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

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 s...

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Main Authors: Long Zhang, Chen Li, Dequan Jiang, Kai Wang, Guangming Niu, Laizhi Sui, Kaijun Yuan, Yonggang Wang
Format: Article
Language:English
Published: Nature Portfolio 2025-08-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-62170-6
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author Long Zhang
Chen Li
Dequan Jiang
Kai Wang
Guangming Niu
Laizhi Sui
Kaijun Yuan
Yonggang Wang
author_facet Long Zhang
Chen Li
Dequan Jiang
Kai Wang
Guangming Niu
Laizhi Sui
Kaijun Yuan
Yonggang Wang
author_sort Long Zhang
collection DOAJ
description 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.
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publisher Nature Portfolio
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series Nature Communications
spelling doaj-art-bdd99207883d41eb92182e5c1a505eda2025-08-20T04:03:00ZengNature PortfolioNature Communications2041-17232025-08-0116111010.1038/s41467-025-62170-6Brightening self-trapped exciton emission in 2D metal-organic chalcogenolates via argentophilicity-mediated anisotropic compressionLong Zhang0Chen Li1Dequan Jiang2Kai Wang3Guangming Niu4Laizhi Sui5Kaijun Yuan6Yonggang Wang7School of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversityState Key Laboratory of Superhard Materials, College of Physics, Jilin UniversityState Key Laboratory of Molecular Reaction Dynamics and Dalian Coherent Light Source, Dalian Institute of Chemical Physics, Chinese Academy of SciencesState Key Laboratory of Molecular Reaction Dynamics and Dalian Coherent Light Source, Dalian Institute of Chemical Physics, Chinese Academy of SciencesState Key Laboratory of Molecular Reaction Dynamics and Dalian Coherent Light Source, Dalian Institute of Chemical Physics, Chinese Academy of SciencesSchool of Materials Science and Engineering, Peking UniversityAbstract 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.https://doi.org/10.1038/s41467-025-62170-6
spellingShingle Long Zhang
Chen Li
Dequan Jiang
Kai Wang
Guangming Niu
Laizhi Sui
Kaijun Yuan
Yonggang Wang
Brightening self-trapped exciton emission in 2D metal-organic chalcogenolates via argentophilicity-mediated anisotropic compression
Nature Communications
title Brightening self-trapped exciton emission in 2D metal-organic chalcogenolates via argentophilicity-mediated anisotropic compression
title_full Brightening self-trapped exciton emission in 2D metal-organic chalcogenolates via argentophilicity-mediated anisotropic compression
title_fullStr Brightening self-trapped exciton emission in 2D metal-organic chalcogenolates via argentophilicity-mediated anisotropic compression
title_full_unstemmed Brightening self-trapped exciton emission in 2D metal-organic chalcogenolates via argentophilicity-mediated anisotropic compression
title_short Brightening self-trapped exciton emission in 2D metal-organic chalcogenolates via argentophilicity-mediated anisotropic compression
title_sort brightening self trapped exciton emission in 2d metal organic chalcogenolates via argentophilicity mediated anisotropic compression
url https://doi.org/10.1038/s41467-025-62170-6
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