Chalcogenide phase‐change materials (PCMs) have offered an appealing material solution by acting as a switchable dielectric layer to tune the electromagnetic properties of terahertz metamaterials and metasurfaces. Here, this work demonstrates large‐scale and lithography‐free manufacturing of all‐PCM terahertz metasurfaces based on direct laser switching of crystalline micro‐domains in a thin film with high switching ratio of the emerging plasmonic PCM, In3SbTe2 (IST). The fabricated high‐quality IST metasurfaces achieve efficient plasmonic resonances and a large modulation depth with ultrafast response (full width at half maxima of the modulation time ≈1.6 ps) in a deep‐subwavelength switching volume. For the dynamic evolution of terahertz resonance modes, theoretical modeling reveals a delicate interplay between amorphous and crystalline IST due to the bonding‐structure‐induced different carrier lifetimes and spatially localized electric fields. These studies open new avenues for realizing all‐PCM terahertz ultrafast nanophotonics.

Thermal radiation modulation facilitated by phase change materials (PCMs) necessitate a large thermal radiation contrast in broadband as well as a non-volatile phase transition, which are only partially satisfied by...