Li⁺-Mediated Topological Regulation of Aluminosilicate Glass Ceramics: Near-Full Crystallinity for Multifunctional Optoelectronic Applications.

Abstract

Developing glass ceramics (GCs) with ultrahigh crystallinity and excellent optical transparency remains a formidable challenge due to the intrinsic trade-off between crystalline volume fraction and grain boundary light scattering. Herein, a Li⁺- doping mediated topological network regulation strategy is developed to address this dilemma in MgO-Al₂O₃-SiO₂ transparent GCs (TGCs). Combined experimental characterizations and molecular dynamics simulations confirm that Li⁺ acts as a network modifier to relax the rigid tetrahedral framework, tailor Al coordination, and optimize crystallization kinetics. This boosts crystallinity from 5.6 to 97.0 vol% (near-full crystallinity) while retaining high transparency via refractive index matching between the crystal and residual glass. Eu²⁺-activated high-crystallinity TGCs exhibit superior multifunctional optical performance, including a high internal quantum efficiency of 63%, good resistance to thermal quenching (82% intensity retention at 150°C), and a high x-ray light yield of 5740 photons/MeV. Their practical applicability is further validated for high-power indoor/horticultural lighting and high-resolution x-ray scintillation. This work establishes a universal topological engineering paradigm for the rational design of glass network topologies, which provides a new solution to the transparency-crystallinity trade-off in GCs and paves the way for next-generation high-performance TGCs-based optoelectronic devices.