Dielectric Relaxation and Dielectric Switching Behaviors in (N,N‐Diisopropylethylamine) Tetrachloroantimonate(III)

Dielectric switches have drawn renewed attention to the study of their many potential applications with the adjustable switch temperatures (Ts). Herein, a novel antimony‐based halide semiconductor, (N,N‐diisopropylethylamine) tetrachloroantimonate ((DIPEA)SbCl4, DIPEA+=N,N‐diisopropylethylamine), with dielectric relaxation behavior and dielectric switches has been successfully synthesized. This compound, consisting of coordinated anion SbCl4∞- ${{\left[{{\rm S}{\rm b}{\rm C}{\rm l}}_{4}\right]}_{\infty }^{-}}$ chains and isolated DIPEA+ cations, undergoes an isostructural order‐disorder phase transition and shows a step‐like dielectric anomaly, which can function as a frequency‐tuned dielectric switch with highly adjustable switch temperature (Ts). Variable‐temperature single‐crystal structure analyses and first‐principles molecular dynamics simulations give information about the general mechanisms of molecular dynamics. This work enriches the dielectric switch family and proves that hybrid metal halides are promising candidates for switchable physical or chemical properties. Dielectric relaxation and dielectric switching behaviors of a novel antimony‐based halide semiconductor are characterized by experiments and first‐principles molecular dynamics simulations. It contains a 1D chain, undergoes an isostructural order‐disorder phase transition and shows a step‐like dielectric anomaly, which can function as a frequency‐tuned dielectric switch with highly adjustable switch temperature.