Defect-Mediated Charge-Carrier Trapping and Nonradiative Recombination in WSe2 Monolayers
Abstract
Nonradiative charge-carrier recombination in transition-metal dichalcogenide (TMD) monolayers severely limits their use in solar energy conversion technologies. Because defects serve as recombination sites, developing a quantitative description of charge-carrier dynamics in defective TMD monolayers can shed light on recombination mechanisms. Herein we report a first-principles investigation of charge-carrier dynamics in pristine and defective WSe2 monolayers with three of the most probable defects, namely, Se vacancies, W vacancies, and SeW antisites. We predict that Se vacancies slow down recombination by nearly an order of magnitude relative to defect-free samples by breaking the monolayer’s symmetry and thereby reducing the spectral intensity of the A1g phonon mode that promotes recombination in the pristine monolayer. By contrast, we find W vacancies accelerate recombination by more than an order of magnitude, with half of the recombination events bypassing charge traps. The subsequent dynamics feature both charge trapping and charge-trap-assisted recombination. Although SeW antisites also slightly accelerate recombination, the predicted mechanism is different from the W vacancy case. First, a shallow energy level traps a photoexcited electron. Then, both shallow- and deep-trap-assisted recombination can occur simultaneously. Accelerated recombination arises for W vacancies and SeW antisites because they introduce new phonon modes that strongly couple to electronmore »
- Publication Date:
- Research Org.:
- Princeton Univ., NJ (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1812547
- Grant/Contract Number:
- SC0002120
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 141; Journal Issue: 26; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 14 SOLAR ENERGY; 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; WSe2 monolayer; charge carrier; defects; nonradiative recombination; monolayers; charge transfer; defects in solids; recombination
Citation Formats
Li, Lesheng, and Carter, Emily A. Defect-Mediated Charge-Carrier Trapping and Nonradiative Recombination in WSe2 Monolayers. United States: N. p., 2019.
Web. doi:10.1021/jacs.9b04663.
Li, Lesheng, & Carter, Emily A. Defect-Mediated Charge-Carrier Trapping and Nonradiative Recombination in WSe2 Monolayers. United States. https://doi.org/10.1021/jacs.9b04663
Li, Lesheng, and Carter, Emily A. Wed .
"Defect-Mediated Charge-Carrier Trapping and Nonradiative Recombination in WSe2 Monolayers". United States. https://doi.org/10.1021/jacs.9b04663. https://www.osti.gov/servlets/purl/1812547.
@article{osti_1812547,
title = {Defect-Mediated Charge-Carrier Trapping and Nonradiative Recombination in WSe2 Monolayers},
author = {Li, Lesheng and Carter, Emily A.},
abstractNote = {Nonradiative charge-carrier recombination in transition-metal dichalcogenide (TMD) monolayers severely limits their use in solar energy conversion technologies. Because defects serve as recombination sites, developing a quantitative description of charge-carrier dynamics in defective TMD monolayers can shed light on recombination mechanisms. Herein we report a first-principles investigation of charge-carrier dynamics in pristine and defective WSe2 monolayers with three of the most probable defects, namely, Se vacancies, W vacancies, and SeW antisites. We predict that Se vacancies slow down recombination by nearly an order of magnitude relative to defect-free samples by breaking the monolayer’s symmetry and thereby reducing the spectral intensity of the A1g phonon mode that promotes recombination in the pristine monolayer. By contrast, we find W vacancies accelerate recombination by more than an order of magnitude, with half of the recombination events bypassing charge traps. The subsequent dynamics feature both charge trapping and charge-trap-assisted recombination. Although SeW antisites also slightly accelerate recombination, the predicted mechanism is different from the W vacancy case. First, a shallow energy level traps a photoexcited electron. Then, both shallow- and deep-trap-assisted recombination can occur simultaneously. Accelerated recombination arises for W vacancies and SeW antisites because they introduce new phonon modes that strongly couple to electron and hole dynamics. This work thus provides a detailed understanding of the mechanisms behind charge-carrier recombination in WSe2 monolayers with distinct defects. Furthermore, materials engineering, particularly to avoid W vacancies, could advance this technology. The insights derived are important for future design of high-performance photoactive devices based on WSe2 monolayers.},
doi = {10.1021/jacs.9b04663},
journal = {Journal of the American Chemical Society},
number = 26,
volume = 141,
place = {United States},
year = {Wed Jun 05 00:00:00 EDT 2019},
month = {Wed Jun 05 00:00:00 EDT 2019}
}
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Works referencing / citing this record:
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