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2D organic-inorganic hybrid perovskites (OIHPs) have shown great promise in direct X-ray detection. The development of high-performance passive X-ray detectors in 2D OIHPs calls for an increase in material density while maintaining structural polarity, which is becoming quite challenging. Here, a high-density, polar 2D alternating-cation-intercalated (ACI) perovskite, (4-AP)Cs 2 Pb 2 I 8 ( B , 4-AP = 4-amidinopyridinium), capable of addressing this problem is successfully constructed by introducing heavy Cs + into the interlayer space of an aromatic Dion-Jacobson (DJ) perovskite (4-AP)PbI 4 ( A ). Through such a DJ-to-ACI design, the newly developed 2D OIHP B not only significantly increases its density to 4.23 g cm -3 (even higher than that of 3D MAPbI 3 ) but also crystallizes in a polar space group ( Ama 2), which further leads to enhanced X-ray attenuation and an obvious polar photovoltage (1.1 V) under X-ray irradiation. As a result, X-ray detectors fabricated by high-quality single crystals of B exhibit excellent and stable detection performance under self-powered mode with a high sensitivity of 107 μC Gy -1 cm -2 and a low detection limit of 289 nGy s -1 . This work provides implications for the future exploration and regulation of novel ACI OIHPs for high-performance photoelectronic devices.

Metal halide perovskites have outperformed conventional inorganic semiconductors in direct X-ray detection due to their ease of synthesis and intriguing photoelectric properties. However, the operational instability caused by severe ion migration under a high external electric field is still a big concern for the practical application of perovskite detectors. Here, we report a 2D (BPEA) 2 PbI 4 (BPEA = R -1-(4-bromophenyl)ethylammonium) perovskite with Br-substituted aromatic spacer capable of introducing abundant interactions, e.g., the molecular electrostatic forces between Br atoms and aromatic rings and halogen bonds of Br-I, in the interlayer space, which effectively suppresses ion migration and thus enables superior operational stability. Constructing direct X-ray detectors based on high-quality single crystals of (BPEA) 2 PbI 4 results in a high sensitivity of 1,003 μC Gy -1 cm -2 , a low detection limit of 366 nGy s -1 , and an ultralow baseline drift of 3.48 × 10 -8 nA cm -1 s -1 V -1 at 80 V bias. More strikingly, it also exhibits exceptional operational stability under high flux, long-time X-ray irradiation, and large working voltage. This work shows an integration of multiple interlayer interactions to stabilize perovskite X-ray detectors, providing new insights into the future design of perovskite optoelectronic devices toward practical application., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

As a next-generation high-power lighting technology, laser lighting has attracted great attention in high-luminance applications. However, thermally robust and highly efficient color converters suitable for high-quality laser lighting are scarce. Despite its versatility, the phosphor-in-glass (PiG) has been seldom applied in laser lighting because of its low thermal conductivity. In this work, we develop a unique architecture in which a phosphor-in-glass (PiG) film was directly sintered on a high thermally conductive sapphire substrate coated by one-dimensional photonic crystals. The designed color converter with the composite architecture exhibits a high internal quantum efficiency close to that of the original phosphor powders and an excellent packaging efficiency up to 90%. Furthermore, the PiG film can even be survived under the 11.2 W mm -2 blue laser excitation. Combining blue laser diodes with the YAG-PiG-on-sapphire plate, a uniform white light with a high luminance of 845 Mcd m -2 (luminous flux: 1839 lm), luminous efficacy of 210 lm W -1 , and correlated color temperature of 6504 K was obtained. A high color rendering index of 74 was attained by adding a robust orange or red phosphor layer to the architecture. These outstanding properties meet the standards of vehicle regulations, enabling the PiG films with the composite architecture to be applied in automotive lighting or other high-power and high-luminance laser lighting.