Elimination of Interfacial‐Electrochemical‐Reaction‐Induced Polarization in Perovskite Single Crystals for Ultrasensitive and Stable X‐Ray Detector Arrays

Organic-inorganic halide perovskites have exhibited bright prospects in high-sensitivity X-ray detection. However, they generally suffer from the severe field-driven polarization issue that remarkably deteriorates the detection performance. Here, it is demonstrated that the interfacial electrochemical reaction between Au electrodes and halogen in MAPbI3 single crystals (SCs) is the major source of the dark current polarization in the metal-semiconductor-metal (MSM)-structured perovskite X-ray detectors at the initial stage of biasing. By introducing the p- and n-type charge transport layers to isolate the electrodes from contacting the SC surface, the polarization is fully eliminated under a large electric field up to 1000 V cm-1 . Moreover, the resultant lateral p-i-n heterojunction suppresses the dark current of the devices by nearly 3 orders of magnitude as compared to the MSM counterparts and therefore enables a high sensitivity of 5.2 × 106 µC Gy-1air cm-2 and a record low X-ray detection limit down to 0.1 nGyair s-1 . The excellent biasing stability and sensitivity of the devices allow to prepare the linear detector arrays for X-ray imaging applications.