Narrow-band high-lying excitons with negative-mass electrons in monolayer WSe2.
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Authors
Faria Junior, Paulo E
Ziegler, Jonas D
Zipfel, Jonas
Bäuml, Christian
Paradiso, Nicola
Strunk, Christoph
Qiu, Diana Y
Publication Date
2021-09-17Journal Title
Nat Commun
ISSN
2041-1723
Publisher
Springer Science and Business Media LLC
Volume
12
Issue
1
Pages
5500
Language
eng
Type
Article
This Version
VoR
Physical Medium
Electronic
Metadata
Show full item recordCitation
Lin, K., Ong, C. S., Bange, S., Faria Junior, P. E., Peng, B., Ziegler, J. D., Zipfel, J., et al. (2021). Narrow-band high-lying excitons with negative-mass electrons in monolayer WSe2.. Nat Commun, 12 (1), 5500. https://doi.org/10.1038/s41467-021-25499-2
Abstract
Monolayer transition-metal dichalcogenides (TMDCs) show a wealth of exciton physics. Here, we report the existence of a new excitonic species, the high-lying exciton (HX), in single-layer WSe2 with an energy of ~3.4 eV, almost twice the band-edge A-exciton energy, with a linewidth as narrow as 5.8 meV. The HX is populated through momentum-selective optical excitation in the K-valleys and is identified in upconverted photoluminescence (UPL) in the UV spectral region. Strong electron-phonon coupling results in a cascaded phonon progression with equidistant peaks in the luminescence spectrum, resolvable to ninth order. Ab initio GW-BSE calculations with full electron-hole correlations explain HX formation and unmask the admixture of upper conduction-band states to this complex many-body excitation. These calculations suggest that the HX is comprised of electrons of negative mass. The coincidence of such high-lying excitonic species at around twice the energy of band-edge excitons rationalizes the excitonic quantum-interference phenomenon recently discovered in optical second-harmonic generation (SHG) and explains the efficient Auger-like annihilation of band-edge excitons.
Identifiers
External DOI: https://doi.org/10.1038/s41467-021-25499-2
This record's URL: https://www.repository.cam.ac.uk/handle/1810/329639
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