Colloidal 2D Mo1−xWxS2 nanosheets

an atomic- to ensemble-level spectroscopic study

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

Organisation(s)
PhoenixD: Photonics, Optics, and Engineering - Innovation Across Disciplines
External Organisation(s)
University of Tübingen
Type
Article
Journal
Physical Chemistry Chemical Physics
Volume
26
Pages
13271-13278
No. of pages
8
ISSN
1463-9076
Publication date
2024
Publication status
Published
Peer reviewed
Yes
ASJC Scopus subject areas
Physics and Astronomy(all), Physical and Theoretical Chemistry
Electronic version(s)
https://doi.org/10.1039/d4cp00530a (Access: Open)