Vertically Oriented Quasi‐2D Perovskite Grown In‐Situ by Carbonyl Array‐Synergized Crystallization for Direct X‐Ray Detectors

Abstract Quasi‐2D perovskite quantum wells are increasingly recognized as promising candidates for direct‐conversion X‐ray detection. However, the fabrication of oriented and uniformly thick quasi‐2D perovskite films, crucial for effective high‐energy X‐ray detection, is hindered by the inherent challenges of preferential crystallization at the gas‐liquid interface, resulting in poor film quality. In addressing this limitation, a carbonyl array‐synergized crystallization (CSC) strategy is employed for the fabrication of thick films of a quasi‐2D Ruddlesden‐Popper (RP) phase perovskite, specifically PEA2MA4Pb5I16. The CSC strategy involves incorporating two forms of carbonyls in the perovskite precursor, generating large and dense intermediates. This design reduces the nucleation rate at the gas‐liquid interface, enhances the binding energies of Pb2+ at (202) and (111) planes, and passivates ion vacancy defects. Consequently, the construction of high‐quality thick films of PEA2MA4Pb5I16 RP perovskite quantum wells is achieved and characterized by vertical orientation and a pure well‐width distribution. The corresponding PEA2MA4Pb5I16 RP perovskite X‐ray detectors exhibit multi‐dimensional advantages in performance compared to previous approaches and commercially available a‐Se detectors. This CSC strategy promotes 2D perovskites as a candidate for next‐generation large‐area flat‐panel X‐ray detection systems.