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Title: Defect-Induced Modification of Low-Lying Excitons and Valley Selectivity in Monolayer Transition Metal Dichalcogenides

Abstract

Here, we study the effect of point-defect chalcogen vacancies on the optical properties of monolayer transition metal dichalcogenides using ab initio GW and Bethe-Salpeter equation calculations. We find that chalcogen vacancies introduce unoccupied in-gap states and occupied resonant defect states within the quasiparticle continuum of the valence band. These defect states give rise to a number of strongly bound defect excitons and hybridize with excitons of the pristine system, reducing the valley-selective circular dichroism. Lastly, our results suggest a pathway to tune spin-valley polarization and other optical properties through defect engineering.

Authors:
 [1];  [1];  [1];  [2]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy Nanosciences Inst. at Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division (SC-22.2)
OSTI Identifier:
1544189
Alternate Identifier(s):
OSTI ID: 1478571; OSTI ID: 1570228
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 121; Journal Issue: 16; 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

Citation Formats

Refaely-Abramson, Sivan, Qiu, Diana Y., Louie, Steven G., and Neaton, Jeffrey B. Defect-Induced Modification of Low-Lying Excitons and Valley Selectivity in Monolayer Transition Metal Dichalcogenides. United States: N. p., 2018. Web. doi:10.1103/PhysRevLett.121.167402.
Refaely-Abramson, Sivan, Qiu, Diana Y., Louie, Steven G., & Neaton, Jeffrey B. Defect-Induced Modification of Low-Lying Excitons and Valley Selectivity in Monolayer Transition Metal Dichalcogenides. United States. doi:10.1103/PhysRevLett.121.167402.
Refaely-Abramson, Sivan, Qiu, Diana Y., Louie, Steven G., and Neaton, Jeffrey B. Tue . "Defect-Induced Modification of Low-Lying Excitons and Valley Selectivity in Monolayer Transition Metal Dichalcogenides". United States. doi:10.1103/PhysRevLett.121.167402. https://www.osti.gov/servlets/purl/1544189.
@article{osti_1544189,
title = {Defect-Induced Modification of Low-Lying Excitons and Valley Selectivity in Monolayer Transition Metal Dichalcogenides},
author = {Refaely-Abramson, Sivan and Qiu, Diana Y. and Louie, Steven G. and Neaton, Jeffrey B.},
abstractNote = {Here, we study the effect of point-defect chalcogen vacancies on the optical properties of monolayer transition metal dichalcogenides using ab initio GW and Bethe-Salpeter equation calculations. We find that chalcogen vacancies introduce unoccupied in-gap states and occupied resonant defect states within the quasiparticle continuum of the valence band. These defect states give rise to a number of strongly bound defect excitons and hybridize with excitons of the pristine system, reducing the valley-selective circular dichroism. Lastly, our results suggest a pathway to tune spin-valley polarization and other optical properties through defect engineering.},
doi = {10.1103/PhysRevLett.121.167402},
journal = {Physical Review Letters},
number = 16,
volume = 121,
place = {United States},
year = {2018},
month = {10}
}

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Figures / Tables:

FIG. 1 FIG. 1: (a) Top and side view of 5×5 TMD supercells with one chalcogen vacancy. Vacancy sites are circled by a black dotted line. (b) left: isosurfaces of the occupied (bottom) and unoccupied (top) wavefunctions associated with the defect states in a 5×5 supercell of MoSe2. Right: The quasiparticle bandstructuremore » of MoSe2, along the$\bar{Γ}$ to $\bar{K}$ line in the supercell BZ (inset), calculated using G0W0@LDA, including SOC corrections. Defect/pristine-like states are labeled as $v$D/Pr ($c$D/Pr) for occupied (unoccupied) states. The inset shows a schematic (not to scale) of the supercell BZ compared to the BZ of a single unit cell of a pristine TMD. (c) Defect-state energy levels, calculated within DFT (LDA) and G0W0 for MoSe2 (left) and WS2 (right). Defect states are shown by black dashed lines, and the bulk states are shown in red and blue shaded regions for the spin up and spin down spin-orbit split bands.« less

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