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The recently reported two-dimensional lead halide perovskites have attracted much attention in high-energy radiation detector applications due to its high structural stability and low ion migration. However, the increased exciton binding energy and the charge transport barrier resulting from the A-site cation can easily limit the charge extraction and device performance. As an emerging material in high-energy detection field, guanidinium {GA+ = [C(NH2)3]+} is a relatively large organic cation composed of three amino groups, which can enhance the hydrogen bond formation and the van der Waals interactions with the metal halide framework. Meanwhile, the polymer symmetry of GA+ cation leads to almost zero dipole moments, excellent electronic properties, and high thermodynamic stability. However, there is a lack of report on the preparation, structure, and properties of GA-based 2D perovskite single crystals as well as their applications in x-ray detection. Herein, we have synthesized large-size two-dimensional GA2PbI4 single crystals with a bandgap of 2.28 eV by cooling crystallization and applied them to x-ray detectors. GA2PbI4 single crystals exhibit a high μτ product of 7.5 × 10−4 cm2 V−1 and a low trap density of 6.44 × 108 cm−3. An effective x-ray photoresponse was realized with a sensitivity as high as 392.4 μC Gyair−1 cm−2. The unique structure and excellent charge transport properties of GA+ organic cations exhibit promising prospects in high-performance x-ray detection. [ABSTRACT FROM AUTHOR]

Two-dimensional (2D) perovskites have been demonstrated great promise in x-ray detection application because of their stability, tunability, and the unique electronic properties. The centimeter-sized 2D perovskite (PMA)2PbI4 single crystal and the corresponding x-ray detector were fabricated. The Cu ion implanted device exhibits an excellent sensitivity of 283 μC Gyair−1 cm−2, the significantly enhanced mobility-lifetime (μτ) product of 8.05 × 10−3 cm2 V−1, and the lowest detectable dose rate of 2.13 μGyair s−1. Experimental observation combined with the DFT calculations shows that the improvement in Cu ion implanted x-ray detection is ascribed to the enhanced photoinduced charge carrier density and μτ product, and the increased carrier dissociation capability associated deeply with the decreased binding energy of exciton in the inorganic layer quasi-quantum well. The incorporation of the Cu interstitials by high-energy Cu ion implantation is able to introduce the donor and acceptor states with additional charge transfer channeling, resulting in the decreased exciton binding energy and fast dissociation of the exciton and the quick carrier extraction. Cu ion implantation regulating the dissociation of charge carriers in low-dimensional perovskites will motivate the application for 2D perovskite in high-performance x-ray detectors. [ABSTRACT FROM AUTHOR]