“…[ 1,12,14–16,33,37–39 ] Recent activities have demonstrated how their crystallization behavior can be tailored through composition, morphology, and microstructural modification. [ 28,33–38,40–44 ] Recently, composites based upon Ge‐As‐Pb‐Se chalcogenide glasses have been shown to yield high refractive index Pb‐containing nanocrystalline phases in an amorphous matrix which can remain stable at elevated temperatures or under photo/electronically excited states. [ 28,33–37,40–44 ] In the present approach, we exploit this simple yet effective process to transform multicomponent GeSe 2 ‐As 2 Se 3 ‐PbSe (GAP‐Se) bulk glasses from an amorphous structure into an optical nanocomposite where the volume fraction of high refractive index Pb‐rich nanocrystals is spatially varied in a low refractive index amorphous matrix, thereby realizing a GRIN structure with smoothly varying index and dispersion properties.…”