Phonon-assisted oscillatory exciton dynamics in monolayer MoSe2

Colin M. Chow; Hongyi Yu; Aaron M. Jones; John R. Schaibley; Michael Koehler; David G. Mandrus; R. Merlin; Wang Yao; Xiaodong Xu

doi:10.1038/s41699-017-0035-1

Phonon-assisted oscillatory exciton dynamics in monolayer MoSe₂

Colin M. Chow, Hongyi Yu, Aaron M. Jones, John R. Schaibley, Michael Koehler, David G. Mandrus, R. Merlin, Wang Yao, Xiaodong Xu

Physics

Research output: Contribution to journal › Article › peer-review

45 Scopus citations

Abstract

In monolayer semiconductor transition metal dichalcogenides, the exciton–phonon interaction strongly affects the photocarrier dynamics. Here, we report on an unusual oscillatory enhancement of the neutral exciton photoluminescence with the excitation laser frequency in monolayer MoSe₂. The frequency of oscillation matches that of the M-point longitudinal acoustic phonon, LA(M), suggesting the significance of zone-edge acoustic phonons and hence the deformation potential in exciton-phonon coupling in MoSe₂. Moreover, oscillatory behavior is observed in the steady-state emission linewidth and in time-resolved PLE data, which reveals variation with excitation energy in the exciton lifetime. These results clearly expose the key role played by phonons in the exciton formation and relaxation dynamics of two-dimensional van der Waals semiconductors.

Original language	English (US)
Article number	33
Journal	npj 2D Materials and Applications
Volume	1
Issue number	1
DOIs	https://doi.org/10.1038/s41699-017-0035-1
State	Published - Dec 1 2017

ASJC Scopus subject areas

Materials Science(all)
Mechanical Engineering
Mechanics of Materials
Condensed Matter Physics
Chemistry(all)

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title = "Phonon-assisted oscillatory exciton dynamics in monolayer MoSe2",

abstract = "In monolayer semiconductor transition metal dichalcogenides, the exciton–phonon interaction strongly affects the photocarrier dynamics. Here, we report on an unusual oscillatory enhancement of the neutral exciton photoluminescence with the excitation laser frequency in monolayer MoSe2. The frequency of oscillation matches that of the M-point longitudinal acoustic phonon, LA(M), suggesting the significance of zone-edge acoustic phonons and hence the deformation potential in exciton-phonon coupling in MoSe2. Moreover, oscillatory behavior is observed in the steady-state emission linewidth and in time-resolved PLE data, which reveals variation with excitation energy in the exciton lifetime. These results clearly expose the key role played by phonons in the exciton formation and relaxation dynamics of two-dimensional van der Waals semiconductors.",

author = "Chow, {Colin M.} and Hongyi Yu and Jones, {Aaron M.} and Schaibley, {John R.} and Michael Koehler and Mandrus, {David G.} and R. Merlin and Wang Yao and Xiaodong Xu",

note = "Funding Information: This work is mainly supported by the Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division (DE-SC0008145 and SC0012509). H.Y. and W.Y. are supported by the Croucher Foundation (Croucher Innovation Award), HKU ORA, and the RGC and UGC of Hong Kong (HKU17305914P, AoE/P-04/08). M.K. and D.G.M. are supported by US DoE, BES, Materials Sciences and Engineering Division. R.M. is supported by the MRSEC Program of the NSF under Grant No. DMR-1120923. X.X. acknowledges a Cottrell Scholar Award, support from the State of Washington funded Clean Energy Institute, and Boeing Distinguished Professorship. Publisher Copyright: {\textcopyright} 2017, The Author(s).",

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AU - Chow, Colin M.

AU - Yu, Hongyi

AU - Jones, Aaron M.

AU - Schaibley, John R.

AU - Koehler, Michael

AU - Mandrus, David G.

AU - Merlin, R.

AU - Yao, Wang

AU - Xu, Xiaodong

N1 - Funding Information: This work is mainly supported by the Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division (DE-SC0008145 and SC0012509). H.Y. and W.Y. are supported by the Croucher Foundation (Croucher Innovation Award), HKU ORA, and the RGC and UGC of Hong Kong (HKU17305914P, AoE/P-04/08). M.K. and D.G.M. are supported by US DoE, BES, Materials Sciences and Engineering Division. R.M. is supported by the MRSEC Program of the NSF under Grant No. DMR-1120923. X.X. acknowledges a Cottrell Scholar Award, support from the State of Washington funded Clean Energy Institute, and Boeing Distinguished Professorship. Publisher Copyright: © 2017, The Author(s).

PY - 2017/12/1

Y1 - 2017/12/1

N2 - In monolayer semiconductor transition metal dichalcogenides, the exciton–phonon interaction strongly affects the photocarrier dynamics. Here, we report on an unusual oscillatory enhancement of the neutral exciton photoluminescence with the excitation laser frequency in monolayer MoSe2. The frequency of oscillation matches that of the M-point longitudinal acoustic phonon, LA(M), suggesting the significance of zone-edge acoustic phonons and hence the deformation potential in exciton-phonon coupling in MoSe2. Moreover, oscillatory behavior is observed in the steady-state emission linewidth and in time-resolved PLE data, which reveals variation with excitation energy in the exciton lifetime. These results clearly expose the key role played by phonons in the exciton formation and relaxation dynamics of two-dimensional van der Waals semiconductors.

AB - In monolayer semiconductor transition metal dichalcogenides, the exciton–phonon interaction strongly affects the photocarrier dynamics. Here, we report on an unusual oscillatory enhancement of the neutral exciton photoluminescence with the excitation laser frequency in monolayer MoSe2. The frequency of oscillation matches that of the M-point longitudinal acoustic phonon, LA(M), suggesting the significance of zone-edge acoustic phonons and hence the deformation potential in exciton-phonon coupling in MoSe2. Moreover, oscillatory behavior is observed in the steady-state emission linewidth and in time-resolved PLE data, which reveals variation with excitation energy in the exciton lifetime. These results clearly expose the key role played by phonons in the exciton formation and relaxation dynamics of two-dimensional van der Waals semiconductors.

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Phonon-assisted oscillatory exciton dynamics in monolayer MoSe₂

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