Brightening self-trapped exciton emission in 2D metal-organic chalcogenolates via argentophilicity-mediated anisotropic compression

Long Zhang, Chen Li, Dequan Jiang, Kai Wang, Guangming Niu, Laizhi Sui (), Kaijun Yuan and Yonggang Wang ()
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Long Zhang: Peking University
Chen Li: Peking University
Dequan Jiang: Peking University
Kai Wang: Jilin University
Guangming Niu: Chinese Academy of Sciences
Laizhi Sui: Chinese Academy of Sciences
Kaijun Yuan: Chinese Academy of Sciences
Yonggang Wang: Peking University

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract An emerging class of two-dimensional semiconductor materials, metal-organic chalcogenolates (MOCs), have garnered significant attention due to the strong excitonic effects arising from their intrinsic soft, hybrid multiquantum-well structures. However, modifying excitonic transitions that strongly couple to the argentophilic networks and constructing their structure-property relationships in MOCs remain daunting challenges. Here, we use silver phenylselenolate (AgSePh) as a model system to manipulate excitonic behavior and uncover the fundamental photophysical mechanisms through pressure engineering. A bright broadband Stokes-shifted emission is observed in AgSePh crystals along with the disappearance of blue narrow emission upon compression, which is attributed to the pressure-induced carrier transformation from free exciton to self-trapping exciton states. The considerable compressibility of the Ag-Se inorganic monolayer, driven by weakly bound argentophilic interactions, generates pronounced argentophilic intralayer distortion while simultaneously enhancing exciton-phonon coupling and excitonic oscillator strength. This work demonstrates the remarkable tunability of excitonic properties in layered MOCs.

Date: 2025
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DOI: 10.1038/s41467-025-62170-6

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