Single-pulse lithography of amorphous photonic architectures inside all-inorganic dielectric crystals

High-efficiency light modulation within transparent substrates is critically important for advancing in-chip integrated optical technologies. However, current micro/nanophotonic platforms primarily rely on 2D surface configurations, rendering them inadequate for 3D optical design in dielectric environments. Here, we introduce a precise phase-transition technique that enables the direct lithography of highly regular amorphous units in multiple transparent dielectric crystals (lithium niobates, quartz, yttrium vanadate, etc.). This unit can be rapidly written with a single ultrafast laser pulse, exhibiting a high-purity amorphization phase transition interior structure and a regular sheet-like anisotropic spatial morphology (aspect ratio reaching 190:1). We reveal that this amorphization stems from ultrafast laser-driven anisotropic thermal deposition, achieved through the synergy of the light-induced high-density free electrons and thermal effects. Such embedded units achieve more than an order of magnitude improvement in the efficiency of nonlinear beam shaping (~3% second harmonic and ~0.1% third harmonic) and offer multiple degrees of freedom for device design. This study establishes a versatile platform for on-demand production of all-dielectric micro/nanophotonic architectures in the free space of transparent dielectrics, unlocking new avenues for 3D integrated photonics.