Characterizing Interlayer Excitons by Spectral Signature in Scattering Visible Near-Field Microscopy

Interlayer excitons (IXs) in van der Waals heterostructures exhibit unique optical properties due to their spatially separated charge carriers. However, the weak oscillator strength and radiative broadening of IXs make them difficult to detect with conventional absorption spectroscopy. Here, we use scattering-type scanning near-field optical microscopy (s-SNOM) to directly probe the dielectric response at the nanoscale. We first validate this approach by measuring the B-exciton in a four-layer MoS<sub>2</sub> sample, where ion irradiation introduced defect-induced broadening. Extending this method to a MoSe<sub>2</sub>/WSe<sub>2</sub> heterostructure, we observe a Lorentzian resonance at 1.35 eV, characteristic of interlayer excitons, with broadening dominated by nonradiative decay. These results demonstrate the capability of s-SNOM to image and characterize weak excitonic resonances at the nanoscale, overcoming the limitations of conventional techniques and providing new insights into localized exciton dynamics in 2D heterostructures.

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Publication Details

Journal
The Journal of Physical Chemistry Letters
Published
2025-06-30
DOI
https://doi.org/10.1021/acs.jpclett.5c01052
Citations
2
Primary Topic
2D Materials and Applications
Type
article
Field-Weighted Citation Impact
1.04

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Characterizing Interlayer Excitons by Spectral Signature in Scattering Visible Near-Field Microscopy

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article

Characterizing Interlayer Excitons by Spectral Signature in Scattering Visible Near-Field Microscopy

Otakar Frank, Gregor Hlawacek, Iris Niehues, Anna Wróblewska, Tobias Korn, Asma S Bukhari, Patryk Kusch, Oisín Garrity, Luka Pirker, Annika Bergmann-Iwe
article en
2 citations

Abstract

Interlayer excitons (IXs) in van der Waals heterostructures exhibit unique optical properties due to their spatially separated charge carriers. However, the weak oscillator strength and radiative broadening of IXs make them difficult to detect with conventional absorption spectroscopy. Here, we use scattering-type scanning near-field optical microscopy (s-SNOM) to directly probe the dielectric response at the nanoscale. We first validate this approach by measuring the B-exciton in a four-layer MoS<sub>2</sub> sample, where ion irradiation introduced defect-induced broadening. Extending this method to a MoSe<sub>2</sub>/WSe<sub>2</sub> heterostructure, we observe a Lorentzian resonance at 1.35 eV, characteristic of interlayer excitons, with broadening dominated by nonradiative decay. These results demonstrate the capability of s-SNOM to image and characterize weak excitonic resonances at the nanoscale, overcoming the limitations of conventional techniques and providing new insights into localized exciton dynamics in 2D heterostructures.

The Journal of Physical Chemistry LettersVol. 16(27)
Warsaw University of Technology (PL), Charles University (CZ), University of Münster (DE), Helmholtz-Zentrum Dresden-Rossendorf (DE), Czech Academy of Sciences, J. Heyrovský Institute of Physical Chemistry (CZ), University of Rostock (DE), Freie Universität Berlin (DE)
Deutsche Forschungsgemeinschaft, Ministerstvo Školství, Mládeže a Tělovýchovy, Grantová Agentura České Republiky
Climate action
Openalex Percentile: Top 24%
2D Materials and Applications
1.04
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