Temperature‐Regulated Dynamic Phase Reconfiguration of Solid‐Liquid Biphasic Ga‐In Nanoparticles

ABSTRACT Phase evolution in liquid metals (LMs) is fundamental to the structural integrity and electrical reliability of LM‐based flexible conductive materials. Physical vapor deposition (PVD) is an important method for preparing LM films. However, their phase evolution during deposition, particularly under nonequilibrium conditions, remains poorly understood. Here, we report an unexpected kinetically driven pathway for Ga‐In alloy deposition, leading to the formation of solid‐liquid biphasic nanoparticles. Contrary to the ideal homogeneous co‐deposition pathway, In preferentially nucleates on the substrate to form solid cores, while liquid Ga subsequently encapsulates them, resulting in core–shell nanoparticles that are stable at room‐temperature. These metastable structures exhibit reversible thermal reconfiguration, transitioning into a homogeneous mixing state upon heating and re‐establishing phase separation at –90°C. As deposition proceeds, the system evolves continuously from discrete biphasic nanoparticles to continuous LM films. This work reveals a previously overlooked nonequilibrium growth mechanism governing multicomponent LM deposition and establishes a general strategy for constructing phase‐separated, thermally reconfigurable metallic architectures. The findings open new opportunities for adaptive conductors and flexible electronic materials.