Dion–Jacobson Phase Perovskite Crystal Assembled by π‐Conjugated Aromatic Spacer for X‐Ray Detectors with an Ultralow Detection Limit

Abstract 2D Dion–Jacobson (DJ) perovskites recently have attracted extensive attention for X‐ray detection owing to their structural rigidity and environmental stability. The chemical incorporation of π‐conjugation aromatic spacing cations into DJ phase perovskites will increase the rigidity of cation and electron cloud density between adjacent inorganic slabs, thus facilitating structural rigidity and charge transport. However, it is still a challenge to synthesize high‐quality single crystals of DJ phase perovskite with aromatic spacers for detecting X‐ray applications. Here, a new DJ phase perovskite by introducing π‐conjugated aromatic cation spacer, (4ABA)PbI₄ (1, 4ABA = 4‐aminobenzylamine), eliminating the van der Waals gap is designed. High‐quality single crystals of 1 are grown via the facile solution method, exhibiting high resistivity (1.97 × 10¹¹ Ω cm), low trap density (3.36 × 10⁹ cm⁻³), and large carrier mobility‐lifetime product (1.03 × 10⁻³ cm² V⁻¹) under X‐ray illumination. Such remarkable physical characteristics endow single crystal 1 detector with high‐performance X‐ray detection including a high sensitivity of 572 µC Gy_air⁻¹cm⁻², an ultralow detection limit of 7.50 nGy_air s⁻¹ and exceptional radiation stability. The X‐ray detection limit of 1 is over 700 times lower than that of routine medical diagnosis (5500 nGy_air s⁻¹), demonstrating potential applications in medical examination.