Proton‐Transfer Ferroelectrics With High Switching Endurance

Reliable organic ferroelectrics for memory applications require high endurance under repeated electrical switching. Here we demonstrate robust fatigue resistance in highly crystalline 2‐methylbenzimidazole (MBI) films grown by low‐temperature deposition followed by restrained crystallization (LDRC) on interdigital electrodes. Switching kinetics analyzed using the Kolmogorov–Avrami–Ishibashi (KAI) model reveals characteristic millisecond switching times and quasi‐one‐dimensional domain growth associated with proton transfer along hydrogen‐bond chains. Guided by these kinetics, we examined the switching endurance under a stringent protocol that ensures complete polarization reversal. After ~10 8 continuous cycles (~2 weeks), the remanent polarization shows a small initial wake‐up behavior (~10% increase within the first 10 4 cycles), followed by stabilization at values close to the initial polarization, indicating robust ferroelectric endurance under prolonged electrical cycling. The combination of LDRC‐enabled high crystallinity and localized proton‐transfer switching, which introduces minimal structural perturbation during polarization reversal, may have enabled this fatigue tolerance and highlight MBI as a simple, fluorine‐free platform for durable organic ferroelectric devices.