Ultrasound‐Assisted Crystallization Enables Large‐Area Perovskite Quasi‐Monocrystalline Film for High‐Sensitive X‐ray Detection and Imaging

Abstract

In recent years, halide perovskites have shown great application potential in X‐ray detection due to their superior optoelectronic properties and high X‐ray attenuation coefficient. However, large‐area perovskite fabrication for high performance X‐ray detectors remains extremely challenging. Herein, ultrasound‐assisted crystallization combined with the hot‐pressing method is proposed to prepare large‐area (10 cm × 10 cm) and high‐quality quasi‐monocrystalline thick film of a mixed‐cation perovskite MA0.42FA0.58PbI3. The rapid ultrasound‐assisted crystallization provides more homogeneous nucleation, which is essential to the fabrication of large‐area and uniform perovskite microcrystalline film. Furthermore, the post hot‐pressing treatment is implemented to fuse the crystal boundaries, rearrange the crystal grains, and eliminate the voids between crystals, resulting in a quasi‐monocrystalline film. After the hot‐pressing treatment, the carrier mobility and the carrier mobility‐lifetime product increased about 13‐fold (from 1.8 to 23.5 cm2 s−1 V−1) and 18 times (from 8.4 × 10−6 to 1.5 × 10−4 cm2 V−1), respectively. As a result, a high‐performance MA0.42FA0.58PbI3 quasi‐monocrystalline X‐ray detector is achieved with an impressively high sensitivity (1.16 × 106 µC Gyair−1 cm−2) and low detection limit (37.4 nGyair s−1), demonstrating the potential of the ultrasound‐assisted crystallization and hot‐pressing strategy from an industrial perspective.

Perovskite materials in X-ray detection and imaging: recent progress, challenges, and future prospects

“…In addition to SCs, polycrystalline perovskitebased X-ray detectors, including lms and wafers, have also established their enhanced performance in comparison with the widely used detectors such as a-Se and CdTe. 147,158 . This improvement is attributed to advancements in synthesis methodologies and optimization of materials and device architectures.…”

“…The common technique is an isostatic-pressing method 182 Size and cost Forming large-size single crystals of perovskite poses challenges including controlling the crystal growth rate, time-consuming preparation, and incapability for realizing exible devices 81,204 Fabricating large-scale lms is comparatively straightforward, involving shorter preparation times and yielding sizable, wearable devices 205 Developing large-sized wafers is also a challenging task Quality Achieving single crystals with minimal cracks has been successful 64 Film quality surpasses that of wafers, but fewer single crystals are observed 64 The perovskite layer quality is relatively poor Only a few studies offered insights into the spatial resolution of the images. The highest stated spatial resolution was 3.3 line pairs per millimeter 147 Several studies furnished information regarding the spatial resolution of the images. The highest reported spatial resolution was of 6 line pairs per millimeter 153…”

Attaining inhibition of sneak current and versatile logic operations in a singular halide perovskite memristive device by introducing appropriate interface barriers

“…Additionally, metal halide perovskites have been extensively researched and applied in various fields, including photocatalysis, luminescence, scintillation, X-ray imaging, photovoltaics, and more, demonstrating their versatility as a material. 21–25…”

Enhanced photoelectric performance in Cu–Bi double halide perovskite single crystals

“…In the last decade, hybrid lead halide perovskite single crystals with low trap density, high charge carrier mobility, and long carrier life time have attracted broad research interest in various optoelectronic applications, such as in solar cells, 1–3 detectors, 4–10 light-emitting diodes 11 and photoelectrochemical cells. 12,13 Despite the impressive performance and cost-effectiveness of three-dimensional (3D) perovskites, 14–16 their practical application is severely restricted by the two challenges posed by the lead toxicity and instability. 17–21 Altering the chemical composition and crystallography to construct lead-free perovskites with desirable band structures and optical properties provides an alternative solution.…”