Kuhn, Henning, Wagner, Julian, Han, Shuangping, Bernhardt, Robin, Gao, Yan, Xiao, Liantuan, Zhu, Jingyi and van Loosdrecht, Paul H. M. ORCID: 0000-0002-3704-9890 (2020). Excitonic Transport and Intervalley Scattering Dynamics in Large-Size Exfoliated MoSe2 Monolayer Investigated by Heterodyned Transient Grating Spectroscopy. Laser Photon. Rev., 14 (12). WEINHEIM: WILEY-V C H VERLAG GMBH. ISSN 1863-8899

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Abstract

Exciton intervalley scattering, annihilation, relaxation dynamics, and diffusive transport in monolayer transition metal dichalcogenides are central to the functionality of devices based on them. Here, these properties in a large-size exfoliated high-quality monolayer MoSe2 are addressed directly using heterodyned transient grating spectroscopy at room temperature. While the free exciton population is found to be long-lived (approximate to 230 ps), an extremely fast intervalley scattering (<= 170 fs) is observed, leading to a negligible valley polarization, consistent with steady state photoluminescence measurements and theoretical calculation. The exciton population decay shows an appreciable contribution from the exciton-exciton annihilation, with an annihilation rate of approximate to 0.01 cm(2) s(-1). The annihilation process also leads to a significant distortion of the transient grating evolution. Taking this distortion into account, consistent exciton diffusion constants D approximate to 1.4 cm(2) s(-1) are found by a model simulation in the excitation density range of 10(11)-10(12) cm(-2). The presented results highlight the importance of correctly considering the many-body annihilation processes to obtain a pronounced understanding of the excitonic properties of monolayer transition metal dichalcogenides.

Item Type: Journal Article
Creators:
CreatorsEmailORCIDORCID Put Code
Kuhn, HenningUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Wagner, JulianUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Han, ShuangpingUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Bernhardt, RobinUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Gao, YanUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Xiao, LiantuanUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Zhu, JingyiUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
van Loosdrecht, Paul H. M.UNSPECIFIEDorcid.org/0000-0002-3704-9890UNSPECIFIED
URN: urn:nbn:de:hbz:38-311365
DOI: 10.1002/lpor.202000029
Journal or Publication Title: Laser Photon. Rev.
Volume: 14
Number: 12
Date: 2020
Publisher: WILEY-V C H VERLAG GMBH
Place of Publication: WEINHEIM
ISSN: 1863-8899
Language: English
Faculty: Faculty of Mathematics and Natural Sciences
Divisions: Faculty of Mathematics and Natural Sciences > Department of Physics > Institute of Physics II
Subjects: no entry
Uncontrolled Keywords:
KeywordsLanguage
VALLEY POLARIZATION; CARRIER-DIFFUSION; ANNIHILATION; SPIN; PHOTOLUMINESCENCE; OPTOELECTRONICS; RECOMBINATION; GENERATION; LIFETIMES; BANDGAPMultiple languages
Optics; Physics, Applied; Physics, Condensed MatterMultiple languages
Refereed: Yes
URI: http://kups.ub.uni-koeln.de/id/eprint/31136

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