Colloidal 2D Mo1−xWxS2 nanosheets: an atomic- to ensemble-level spectroscopic study

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Authors

  • Markus Fröhlich
  • Marco Kögel
  • Jonas Hiller
  • Leo Kahlmeyer
  • Alfred J. Meixner
  • Marcus Scheele
  • Jannika Lauth
  • Jannik C. Meyer

External Research Organisations

  • University of Tübingen
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Details

Original languageEnglish
Pages (from-to)13271-13278
Number of pages8
JournalPhysical Chemistry Chemical Physics
Volume26
Issue number17
Early online date1 Apr 2024
Publication statusPublished - 2024

Abstract

Composition dependent tuning of electronic and optical properties in semiconducting two-dimensional (2D) transition metal dichalcogenide (TMDC) alloys is promising for tailoring the materials for optoelectronics. Here, we report a solution-based synthesis suitable to obtain predominantly monolayered 2D semiconducting Mo1−xWxS2 nanosheets (NSs) with controlled composition as substrate-free colloidal inks. Atomic-level structural analysis by high-angle annular dark-field (HAADF) scanning transmission electron microscopy (STEM) coupled with energy dispersive X-ray spectroscopy (EDXS) depicts the distribution of individual atoms within the Mo1−xWxS2 NSs and reveals the tendency for domain formation, especially at low molar tungsten fractions. These domains cause a broadening in the associated ensemble-level Raman spectra, confirming the extrapolation of the structural information from the microscopic scale to the properties of the entire sample. A characterization of the Mo1−xWxS2 NSs by steady-state optical spectroscopy shows that a band gap tuning in the range of 1.89-2.02 eV (614-655 nm) and a spin-orbit coupling-related exciton splitting of 0.16-0.38 eV can be achieved, which renders colloidal methods viable for upscaling low cost synthetic approaches toward application-taylored colloidal TMDCs.

Cite this

Colloidal 2D Mo1−xWxS2 nanosheets: an atomic- to ensemble-level spectroscopic study. / Fröhlich, Markus; Kögel, Marco; Hiller, Jonas et al.
In: Physical Chemistry Chemical Physics, Vol. 26, No. 17, 2024, p. 13271-13278.

Research output: Contribution to journalArticleResearchpeer review

Fröhlich, M, Kögel, M, Hiller, J, Kahlmeyer, L, Meixner, AJ, Scheele, M, Lauth, J & Meyer, JC 2024, 'Colloidal 2D Mo1−xWxS2 nanosheets: an atomic- to ensemble-level spectroscopic study', Physical Chemistry Chemical Physics, vol. 26, no. 17, pp. 13271-13278. https://doi.org/10.1039/d4cp00530a
Fröhlich, M., Kögel, M., Hiller, J., Kahlmeyer, L., Meixner, A. J., Scheele, M., Lauth, J., & Meyer, J. C. (2024). Colloidal 2D Mo1−xWxS2 nanosheets: an atomic- to ensemble-level spectroscopic study. Physical Chemistry Chemical Physics, 26(17), 13271-13278. https://doi.org/10.1039/d4cp00530a
Fröhlich M, Kögel M, Hiller J, Kahlmeyer L, Meixner AJ, Scheele M et al. Colloidal 2D Mo1−xWxS2 nanosheets: an atomic- to ensemble-level spectroscopic study. Physical Chemistry Chemical Physics. 2024;26(17):13271-13278. Epub 2024 Apr 1. doi: 10.1039/d4cp00530a
Fröhlich, Markus ; Kögel, Marco ; Hiller, Jonas et al. / Colloidal 2D Mo1−xWxS2 nanosheets : an atomic- to ensemble-level spectroscopic study. In: Physical Chemistry Chemical Physics. 2024 ; Vol. 26, No. 17. pp. 13271-13278.
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title = "Colloidal 2D Mo1−xWxS2 nanosheets: an atomic- to ensemble-level spectroscopic study",
abstract = "Composition dependent tuning of electronic and optical properties in semiconducting two-dimensional (2D) transition metal dichalcogenide (TMDC) alloys is promising for tailoring the materials for optoelectronics. Here, we report a solution-based synthesis suitable to obtain predominantly monolayered 2D semiconducting Mo1−xWxS2 nanosheets (NSs) with controlled composition as substrate-free colloidal inks. Atomic-level structural analysis by high-angle annular dark-field (HAADF) scanning transmission electron microscopy (STEM) coupled with energy dispersive X-ray spectroscopy (EDXS) depicts the distribution of individual atoms within the Mo1−xWxS2 NSs and reveals the tendency for domain formation, especially at low molar tungsten fractions. These domains cause a broadening in the associated ensemble-level Raman spectra, confirming the extrapolation of the structural information from the microscopic scale to the properties of the entire sample. A characterization of the Mo1−xWxS2 NSs by steady-state optical spectroscopy shows that a band gap tuning in the range of 1.89-2.02 eV (614-655 nm) and a spin-orbit coupling-related exciton splitting of 0.16-0.38 eV can be achieved, which renders colloidal methods viable for upscaling low cost synthetic approaches toward application-taylored colloidal TMDCs.",
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T1 - Colloidal 2D Mo1−xWxS2 nanosheets

T2 - an atomic- to ensemble-level spectroscopic study

AU - Fröhlich, Markus

AU - Kögel, Marco

AU - Hiller, Jonas

AU - Kahlmeyer, Leo

AU - Meixner, Alfred J.

AU - Scheele, Marcus

AU - Lauth, Jannika

AU - Meyer, Jannik C.

N1 - Funding Information: Financial support of this work has been provided by the German Research Foundation (DFG) under grant SCHE1905/9-1 (project no. 426008387), and ME3313-6 (project no. 500512256). J. L. gratefully acknowledges funding under the Excellence Strategy within the Cluster of Excellence PhoenixD (EXC 2122, Project ID 390833453) and funding by an Athene Grant of the University of Tübingen (by the Federal Ministry of Education and Research (BMBF) and the Baden-Württemberg Ministry of Science as part of the Excellence Strategy of the German Federal and State Governments).

PY - 2024

Y1 - 2024

N2 - Composition dependent tuning of electronic and optical properties in semiconducting two-dimensional (2D) transition metal dichalcogenide (TMDC) alloys is promising for tailoring the materials for optoelectronics. Here, we report a solution-based synthesis suitable to obtain predominantly monolayered 2D semiconducting Mo1−xWxS2 nanosheets (NSs) with controlled composition as substrate-free colloidal inks. Atomic-level structural analysis by high-angle annular dark-field (HAADF) scanning transmission electron microscopy (STEM) coupled with energy dispersive X-ray spectroscopy (EDXS) depicts the distribution of individual atoms within the Mo1−xWxS2 NSs and reveals the tendency for domain formation, especially at low molar tungsten fractions. These domains cause a broadening in the associated ensemble-level Raman spectra, confirming the extrapolation of the structural information from the microscopic scale to the properties of the entire sample. A characterization of the Mo1−xWxS2 NSs by steady-state optical spectroscopy shows that a band gap tuning in the range of 1.89-2.02 eV (614-655 nm) and a spin-orbit coupling-related exciton splitting of 0.16-0.38 eV can be achieved, which renders colloidal methods viable for upscaling low cost synthetic approaches toward application-taylored colloidal TMDCs.

AB - Composition dependent tuning of electronic and optical properties in semiconducting two-dimensional (2D) transition metal dichalcogenide (TMDC) alloys is promising for tailoring the materials for optoelectronics. Here, we report a solution-based synthesis suitable to obtain predominantly monolayered 2D semiconducting Mo1−xWxS2 nanosheets (NSs) with controlled composition as substrate-free colloidal inks. Atomic-level structural analysis by high-angle annular dark-field (HAADF) scanning transmission electron microscopy (STEM) coupled with energy dispersive X-ray spectroscopy (EDXS) depicts the distribution of individual atoms within the Mo1−xWxS2 NSs and reveals the tendency for domain formation, especially at low molar tungsten fractions. These domains cause a broadening in the associated ensemble-level Raman spectra, confirming the extrapolation of the structural information from the microscopic scale to the properties of the entire sample. A characterization of the Mo1−xWxS2 NSs by steady-state optical spectroscopy shows that a band gap tuning in the range of 1.89-2.02 eV (614-655 nm) and a spin-orbit coupling-related exciton splitting of 0.16-0.38 eV can be achieved, which renders colloidal methods viable for upscaling low cost synthetic approaches toward application-taylored colloidal TMDCs.

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U2 - 10.1039/d4cp00530a

DO - 10.1039/d4cp00530a

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VL - 26

SP - 13271

EP - 13278

JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

SN - 1463-9076

IS - 17

ER -

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