Synergistic Effects of Ferroelectric Polarization and Biaxial Strain on Photocatalytic Properties in GaTe/In 2 Se 3 Heterostructures

Ferroelectric polarization materials have emerged as a revolutionary pathway for designing efficient heterojunction photocatalysts, offering unique advantages in manipulating charge carrier dynamics through built‐in electric fields. This study systematically investigates how the coupling of ferroelectric polarization and strain engineering modulate the electronic structure and optoelectronic properties performance of GaTe/In 2 Se 3 heterostructure (HS), aiming to establish structure–activity relationships for multifunctional optoelectronic applications. Reversible switching of band alignment in the GaTe/In 2 Se 3 HS from Type‐I to Type‐II was achieved through biaxial strain and ferroelectric polarization reversal of In 2 Se 3 between positive (+P) and negative (−P) states, driven by interfacial charge redistribution and built‐in electric field modulation. This work demonstrates that coupling ferroelectric polarization with strain engineering provides a versatile strategy to tailor HS functionalities. Synergistic ferroelectric polarization and strain engineering enable multifunctional optimization of HS, paving the way for adaptive optoelectronic catalytic devices via band alignment and carrier dynamics modulation. This study shows that ferroelectric polarization coupled with strain engineering enables effective tuning of band alignment and carrier dynamics in GaTe/In 2 Se 3 heterostructures. Polarization reversal and strain synergistically modulate interfacial electric fields, achieving reversible Type‐I/Type‐II band switching for multifunctional optoelectronic applications.