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Abstract Over the past decade, lead halide perovskites have gained significant interest for ionizing radiation detection, owing to their exceptional performance, and cost-effective fabrication in a wide range of form factors, from thick films to large single crystals. However, the toxicity of lead, limited environmental and thermal stability of these materials, as well as dark current drift due to ionic conductivity, have prompted the development of alternative materials that can address these challenges. Bismuth-based compounds (including perovskite derivatives and nonperovskite materials) have similarly high atomic numbers, leading to strong X-ray attenuation, but have lower toxicity, tend to be more environmentally stable, and can have lower ionic conductivity, especially in low-dimensional materials. These materials are also advantageous over commercial direct X-ray detectors by being able to detect lower dose rates of X-rays than amorphous selenium by at least two orders of magnitude, are potentially more cost-effective to mass produce than cadmium zinc telluride, and can operate at room temperature (unlike high-purity Ge). Given the strong interest in this area, we here discuss recent advances in the development of bismuth-based perovskite derivatives (with 3D, 2D and 0D structural dimensionality), and other bismuth-based perovskite-inspired materials for direct X-ray detection. We discuss the critical properties of these materials that underpin the strong performances achieved, particularly the ability to detect low-dose rates of X-rays. We cover key strategies for enhancing the performance of these materials, as well as the challenges that need to be overcome to commercialize these emerging technologies. Graphical abstractmore » « less
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The prototypical chalcogenide perovskite, BaZrS3 (BZS), with its direct bandgap of 1.7–1.8 eV, high chemical stability, and strong light–matter interactions, has garnered significant interest over the past few years. So far, attempts to grow BaZrS3 films have been limited mainly to physical vapor deposition techniques. Here, we report the fabrication of BZS thin films via a facile aqueous solution route of polymer-assisted deposition (PAD), where the polymer-chelated cation precursor films were sulfurized in a mixed CS2 and Ar atmosphere. The formation of a single-phase polycrystalline BZS thin film at a processing temperature of 900 °C was confirmed by X-ray diffraction and Raman spectroscopy. The stoichiometry of the films was verified by Rutherford Backscattering spectrometry and energy-dispersive X-ray spectroscopy. The BZS films showed a photoluminescence peak at around 1.8 eV and exhibited a photogenerated current under light illumination at a wavelength of 530 nm. Temperature-dependent resistivity analysis revealed that the conduction of BaZrS3 films under the dark condition could be described by the Efros–Shklovskii variable range hopping model in the temperature range of 60–300 K, with an activation energy of about 44 meV.more » « less
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Perovskite offers a framework that boasts various functionalities and physical properties of interest such as ferroelectricity, magnetic orderings, multiferroicity, superconductivity, semiconductor, and optoelectronic properties owing to their rich compositional diversity. These properties are also uniquely tied to their crystal distortion which is directly affected by lattice strain. Therefore, many important properties of perovskite can be further tuned through strain engineering which can be accomplished by chemical doping or simply element substitution, interface engineering in epitaxial thin films, and special architectures such as nanocomposites. In this review, we focus on and highlight the structure–property relationships of perovskite metal oxide films and elucidate the principles to manipulate the functionalities through different modalities of strain engineering approaches.more » « less
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Abstract Quasi‐2D perovskite made with organic spacers co‐crystallized with inorganic cesium lead bromide inorganics is demonstrated for near unity photoluminescence quantum yield at room temperature. However, light emitting diodes made with quasi‐2D perovskites rapidly degrade which remains a major bottleneck in this field. In this work, It is shown that the bright emission originates from finely tuned multi‐component 2D nano‐crystalline phases that are thermodynamically unstable. The bright emission is extremely sensitive to external stimuli and the emission quickly dims away upon heating. After a detailed analysis of their optical and morphological properties, the degradation is attributed to 2D phase redistribution associated with the dissociation of the organic spacers departing from the inorganic lattice. To circumvent the instability problem, a diamine is investigated spacer that has both sides attached to the inorganic lattice. The diamine spacer incorporated perovskite film shows significantly improved thermal tolerance over maintaining a high photoluminescence quantum yield of over 50%, which will be a more robust material for lighting applications. This study guides designing quasi‐2D perovskites to stabilize the emission properties.more » « less
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Abstract Perovskite optoelectronics are regarded as a disruptive technology, but their susceptibility to environmental degradation and reliance on toxic solvents in traditional processing methods pose significant challenges to their practical implementation. Herein, methylammonium lead iodide (MAPbI3) perovskite films processed via a solvent‐free laser printing technique, that exhibit exceptional stability, are reported. These films withstand extreme conditions, including high doses of X‐ray radiation exceeding 200 Gy, blue laser illumination, 90% relative humidity, and thermal stress up to 80 °C for over 300 min in air. We demonstrate that laser‐printed films maintain their structural integrity and optoelectronic properties even after prolonged exposure to these stressors, significantly surpassing the stability of conventionally processed films. The enhanced stability is attributed to the unique film formation mechanism and resulting defect‐tolerant microstructure. These results underscore the potential of laser printing as a scalable, safe, and sustainable manufacturing route for producing stable perovskite‐based devices with potential applications in diverse fields, ranging from renewable energy to large‐area electronics and space exploration.more » « less
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