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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. [ABSTRACT FROM AUTHOR]

Crystalline organic–inorganic hybrids, which exhibit colorimetric responses to ionizing radiation, have recently been recognized as promising alternatives to conventional X‐ray dosimeters. However, X‐ray‐responsive organic–inorganic hybrids are scarce and the strategy to fine‐tune their detection sensitivity remains elusive. Herein, an unprecedented mixed‐ligand strategy is reported to modulate the X‐ray detection efficacy of organic–inorganic hybrids. Deliberately blending the stimuli‐responsive terpyridine carboxylate ligand (tpc−) and the auxiliary pba− group with different ratios gives rise to two OD thorium‐bearing clusters (Th‐102 and Th‐103) and a 1D coordination polymer (Th‐104). Notably, distinct X‐ray sensitivity is evident as a function of molar ratio of the tpc− ligand, following the trend of Th‐102 > Th‐103 > Th‐104. Moreover, Th‐102, which is exclusively built from the tpc− ligands with the highest degree of π–π interactions, exhibits the most sensitive radiochromic and fluorochromic responses toward X‐ray with the lowest detection limit of 1.5 mGy. The study anticipates that this mixed‐ligand strategy will be a versatile approach to tune the X‐ray sensing efficacy of organic–inorganic hybrids. [ABSTRACT FROM AUTHOR]

High‐resolution X‐ray imaging is increasingly required for medical diagnosis and large‐area detection. However, the issues of scattering and optical crosstalk are limiting the spatial resolution of the indirect X‐ray imaging. In this study, a feasible and efficient strategy is proposed to in situ synthesize flexible Cs3Cu2I5:2%In+@paper as a superior scintillator film, which can be scaled up to an ultra‐large area of 4800 cm2. The as‐obtained Cs3Cu2I5:2%In+@paper performs a fascinating photoluminescence quantum efficiency up to 88.14%, a steady state light yield of 70169 photons/MeV, and spatial resolution of 15 lp mm−1. Moreover, the suppressed physical scattering and optical crosstalk of the corresponding film are demonstrated. Accordingly, this work explores a feasible fabrication of customizable scintillation films with large area for high‐resolution X‐ray detection. [ABSTRACT FROM AUTHOR]

Lead halide perovskites have made remarkable progress in the field of radiation detection owing to the excellent and unique optoelectronic properties. However, the instability and the toxicity of lead‐based perovskites have greatly hindered its practical applications. Alternatively, lead‐free perovskites with high stability and environmental friendliness thus have fascinated significant research attention for direct X‐ray detection. In this review, the current research progress of X‐ray detectors based on lead‐free halide perovskites is focused. First, the synthesis methods of lead‐free perovskites including single crystals and films are discussed. In addition, the properties of these materials and the detectors, which can provide a better understanding and designing satisfactory devices are also presented. Finally, the challenge and outlook for developing high‐performance lead‐free perovskite X‐ray detectors are also provided. [ABSTRACT FROM AUTHOR]

Broadband photodetectors (PDs) with low detection limits hold significant importance to next‐generation optoelectronic devices. However, simultaneously detecting broadband (i.e., X‐ray to visible regimes) and weak lights in a single semiconducting material remains highly challenging. Here, by alloying iodine‐substituted short‐chain cations into the 3D FAPbI3 (FA = formamidine), a new 2D bilayered lead iodide hybrid perovskite, (2IPA)2FAPb2I7 (1, 2IPA = 2‐iodopropylammonium), that enables addressing this challenge is reported. Such a 2D multilayered structure and lead iodide composition jointly endow 1 with a minimized dark current (6.04 pA), excellent electrical property, and narrow bandgap (2.03 eV), which further gives it great potential for detecting broadband weak lights. Consequently, its high‐quality single crystal PDs exhibit remarkable photoresponses to weak ultraviolet–visible lights (377–637 nm) at several tens of nW cm−2 with high responsivities (>102 mA W−1) and significant detectivities (>1012 Jones). Moreover, 1 has an excellent X‐ray detection performance with a high sensitivity of 438 µC Gy−1 cm−2 and an ultralow detection limit of 20 nGy s−1. These exceptional attributes make 1 a promising material for broadband weak lights detection, which also sheds light on future explorations of high‐performance PDs based on 2D hybrid perovskites. [ABSTRACT FROM AUTHOR]

Abstract Broadband photodetectors (PDs) with low detection limits hold significant importance to next‐generation optoelectronic devices. However, simultaneously detecting broadband (i.e., X‐ray to visible regimes) and weak lights in a single semiconducting material remains highly challenging. Here, by alloying iodine‐substituted short‐chain cations into the 3D FAPbI3 (FA = formamidine), a new 2D bilayered lead iodide hybrid perovskite, (2IPA)2FAPb2I7 (1, 2IPA = 2‐iodopropylammonium), that enables addressing this challenge is reported. Such a 2D multilayered structure and lead iodide composition jointly endow 1 with a minimized dark current (6.04 pA), excellent electrical property, and narrow bandgap (2.03 eV), which further gives it great potential for detecting broadband weak lights. Consequently, its high‐quality single crystal PDs exhibit remarkable photoresponses to weak ultraviolet–visible lights (377–637 nm) at several tens of nW cm−2 with high responsivities (>102 mA W−1) and significant detectivities (>1012 Jones). Moreover, 1 has an excellent X‐ray detection performance with a high sensitivity of 438 µC Gy−1 cm−2 and an ultralow detection limit of 20 nGy s−1. These exceptional attributes make 1 a promising material for broadband weak lights detection, which also sheds light on future explorations of high‐performance PDs based on 2D hybrid perovskites.

Semiconductor‐based X‐ray detectors with low detectable thresholds become critical in medical radiography applications. However, their performance is generally limited by intrinsic defects or unresolved issues of materials, and developing a novel scintillation semiconductor for low‐dose X‐ray detection is a highly urgent objective. Herein, a high‐quality rare‐earth iodate Tm(IO3)3 single crystal grown through low‐cost solution processing is reported with a wide bandgap of 4.1 eV and a large atomic number of 53.2. The roles of IO and TmO groups for charge transport in the Tm(IO3)3 are revealed with the structural difference between the [101] and [1¯01]$[{\bar{1}}01]$ crystal orientations. Based on anisotropic responses of material properties and detection performances, it is found that the [1¯01${\bar{1}}01$] orientation, the path with fewer IO groups, achieves a high resistivity of 1.02 × 1011 Ω cm. Consequently, a single‐crystal detector exhibits a low dark current and small baseline drifting due to the wide bandgap, high resistivity and less ion migration of Tm(IO3)3, resulting in a low detection limit of 85.2 nGyair s−1. An excellent X‐ray imaging performance with a high sensitivity of 4406.6 µC Gyair−1 cm−2 is also shown in the Tm(IO3)3 device. These findings provide a new material design perspective for high‐performance X‐ray imaging applications. [ABSTRACT FROM AUTHOR]

In the past decade, metal halide perovskite (HP) has become a superstar semiconductor material due to its great application potential in the photovoltaic and photoelectric fields. In fact, HP initially attracted worldwide attention because of its excellent photovoltaic efficiency. However, HP and its derivatives also show great promise in X‐ray detection due to their strong X‐ray absorption, high bulk resistivity, suitable optical bandgap, and compatibility with integrated circuits. In this review, the basic working principles and modes of both the direct‐type and the indirect‐type X‐ray detectors are first summarized before discussing the applicability of HP for these two types of detection based on the pros and cons of different perovskites. Furthermore, the authors expand their view to different preparation methods developed for HP including single crystals and polycrystalline materials. Upon systematically analyzing their potential for X‐ray detection and photoelectronic characteristics on the basis of different structures and dimensions (0D, 2D, and 3D), recent progress of HPs (mainly polycrystalline) applied to flexible X‐ray detection are reviewed, and their practicability and feasibility are discussed. Finally, by reviewing the current research on HP‐based X‐ray detection, the challenges in this field are identified, and the main directions and prospects of future research are suggested. [ABSTRACT FROM AUTHOR]

Although perovskite wafers with a scalable size and thickness are suitable for direct X‐ray detection, polycrystalline perovskite wafers have drawbacks such as the high defect density, defective grain boundaries, and low crystallinity. Herein, PbI2‐DMSO powders are introduced into the MAPbI3 wafer to facilitate crystal growth. The PbI2 powders absorb a certain amount of DMSO to form the PbI2‐DMSO powders and PbI2‐DMSO is converted back into PbI2 under heating while releasing DMSO vapor. During isostatic pressing of the MAPbI3 wafer with the PbI2‐DMSO solid additive, the released DMSO vapor facilitates in situ growth in the MAPbI3 wafer with enhanced crystallinity and reduced defect density. A dense and compact MAPbI3 wafer with a high mobility‐lifetime (µτ) product of 8.70 × 10−4 cm2 V−1 is produced. The MAPbI3‐based direct X‐ray detector fabricated for demonstration shows a high sensitivity of 1.58 × 104 µC Gyair−1 cm−2 and a low detection limit of 410 nGyair s−1. [ABSTRACT FROM AUTHOR]

Abstract Semiconductor‐based X‐ray detectors with low detectable thresholds become critical in medical radiography applications. However, their performance is generally limited by intrinsic defects or unresolved issues of materials, and developing a novel scintillation semiconductor for low‐dose X‐ray detection is a highly urgent objective. Herein, a high‐quality rare‐earth iodate Tm(IO3)3 single crystal grown through low‐cost solution processing is reported with a wide bandgap of 4.1 eV and a large atomic number of 53.2. The roles of IO and TmO groups for charge transport in the Tm(IO3)3 are revealed with the structural difference between the [101] and [1¯01]$[{ar{1}}01]$ crystal orientations. Based on anisotropic responses of material properties and detection performances, it is found that the [1¯01${ar{1}}01$] orientation, the path with fewer IO groups, achieves a high resistivity of 1.02 × 1011 Ω cm. Consequently, a single‐crystal detector exhibits a low dark current and small baseline drifting due to the wide bandgap, high resistivity and less ion migration of Tm(IO3)3, resulting in a low detection limit of 85.2 nGyair s−1. An excellent X‐ray imaging performance with a high sensitivity of 4406.6 µC Gyair−1 cm−2 is also shown in the Tm(IO3)3 device. These findings provide a new material design perspective for high‐performance X‐ray imaging applications.

Metal halide perovskite scintillators encounter unprecedented opportunities in indirect ionizing radiation detection due to their high quantum yields. However, the long scintillation lifetime of microseconds upon irradiation, known as the afterglow phenomenon, obviously limits their fast development. Here, a new type of hybrid X‐ray detector wafer combining direct methylamine lead iodide (MAPbI3) semiconductor and indirect zero‐dimensional cesium copper iodide (Cs3Cu2I5) scintillator through low‐cost fast tableting processes is reported. Due to the fast energy transfer from Cs3Cu2I5 to MAPbI3, the device response time to X‐rays is dramatically reduced by nearly 30 times to 36.6 ns, which enables fast X‐ray detection capability by a large area detector arrays within 1 s. Moreover, Cs3Cu2I5 exists at the grain boundaries of MAPbI3 crystals, and blocks the paths of mobile ions of perovskite, leading to the lowest detectable dose rate of hybrid X‐ray detector is thus reduced by 1.5 times compared with control MAPbI3 direct‐type semiconductor, and 10 times compared with the Cs3Cu2I5 indirect‐type scintillator. The direct/indirect hybrid wafer also exhibits improved operation stability at ambient conditions without any encapsulation. This new kind of hybrid X‐ray detectors provides strong competitiveness by combining the advantages of both direct perovskite semiconductors and indirect perovskite scintillators for next‐generation products. [ABSTRACT FROM AUTHOR]

Perovskite materials in different dimensions show great potential in direct X‐ray detection, but each with limitations stemming from its own intrinsic properties. Particularly, the sensitivity of two‐dimensional (2D) perovskites is limited by poor carrier transport while ion migration in three‐dimensional (3D) perovskites causes the baseline drifting problem. To circumvent these limitations, herein a double‐layer perovskite film is developed with properly aligned energy level, where 2D (PEA)2MA3Pb4I13 (PEA=2‐phenylethylammonium, MA=methylammonium) is cascaded with vertically crystallized 3D MAPbI3. In this new design paradigm, the 3D layer ensures fast carrier transport while the 2D layer mitigates ion migration, thus offering a high sensitivity and a greatly stabilized baseline. Besides, the 2D layer increases the film resistivity and enlarges the energy barrier for hole injection without compromising carrier extraction. Consequently, the double‐layer perovskite detector delivers a high sensitivity (1.95 × 104μC Gyair−1 cm−2) and a low detection limit (480 nGyair s−1). Also demonstrated is the X‐ray imaging capacity using a circuit board as the object. This work opens up a new avenue for enhancing X‐ray detection performance via cascade assembly of various perovskites with complementary properties. [ABSTRACT FROM AUTHOR]