A Novel Polar Zinc‐Based Hybrid Material: Structure, Properties, and Memristive Performance

Memristors are promising components for neuromorphic computing because of their resistive switching and synaptic functionalities, enabling more energy‐efficient computing architectures. Lead halide perovskites are attractive memristive materials due to their coupled ionic‐electronic conductivity, but lead toxicity limits their practical use. Herein, we report a new lead‐free hybrid zinc halide, (CHA) ₂ [ZnI ₄ ] (CHA = cyclohexylammonium), synthesized through a simple, scalable, and environmentally friendly route. Single‐crystal X‐ray diffraction shows that the compound crystallizes in a noncentrosymmetric structure composed of isolated (ZnI ₄ ) ²⁻ tetrahedra separated by CHA cations, resembling Ruddlesden–Popper phases despite its zero‐dimensional nature. Although the material is polar, no ferroelectric behavior is observed due to dominant electrical losses, likely related to its relatively narrow 2.3 eV bandgap. Memristors based on (CHA) ₂ [ZnI ₄ ] exhibit stable and reproducible electroforming‐free resistive switching at low voltages, together with short‐ and long‐term synaptic plasticity under pulsed bias. These results establish (CHA) ₂ [ZnI ₄ ] as a promising sustainable material for memory and neuromorphic applications and demonstrate the potential of Zn‐based hybrid halides for advanced electronic devices.