Molecular π-Extension Strategy Enables All-in-One Polar Hybrid Glass-Ceramics Integrating Multidimensional Optical Properties.

Authors

Xiong Pan, Hao Zhuo, Ming-Yu Guo, Yu-Xin Chen, Ruiqi Huang, Zi-Luo Fang, Yuefei Xiang, Qiye Liu, Jiayi Wu, Mei Pan, Wei-Xiong Zhang

Published in

Small (Weinheim an der Bergstrasse, Germany). Pages e75509. Sep 02, 2026. Epub Sep 02, 2026.

Abstract

Mastering phase transitions of molecular materials is essential for regulating their optical functionalities, yet realizing glass materials that integrate multidimensional optical properties still poses a major challenge. Herein, we report a molecular π-extension strategy to modulate phase evolution for constructing all-in-one polar hybrid glass-ceramics featuring integrated multidimensional optical properties, as demonstrated by a pair of new hybrids, (benzyltriphenylphosphonium)[ReO₄] (1) and (1-naphthylmethyltriphenylphosphonium)[ReO₄] (2). Unlike the simple melting-crystallization cycle of 1, the π-expanded bulky naphthylmethyl moiety in 2 simultaneously strengthens steric hindrance and intermolecular interactions, elevating its melting point by 52 K relative to 1 and kinetically trapping the molten state. Accordingly, 2 undergoes reversible crystal-liquid-glass-crystal phase transitions. Thermal annealing transforms the highly transparent glass phase 2-G (transmittance = 97.82% over 400-800 nm) into polar hybrid glass-ceramic 2-GC with synergistic multidimensional optical performance. All phases exhibit distinctive multiband luminescence originating from combined concurrent Kasha emission, tunable anti-Kasha emission, and low-temperature phosphorescence. Remarkably, 2-GC achieves a 1.5-fold enhancement in second-harmonic generation compared with crystalline 2, and displays the first two-photon-excited upconversion fluorescence in hybrid glass-ceramic systems. This work verifies that molecular π-extension engineering offers a robust strategy for fabricating reconfigurable, all-in-one multifunctional photonic materials with integrated multidimensional optical properties.

PMID:
42683693
Bibliographic data and abstract were imported from PubMed on 02 Sep 2026.

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