AbstractTransparent glass‐ceramics, merging the attributes of both glass and ceramics, have diverse applications in ballistic protection, armor materials, dentistry, light‐emitting diode, and optical domains. A limitation of conventional methods for glass‐ceramic fabrication is their inadequacy in precisely controlling the morphology of crystallization, consequently constraining their prospective advancements in diverse areas. Here, a method that facilitates precise control over the formation and growth of polarization‐dependent nonperiodic anisotropic nanocrystals, with a short axis ranging from 15 to 280 nm, in Li2O‐Al2O3‐SiO2 (LAS) glass is proposed. The method utilizes the principles of near‐field anisotropy between light and matter, building upon the classical nucleation‐growth model of glass crystallization. Notably, the glass‐ceramics possessing laser‐induced nanocrystals within the Rayleigh size regime showcase an impressive 99.7% transmittance in the visible and near‐infrared wavelengths. Additionally, the glass‐ceramics with non‐periodic anisotropic nanocrystals macroscopically exhibit form‐birefringence properties, thus enabling transparent optical applications, such as polarization elements, geometric phase elements, and multi‐dimensional optical data storage. This work opens up new avenues for morphological manipulation of nanocrystallization, with potential applications in optics, nanophotonics, functional glass‐ceramics, and high mechanical performance devices.
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