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research article

Spectroscopic view of ultrafast charge carrier dynamics in single- and bilayer transition metal dichalcogenide semiconductors

Majchrzak, Paulina
•
Volckaert, Klara
•
Dabo, Antonija Grubisic
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July 1, 2021
Journal Of Electron Spectroscopy And Related Phenomena

The quasiparticle spectra of atomically thin semiconducting transition metal dichalcogenides (TMDCs) and their response to an ultrafast optical excitation critically depend on interactions with the underlying substrate. Here, we present a comparative time- and angle-resolved photoemission spectroscopy (TR-ARPES) study of the transient electronic structure and ultrafast carrier dynamics in the single- and bilayer TMDCs MoS2 and WS2 on three different substrates: Au(111), Ag(111) and graphene/SiC. The photoexcited quasiparticle bandgaps are observed to vary over the range of 1.9-2.5 eV between our systems. The transient conduction band signals decay on a sub-50 fs timescale on the metals, signifying an efficient removal of photoinduced carriers into the bulk metallic states. On graphene, we instead observe a fast timescale on the order of 170 fs, followed by a slow dynamics for the conduction band decay in MoS2. These timescales are explained by Auger recombination involving MoS2 and in-gap defect states. In bilayer TMDCs on metals we observe a complex redistribution of excited holes along the valence band that is substantially affected by interactions with the continuum of bulk metallic states.

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Type
research article
DOI
10.1016/j.elspec.2021.147093
Web of Science ID

WOS:000670411800009

Author(s)
Majchrzak, Paulina
Volckaert, Klara
Dabo, Antonija Grubisic
Biswas, Deepnarayan
Bianchi, Marco
Mahatha, Sanjoy K.
Dendzik, Maciej
Andreatta, Federico
Gronborg, Signe S.
Markovic, Igor
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Date Issued

2021-07-01

Publisher

ELSEVIER

Published in
Journal Of Electron Spectroscopy And Related Phenomena
Volume

250

Article Number

147093

Subjects

Spectroscopy

•

time-and angle-resolved photoemission spectroscopy

•

transition metal dichalcogenides

•

ultrafast carrier dynamics

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bandgap renormalization

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giant bandgap renormalization

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electronic-properties

•

ws2

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optoelectronics

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mechanism

•

excitons

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mos2

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LSE  
Available on Infoscience
July 31, 2021
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/180386
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