Nonuniform Chemical Passivation Dynamics in Monolayer MoS <sub>2</sub> from Real-Time Photoluminescence Imaging

Postchemical treatment is a major strategy for improving the optical and electronic performance of two-dimensional transition-metal dichalcogenides (TMDs), where surface defects and unintentional doping limit radiative recombination. Despite its broad application, the passivation dynamics in both time and space remain insufficiently understood. Here, we employ real-time, spatially resolved photoluminescence (PL) imaging to track the evolution of PL emission from monolayer MoS2 during the Li-TFSI treatment. The PL intensity increases gradually over 4.7 min, indicating reaction-limited passivation kinetics. At the same time, the spatial variation in PL becomes more pronounced, revealing position-dependent reactivity and heterogeneous treatment across the flake. Pixel-level PL statistics compared with noise-based simulations confirm that this broadening originates from the intrinsic spatial heterogeneity of the material. These results demonstrate that chemical treatment enhances radiative recombination while simultaneously amplifying pre-existing spatial differences, establishing real-time PL imaging as a sensitive approach to probing heterogeneous surface reactions in 2D semiconductors.

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Journal
The Journal of Physical Chemistry Letters
Published
2026-05-22
DOI
https://doi.org/10.1021/acs.jpclett.6c00839
Primary Topic
2D Materials and Applications
Type
article
Field-Weighted Citation Impact
0.00

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article

Nonuniform Chemical Passivation Dynamics in Monolayer MoS 2 from Real-Time Photoluminescence Imaging

Jung-In Lee, Christoph Schnedermann, Nicolas Gauriot, Z Li et al.
The Journal of Physical Chemistry Letters
2D Materials and Applications
article

Nonuniform Chemical Passivation Dynamics in Monolayer MoS 2 from Real-Time Photoluminescence Imaging

Jung-In Lee, Christoph Schnedermann, Nicolas Gauriot, Z Li, Juhwan Lim, Jiho Han, Manish Chhowalla, Akshay Rao
article en

Abstract

Postchemical treatment is a major strategy for improving the optical and electronic performance of two-dimensional transition-metal dichalcogenides (TMDs), where surface defects and unintentional doping limit radiative recombination. Despite its broad application, the passivation dynamics in both time and space remain insufficiently understood. Here, we employ real-time, spatially resolved photoluminescence (PL) imaging to track the evolution of PL emission from monolayer MoS2 during the Li-TFSI treatment. The PL intensity increases gradually over 4.7 min, indicating reaction-limited passivation kinetics. At the same time, the spatial variation in PL becomes more pronounced, revealing position-dependent reactivity and heterogeneous treatment across the flake. Pixel-level PL statistics compared with noise-based simulations confirm that this broadening originates from the intrinsic spatial heterogeneity of the material. These results demonstrate that chemical treatment enhances radiative recombination while simultaneously amplifying pre-existing spatial differences, establishing real-time PL imaging as a sensitive approach to probing heterogeneous surface reactions in 2D semiconductors.

The Journal of Physical Chemistry Letters
Uppsala University (SE), University of Cambridge (GB)
Faraday Institution, Royal Society, University of Cambridge, Wolfson Foundation, Engineering and Physical Sciences Research Council, H2020 European Research Council
Openalex Percentile: Top 11%
2D Materials and Applications
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