Abstract
2D van der Waals ferroelectrics, particularly α-In(2)Se(3), have emerged as an attractive building block for next-generation information storage technologies due to their moderate band gap and robust ferroelectricity stabilized by dipole locking. α-In(2)Se(3) can adopt either the distorted zincblende or wurtzite structures; however, the wurtzite phase has yet to be experimentally validated, and its large-scale synthesis poses significant challenges. Here, we report an in-situ transport growth of centimeter-scale wurtzite type α-In(2)Se(3) films directly on SiO(2) substrates using a process combining pulsed laser deposition and chemical vapor deposition. We demonstrate that it is a narrow bandgap ferroelectric semiconductor, featuring a Curie temperature exceeding 620 K, a tunable bandgap (0.8-1.6 eV) modulated by charged domain walls, and a large optical absorption coefficient of 1.3 × 10(6)/cm. Moreover, light absorption promotes the dynamic conductance range, linearity, and symmetry of the synapse devices, leading to a high recognition accuracy of 92.3% in a supervised pattern classification task for neuromorphic computing. Our findings demonstrate a ferroelectric polymorphism of In(2)Se(3), highlighting its potential in ferroelectric synapses for neuromorphic computing.