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

Paulina Majchrzak; Klara Volckaert; Antonija Grubišić Čabo; Deepnarayan Biswas; Marco Bianchi; Sanjoy K. Mahatha; Maciej Dendzik; Federico Andreatta; Signe S. Grønborg; Igor Marković; Jonathon M. Riley; Jens C. Johannsen; Daniel Lizzit; Luca Bignardi; Silvano Lizzit; Cephise Cacho; Oliver Alexander; Dan Matselyukh; Adam S. Wyatt; Richard T. Chapman; Emma Springate; Jeppe V. Lauritsen; Phil D.C. King; Charlotte E. Sanders; Jill A. Miwa; Philip Hofmann; Søren Ulstrup

doi:10.1016/j.elspec.2021.147093

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

Paulina Majchrzak, Klara Volckaert, Antonija Grubišić Čabo, Deepnarayan Biswas, Marco Bianchi, Sanjoy K. Mahatha, Maciej Dendzik, Federico Andreatta, Signe S. Grønborg, Igor Marković, Jonathon M. Riley, Jens C. Johannsen, Daniel Lizzit, Luca Bignardi, Silvano Lizzit, Cephise Cacho, Oliver Alexander, Dan Matselyukh, Adam S. Wyatt, Richard T. ChapmanEmma Springate, Jeppe V. Lauritsen, Phil D.C. King, Charlotte E. Sanders, Jill A. Miwa, Philip Hofmann, Søren Ulstrup^*

^*Corresponding author for this work

Physics and Astronomy

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

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Abstract

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.

Original language	English
Article number	147093
Number of pages	7
Journal	Journal of Electron Spectroscopy and Related Phenomena
Volume	250
Early online date	19 Jun 2021
DOIs	https://doi.org/10.1016/j.elspec.2021.147093
Publication status	Published - Jul 2021

Bibliographical note

Funding Information:
We thank Phil Rice and Alistair Cox for technical support during the Artemis beamtimes. We gratefully acknowledge funding from VILLUM FONDEN, Denmark through the Young Investigator Program (Grant. No. 15375) and the Centre of Excellence for Dirac Materials, Denmark (Grant. No. 11744), the Danish Council for Independent Research, Natural Sciences, Denmark under the Sapere Aude program (Grant Nos. DFF-9064-00057B and DFF-6108-00409). Access to the Artemis Facility was funded by STFC. I.M. acknowledges financial support by the International Max Planck Research School for Chemistry and Physics of Quantum Materials (IMPRS-CPQM). The authors also acknowledge The Royal Society and The Leverhulme Trust.

Publisher Copyright:
© 2021 The Author(s)

Keywords

Bandgap renormalization
Time-and angle-resolved photoemission spectroscopy
Transition metal dichalcogenides
Ultrafast carrier dynamics

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Radiation
Atomic and Molecular Physics, and Optics
Condensed Matter Physics
Spectroscopy
Physical and Theoretical Chemistry

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Majchrzak, P., Volckaert, K., Čabo, A. G., Biswas, D., Bianchi, M., Mahatha, S. K., Dendzik, M., Andreatta, F., Grønborg, S. S., Marković, I., Riley, J. M., Johannsen, J. C., Lizzit, D., Bignardi, L., Lizzit, S., Cacho, C., Alexander, O., Matselyukh, D., Wyatt, A. S., ... Ulstrup, S. (2021). Spectroscopic view of ultrafast charge carrier dynamics in single- and bilayer transition metal dichalcogenide semiconductors. Journal of Electron Spectroscopy and Related Phenomena, 250, Article 147093. https://doi.org/10.1016/j.elspec.2021.147093

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

abstract = "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.",

keywords = "Bandgap renormalization, Time-and angle-resolved photoemission spectroscopy, Transition metal dichalcogenides, Ultrafast carrier dynamics",

author = "Paulina Majchrzak and Klara Volckaert and {\v C}abo, {Antonija Grubi{\v s}i{\'c}} and Deepnarayan Biswas and Marco Bianchi and Mahatha, {Sanjoy K.} and Maciej Dendzik and Federico Andreatta and Gr{\o}nborg, {Signe S.} and Igor Markovi{\'c} and Riley, {Jonathon M.} and Johannsen, {Jens C.} and Daniel Lizzit and Luca Bignardi and Silvano Lizzit and Cephise Cacho and Oliver Alexander and Dan Matselyukh and Wyatt, {Adam S.} and Chapman, {Richard T.} and Emma Springate and Lauritsen, {Jeppe V.} and King, {Phil D.C.} and Sanders, {Charlotte E.} and Miwa, {Jill A.} and Philip Hofmann and S{\o}ren Ulstrup",

note = "Funding Information: We thank Phil Rice and Alistair Cox for technical support during the Artemis beamtimes. We gratefully acknowledge funding from VILLUM FONDEN, Denmark through the Young Investigator Program (Grant. No. 15375) and the Centre of Excellence for Dirac Materials, Denmark (Grant. No. 11744), the Danish Council for Independent Research, Natural Sciences, Denmark under the Sapere Aude program (Grant Nos. DFF-9064-00057B and DFF-6108-00409). Access to the Artemis Facility was funded by STFC. I.M. acknowledges financial support by the International Max Planck Research School for Chemistry and Physics of Quantum Materials (IMPRS-CPQM). The authors also acknowledge The Royal Society and The Leverhulme Trust. Publisher Copyright: {\textcopyright} 2021 The Author(s)",

year = "2021",

month = jul,

doi = "10.1016/j.elspec.2021.147093",

language = "English",

volume = "250",

journal = "Journal of Electron Spectroscopy and Related Phenomena",

issn = "0368-2048",

publisher = "Elsevier",

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Majchrzak, P, Volckaert, K, Čabo, AG, Biswas, D, Bianchi, M, Mahatha, SK, Dendzik, M, Andreatta, F, Grønborg, SS, Marković, I, Riley, JM, Johannsen, JC, Lizzit, D, Bignardi, L, Lizzit, S, Cacho, C, Alexander, O, Matselyukh, D, Wyatt, AS, Chapman, RT, Springate, E, Lauritsen, JV, King, PDC, Sanders, CE, Miwa, JA, Hofmann, P & Ulstrup, S 2021, 'Spectroscopic view of ultrafast charge carrier dynamics in single- and bilayer transition metal dichalcogenide semiconductors', Journal of Electron Spectroscopy and Related Phenomena, vol. 250, 147093. https://doi.org/10.1016/j.elspec.2021.147093

TY - JOUR

T1 - Spectroscopic view of ultrafast charge carrier dynamics in single- and bilayer transition metal dichalcogenide semiconductors

AU - Majchrzak, Paulina

AU - Volckaert, Klara

AU - Čabo, Antonija Grubišić

AU - Biswas, Deepnarayan

AU - Bianchi, Marco

AU - Mahatha, Sanjoy K.

AU - Dendzik, Maciej

AU - Andreatta, Federico

AU - Grønborg, Signe S.

AU - Marković, Igor

AU - Riley, Jonathon M.

AU - Johannsen, Jens C.

AU - Lizzit, Daniel

AU - Bignardi, Luca

AU - Lizzit, Silvano

AU - Cacho, Cephise

AU - Alexander, Oliver

AU - Matselyukh, Dan

AU - Wyatt, Adam S.

AU - Chapman, Richard T.

AU - Springate, Emma

AU - Lauritsen, Jeppe V.

AU - King, Phil D.C.

AU - Sanders, Charlotte E.

AU - Miwa, Jill A.

AU - Hofmann, Philip

AU - Ulstrup, Søren

N1 - Funding Information: We thank Phil Rice and Alistair Cox for technical support during the Artemis beamtimes. We gratefully acknowledge funding from VILLUM FONDEN, Denmark through the Young Investigator Program (Grant. No. 15375) and the Centre of Excellence for Dirac Materials, Denmark (Grant. No. 11744), the Danish Council for Independent Research, Natural Sciences, Denmark under the Sapere Aude program (Grant Nos. DFF-9064-00057B and DFF-6108-00409). Access to the Artemis Facility was funded by STFC. I.M. acknowledges financial support by the International Max Planck Research School for Chemistry and Physics of Quantum Materials (IMPRS-CPQM). The authors also acknowledge The Royal Society and The Leverhulme Trust. Publisher Copyright: © 2021 The Author(s)

PY - 2021/7

Y1 - 2021/7

N2 - 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.

AB - 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.

KW - Bandgap renormalization

KW - Time-and angle-resolved photoemission spectroscopy

KW - Transition metal dichalcogenides

KW - Ultrafast carrier dynamics

UR - http://www.scopus.com/inward/record.url?scp=85108349218&partnerID=8YFLogxK

U2 - 10.1016/j.elspec.2021.147093

DO - 10.1016/j.elspec.2021.147093

M3 - Article

AN - SCOPUS:85108349218

SN - 0368-2048

VL - 250

JO - Journal of Electron Spectroscopy and Related Phenomena

JF - Journal of Electron Spectroscopy and Related Phenomena

M1 - 147093

ER -

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

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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