional semiconductors in the regime of strong light-matter coupling
    journal, July 2018


    Intrinsic lifetime of higher excitonic states in tungsten diselenide monolayers
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    • Brem, Samuel; Zipfel, Jonas; Selig, Malte
    • Nanoscale, Vol. 11, Issue 25
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    Two-dimensional semiconductors in the regime of strong light-matter coupling
    journal, July 2018


    The role of momentum-dark excitons in the elementary optical response of bilayer WSe2
    journal, July 2018


    Evidence for line width and carrier screening effects on excitonic valley relaxation in 2D semiconductors
    journal, July 2018


    Tuning the Fröhlich exciton-phonon scattering in monolayer MoS2
    journal, February 2019


    Intrinsic lifetime of higher excitonic states in tungsten diselenide monolayers
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    • Brem, Samuel; Zipfel, Jonas; Selig, Malte
    • Nanoscale, Vol. 11, Issue 25
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