Synergetic Electrostatic and Steric Effects in α‐FAPbI3 Single Crystals For X‐Ray Detection and Imaging

Abstract

AbstractIt is still challenging to stabilize α‐FAPbI3 perovskite for high performance optoelectrical devices. Herein, a novel strategy is proposed utilizing the synergetic electrostatic and steric effect to stabilize the α‐FAPbI3 phase and suppress the ion migration. Dimethylamine (DMA+) cations are chosen as the dopant to fabricate FA0.96DMA0.04PbI3 single crystals (SCs). DFT calculations reveal that DMA+ cations can improve the stability of α‐FAPbI3 phase in both thermodynamics (lower Gibbs free energy) and kinetics (higher defect formation and migration energy). The resulting SCs exhibit an environmental stability over 100 days and an extraordinary low dark current drift of 3.7 × 10−7 nA cm−1 s−1 V−1, comparable to 2D perovskite SCs. The X‐ray detectors have also achieved the‐state‐of‐the‐art performance in X‐ray detection and imaging. This work demonstrates the significance of electrostatic and steric effects in improving the phase and operational stability of perovskites.