Electronic Structure of Colloidal 2H-MoS2 Mono and Bilayers Determined by Spectroelectrochemistry

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Autoren

  • Kai M. Wurst
  • Onno Strolka
  • Jonas Hiller
  • Jakob Keck
  • Alfred J. Meixner
  • Jannika Lauth
  • Marcus Scheele
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Details

OriginalspracheEnglisch
Aufsatznummer2207101
FachzeitschriftSMALL
Jahrgang19
Ausgabenummer23
Frühes Online-Datum9 März 2023
PublikationsstatusVeröffentlicht - 7 Juni 2023

Abstract

The electronic structure of mono and bilayers of colloidal 2H-MoS2 nanosheets synthesized by wet-chemistry using potential-modulated absorption spectroscopy (EMAS), differential pulse voltammetry, and electrochemical gating measurements is investigated. The energetic positions of the conduction and valence band edges of the direct and indirect bandgap are reported and observe strong bandgap renormalization effects, charge screening of the exciton, as well as intrinsic n-doping of the as-synthesized material. Two distinct transitions in the spectral regime associated with the C exciton are found, which overlap into a broad signal upon filling the conduction band. In contrast to oxidation, the reduction of the nanosheets is largely reversible, enabling potential applications for reductive electrocatalysis. This work demonstrates that EMAS is a highly sensitive tool for determining the electronic structure of thin films with a few nanometer thicknesses and that colloidal chemistry affords high-quality transition metal dichalcogenide nanosheets with an electronic structure comparable to that of exfoliated samples.

ASJC Scopus Sachgebiete

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Electronic Structure of Colloidal 2H-MoS2 Mono and Bilayers Determined by Spectroelectrochemistry. / Wurst, Kai M.; Strolka, Onno; Hiller, Jonas et al.
in: SMALL, Jahrgang 19, Nr. 23, 2207101, 07.06.2023.

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Wurst, KM, Strolka, O, Hiller, J, Keck, J, Meixner, AJ, Lauth, J & Scheele, M 2023, 'Electronic Structure of Colloidal 2H-MoS2 Mono and Bilayers Determined by Spectroelectrochemistry', SMALL, Jg. 19, Nr. 23, 2207101. https://doi.org/10.1002/smll.202207101
Wurst, K. M., Strolka, O., Hiller, J., Keck, J., Meixner, A. J., Lauth, J., & Scheele, M. (2023). Electronic Structure of Colloidal 2H-MoS2 Mono and Bilayers Determined by Spectroelectrochemistry. SMALL, 19(23), Artikel 2207101. https://doi.org/10.1002/smll.202207101
Wurst KM, Strolka O, Hiller J, Keck J, Meixner AJ, Lauth J et al. Electronic Structure of Colloidal 2H-MoS2 Mono and Bilayers Determined by Spectroelectrochemistry. SMALL. 2023 Jun 7;19(23):2207101. Epub 2023 Mär 9. doi: 10.1002/smll.202207101
Wurst, Kai M. ; Strolka, Onno ; Hiller, Jonas et al. / Electronic Structure of Colloidal 2H-MoS2 Mono and Bilayers Determined by Spectroelectrochemistry. in: SMALL. 2023 ; Jahrgang 19, Nr. 23.
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abstract = "The electronic structure of mono and bilayers of colloidal 2H-MoS2 nanosheets synthesized by wet-chemistry using potential-modulated absorption spectroscopy (EMAS), differential pulse voltammetry, and electrochemical gating measurements is investigated. The energetic positions of the conduction and valence band edges of the direct and indirect bandgap are reported and observe strong bandgap renormalization effects, charge screening of the exciton, as well as intrinsic n-doping of the as-synthesized material. Two distinct transitions in the spectral regime associated with the C exciton are found, which overlap into a broad signal upon filling the conduction band. In contrast to oxidation, the reduction of the nanosheets is largely reversible, enabling potential applications for reductive electrocatalysis. This work demonstrates that EMAS is a highly sensitive tool for determining the electronic structure of thin films with a few nanometer thicknesses and that colloidal chemistry affords high-quality transition metal dichalcogenide nanosheets with an electronic structure comparable to that of exfoliated samples.",
keywords = "colloidal synthesized 2H-MoS, differential pulse voltammetry, potential-dependent conductivity, potential-modulated absorption spectroscopy, thin films",
author = "Wurst, {Kai M.} and Onno Strolka and Jonas Hiller and Jakob Keck and Meixner, {Alfred J.} and Jannika Lauth and Marcus Scheele",
note = "Funding Information: The authors thank Andr{\'e} Niebur, excellence cluster PhoenixD, and the Institute of Physical Chemistry and Electrochemistry, Hannover for performing TEM measurements. Distilled solvents used for electrochemical experiments were kindly provided by Florian Fetzer and Andreas Schnepf, Institute of Inorganic Chemistry, University of T{\"u}bingen. The authors thank Elke Nadler, Institute of Physical and Theoretical Chemistry, University of T{\"u}bingen, for performing SEM/EDX measurements using a Hitachi SU 8030 SEM, which was funded by the DFG under the contract INST 37/829‐1 FUGG. The glass and metal workshops of the Central Chemistry Institute, University of T{\"u}bingen, are acknowledged for the fabrication of many components used in the measurement setups. J.L. is thankful for funding from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy within the Cluster of Excellence PhoenixD (EXC2122, Project ID 390833453). Financial support for this work was provided by the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (grant agreement No 802822), as well as the DFG under grant SCHE1905/9‐1. ",
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Download

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T1 - Electronic Structure of Colloidal 2H-MoS2 Mono and Bilayers Determined by Spectroelectrochemistry

AU - Wurst, Kai M.

AU - Strolka, Onno

AU - Hiller, Jonas

AU - Keck, Jakob

AU - Meixner, Alfred J.

AU - Lauth, Jannika

AU - Scheele, Marcus

N1 - Funding Information: The authors thank André Niebur, excellence cluster PhoenixD, and the Institute of Physical Chemistry and Electrochemistry, Hannover for performing TEM measurements. Distilled solvents used for electrochemical experiments were kindly provided by Florian Fetzer and Andreas Schnepf, Institute of Inorganic Chemistry, University of Tübingen. The authors thank Elke Nadler, Institute of Physical and Theoretical Chemistry, University of Tübingen, for performing SEM/EDX measurements using a Hitachi SU 8030 SEM, which was funded by the DFG under the contract INST 37/829‐1 FUGG. The glass and metal workshops of the Central Chemistry Institute, University of Tübingen, are acknowledged for the fabrication of many components used in the measurement setups. J.L. is thankful for funding from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy within the Cluster of Excellence PhoenixD (EXC2122, Project ID 390833453). Financial support for this work was provided by the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (grant agreement No 802822), as well as the DFG under grant SCHE1905/9‐1.

PY - 2023/6/7

Y1 - 2023/6/7

N2 - The electronic structure of mono and bilayers of colloidal 2H-MoS2 nanosheets synthesized by wet-chemistry using potential-modulated absorption spectroscopy (EMAS), differential pulse voltammetry, and electrochemical gating measurements is investigated. The energetic positions of the conduction and valence band edges of the direct and indirect bandgap are reported and observe strong bandgap renormalization effects, charge screening of the exciton, as well as intrinsic n-doping of the as-synthesized material. Two distinct transitions in the spectral regime associated with the C exciton are found, which overlap into a broad signal upon filling the conduction band. In contrast to oxidation, the reduction of the nanosheets is largely reversible, enabling potential applications for reductive electrocatalysis. This work demonstrates that EMAS is a highly sensitive tool for determining the electronic structure of thin films with a few nanometer thicknesses and that colloidal chemistry affords high-quality transition metal dichalcogenide nanosheets with an electronic structure comparable to that of exfoliated samples.

AB - The electronic structure of mono and bilayers of colloidal 2H-MoS2 nanosheets synthesized by wet-chemistry using potential-modulated absorption spectroscopy (EMAS), differential pulse voltammetry, and electrochemical gating measurements is investigated. The energetic positions of the conduction and valence band edges of the direct and indirect bandgap are reported and observe strong bandgap renormalization effects, charge screening of the exciton, as well as intrinsic n-doping of the as-synthesized material. Two distinct transitions in the spectral regime associated with the C exciton are found, which overlap into a broad signal upon filling the conduction band. In contrast to oxidation, the reduction of the nanosheets is largely reversible, enabling potential applications for reductive electrocatalysis. This work demonstrates that EMAS is a highly sensitive tool for determining the electronic structure of thin films with a few nanometer thicknesses and that colloidal chemistry affords high-quality transition metal dichalcogenide nanosheets with an electronic structure comparable to that of exfoliated samples.

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KW - differential pulse voltammetry

KW - potential-dependent conductivity

KW - potential-modulated absorption spectroscopy

KW - thin films

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DO - 10.1002/smll.202207101

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JO - SMALL

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SN - 1613-6810

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M1 - 2207101

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