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| Main Authors: | , , , , , , , , , , , , , , , , |
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| Format: | Preprint |
| Published: |
2025
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| Subjects: | |
| Online Access: | https://arxiv.org/abs/2512.24328 |
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| _version_ | 1866917262310506496 |
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| author | Xin, Yuxiang Yu, Chen-Xin Wang, Jianru Jin, Jianbo Lai, Minliang Wang, Yinan Yan, Shuwen Chen, Gu-wen Fan, Liang Xiao, Xiachu Yang, Yutao Li, Luying Wang, Han Liu, Zhi-Pan Tang, Jiang Yang, Li-Ming Zhang, Zhuolei |
| author_facet | Xin, Yuxiang Yu, Chen-Xin Wang, Jianru Jin, Jianbo Lai, Minliang Wang, Yinan Yan, Shuwen Chen, Gu-wen Fan, Liang Xiao, Xiachu Yang, Yutao Li, Luying Wang, Han Liu, Zhi-Pan Tang, Jiang Yang, Li-Ming Zhang, Zhuolei |
| contents | The high-entropy halide-perovskite field has expanded rapidly, yet a key gap remains: configurational entropy is not yet a reliable, designable lever to co-deliver expanded photonic functionality and operational robustness with a composition-transferable mechanistic basis. Here we develop entropy-engineered rare-earth halide double-perovskite single crystals, Cs2Na(Sb, RE)Cl6 (RE3+ = Sc3+, Er3+, Yb3+, Tm3+), that simultaneously expand near-infrared (NIR) functionality and establish a mechanistic stability rule. Near-equiatomic B(III)-site alloying yields a single-phase high-entropy solid solution (Delta_Sconfig about 1.6R). Sb3+ serves as a sensitizer that unifies excitation and cooperatively activates multiple lanthanide channels, transforming the parent single-mode response into a broadband NIR output (~850-1600 nm) with three spectrally orthogonal fingerprint bands at 996, 1220, and 1540 nm. This tri-peak, self-referenced output enables redundancy-based ratiometric solvent identification and quantitative mixture sensing with reduced susceptibility to intensity drift. Accelerated aging under humidity and oxygen shows improved phase and emission stability versus single-component analogues. DFT and molecular dynamics attribute the robustness to strongly suppressed RE$^{3+}$/Cl$^-$ self-diffusion despite comparable H$_2$O/O$_2$ adsorption, kinetically impeding ion-migration-assisted reconstruction and degradation. Integration into a phosphor-converted LED delivers spectrally stable, broadband NIR illumination, establishing entropy engineering as a practical handle to couple expanded photonic functionality with mechanistically accountable durability in metal-halide photonics. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2512_24328 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | From Disorder to Function: Entropy-Engineered Broadband Photonics with Ion-Transport-Stabilized Spectral Fidelity Xin, Yuxiang Yu, Chen-Xin Wang, Jianru Jin, Jianbo Lai, Minliang Wang, Yinan Yan, Shuwen Chen, Gu-wen Fan, Liang Xiao, Xiachu Yang, Yutao Li, Luying Wang, Han Liu, Zhi-Pan Tang, Jiang Yang, Li-Ming Zhang, Zhuolei Optics Materials Science The high-entropy halide-perovskite field has expanded rapidly, yet a key gap remains: configurational entropy is not yet a reliable, designable lever to co-deliver expanded photonic functionality and operational robustness with a composition-transferable mechanistic basis. Here we develop entropy-engineered rare-earth halide double-perovskite single crystals, Cs2Na(Sb, RE)Cl6 (RE3+ = Sc3+, Er3+, Yb3+, Tm3+), that simultaneously expand near-infrared (NIR) functionality and establish a mechanistic stability rule. Near-equiatomic B(III)-site alloying yields a single-phase high-entropy solid solution (Delta_Sconfig about 1.6R). Sb3+ serves as a sensitizer that unifies excitation and cooperatively activates multiple lanthanide channels, transforming the parent single-mode response into a broadband NIR output (~850-1600 nm) with three spectrally orthogonal fingerprint bands at 996, 1220, and 1540 nm. This tri-peak, self-referenced output enables redundancy-based ratiometric solvent identification and quantitative mixture sensing with reduced susceptibility to intensity drift. Accelerated aging under humidity and oxygen shows improved phase and emission stability versus single-component analogues. DFT and molecular dynamics attribute the robustness to strongly suppressed RE$^{3+}$/Cl$^-$ self-diffusion despite comparable H$_2$O/O$_2$ adsorption, kinetically impeding ion-migration-assisted reconstruction and degradation. Integration into a phosphor-converted LED delivers spectrally stable, broadband NIR illumination, establishing entropy engineering as a practical handle to couple expanded photonic functionality with mechanistically accountable durability in metal-halide photonics. |
| title | From Disorder to Function: Entropy-Engineered Broadband Photonics with Ion-Transport-Stabilized Spectral Fidelity |
| topic | Optics Materials Science |
| url | https://arxiv.org/abs/2512.24328 |