Spacer Conformation Induced Multiple Hydrogen Bonds in 2D Perovskite toward Highly Efficient Optoelectronic Devices.

Two-dimensional (2D) Dion-Jacobson (DJ) perovskites typically outperform Ruddlesden-Popper (RP) analogs in terms of photodetection (PD). However, the mechanism behind this enhanced performance remains elusive. Theoretical calculations for elucidating interlayer spacer conformation-induced multiple hydrogen bonds in 2D perovskite are presented, along with the synthesis of DPAPbBr4 (DPB) single crystals (SCs) and their PD properties under X-ray/ultraviolet (UV) excitation. The high-quality DPB SC enhances PD with exceptional photoresponse attributes, including a high on/off ratio (4.89 × 104), high responsivity (2.44 A W⁻1), along with large dynamic linear range (154 dB) and low detection limit (7.1 nW cm⁻2), which are currently the best results among 2D perovskite SC detectors, respectively. Importantly, high-resolution images are obtained under UV illumination with weak light levels. The SC X-ray detector exhibits a high sensitivity of 663 µC Gyair⁻1 cm-2 at 10 V and a detection limit of 1.44 µGyair s⁻1. This study explores 2D DJ perovskites for efficient and innovative optoelectronic applications.

Spontaneous crystallization of strongly confined CsSnxPb1-xI3 perovskite colloidal quantum dots at room temperature.

The scalable and low-cost room temperature (RT) synthesis for pure-iodine all-inorganic perovskite colloidal quantum dots (QDs) is a challenge due to the phase transition induced by thermal unequilibrium. Here, we introduce a direct RT strongly confined spontaneous crystallization strategy in a Cs-deficient reaction system without polar solvents for synthesizing stable pure-iodine all-inorganic tin-lead (Sn-Pb) alloyed perovskite colloidal QDs, which exhibit bright yellow luminescence. By tuning the ratio of Cs/Pb precursors, the size confinement effect and optical band gap of the resultant CsSnxPb1-xI3 perovskite QDs can be well controlled. This strongly confined RT approach is universal for wider bandgap bromine- and chlorine-based all-inorganic and iodine-based hybrid perovskite QDs. The alloyed CsSn0.09Pb0.91I3 QDs show superior yellow emission properties with prolonged carrier lifetime and significantly increased colloidal stability compared to the pristine CsPbI3 QDs, which is enabled by strong size confinement, Sn2+ passivation and enhanced formation energy. These findings provide a RT size-stabilized synthesis pathway to achieve high-performance pure-iodine all-inorganic Sn-Pb mixed perovskite colloidal QDs for optoelectronic applications.

Micro/Nano Perovskite Materials for Advanced X-ray Detection and Imaging.

Halide perovskites have emerged as highly promising materials for ionizing radiation detection due to their exceptional characteristics, including a large mobility-lifetime product, strong stopping power, tunable band gap, and cost-effective crystal growth via solution processes. Semiconductor-type X-ray detectors employing various micro/nano perovskite materials have shown impressive progress in achieving heightened sensitivity and lower detection limits. Here, we present a comprehensive review of the applications of micro/nano perovskite materials for direct type X-ray detection, with a focus on the requirements for micro/nano crystal assembly and device properties in advanced X-ray detectors. We explore diverse processing techniques and optoelectronic considerations applied to perovskite X-ray detectors. Additionally, this review highlights the challenges and promising opportunities for perovskite X-ray detector arrays in real-world applications, potentially necessitating further research efforts.

Aspartate all-in-one doping strategy enables efficient all-perovskite tandems.

All-perovskite tandem solar cells hold great promise in surpassing the Shockley-Queisser limit for single-junction solar cells1-3. However, the practical use of these cells is currently hampered by the subpar performance and stability issues associated with mixed tin-lead (Sn-Pb) narrow-bandgap perovskite subcells in all-perovskite tandems4-7. In this study, we focus on the narrow-bandgap subcells and develop an all-in-one doping strategy for them. We introduce aspartate hydrochloride (AspCl) into both the bottom poly(3,4-ethylene dioxythiophene)-poly(styrene sulfonate) and bulk perovskite layers, followed by another AspCl posttreatment. We show that a single AspCl additive can effectively passivate defects, reduce Sn4+ impurities and shift the Fermi energy level. Additionally, the strong molecular bonding of AspCl-Sn/Pb iodide and AspCl-AspCl can strengthen the structure and thereby improve the stability of Sn-Pb perovskites. Ultimately, the implementation of AspCl doping in Sn-Pb perovskite solar cells yielded power conversion efficiencies of 22.46% for single-junction cells and 27.84% (27.62% stabilized and 27.34% certified) for tandems with 95% retention after being stored in an N2-filled glovebox for 2,000 h. These results suggest that all-in-one AspCl doping is a favourable strategy for enhancing the efficiency and stability of single-junction Sn-Pb perovskite solar cells and their tandems.

Perovskite-like Silver Halide Single-Crystal Microbelt Enables Ultrasensitive Flexible X-ray Detectors.

Lead halide perovskite single crystals have attracted wide interest in the field of X-ray detection due to their excellent photophysical properties. However, their inherent toxicity and high thickness restrict their applications in flexible devices. In this paper, designing a micronanometer-scale X-ray detector based on all-inorganic lead-free CsAg2I3 (CAI) single crystal microbelts (MBs) has addressed the above issues. These CAI single crystal MBs can be synthesized on various substrates with high crystal quality and excellent stability. Based on their excellent characteristics of the CAI MBs, we fabricate single CAI MB devices with an Au/CAI/Au structure, which shows not only good ultraviolet photoresponse characteristics, but also excellent X-ray detection performance. The optimized CAI photodetectors exhibit a responsivity of 23.59 mA/W, a high detectivity of 1010 Jones, and a fast response speed. For X-ray detection performance, a sensitivity of up to 515.49 µC Gyair-1 cm-2 and a detection limit of as low as 14.65 µGyair s-1 are achieved with outstanding operation stability and excellent long-term stability. Furthermore, our devices also showed excellent applicability for X-ray imaging, which is promising for their use in X-ray detection and imaging. Finally, flexible X-ray detectors are fabricated by using thin CAI single-crystal MBs and demonstrate good flexibility under different bending radii and bending cycles. Our work shows the potential for developing highly sensitive flexible integrated micro/nano optoelectronic devices by using lead-free perovskite analogue single crystals.

Synergistic passivation and stepped-dimensional perovskite analogs enable high-efficiency near-infrared light-emitting diodes.

Formamidinium lead iodide (FAPbI3) perovskites are promising emitters for near-infrared light-emitting diodes. However, their performance is still limited by defect-assisted nonradiative recombination and band offset-induced carrier aggregation at the interface. Herein, we introduce a couple of cadmium salts with acetate or halide anion into the FAPbI3 perovskite precursors to synergistically passivate the material defects and optimize the device band structure. Particularly, the perovskite analogs, containing zero-dimensional formamidinium cadmium iodide, one-dimensional δ-FAPbI3, two-dimensional FA2FAn-1PbnI3n+1, and three-dimensional α-FAPbI3, can be obtained in one pot and play a pivotal and positive role in energy transfer in the formamidinium iodide-rich lead-based perovskite films. As a result, the near-infrared FAPbI3-based devices deliver a maximum external quantum efficiency of 24.1% together with substantially improved operational stability. Combining our findings on defect passivation and energy transfer, we also achieve near-infrared light communication with device twins of light emitting and unprecedented self-driven detection.

Defect Passivation on Lead-Free CsSnI3 Perovskite Nanowires Enables High-Performance Photodetectors with Ultra-High Stability.

In recent years, Pb-free CsSnI3 perovskite materials with excellent photoelectric properties as well as low toxicity are attracting much attention in photoelectric devices. However, deep level defects in CsSnI3, such as high density of tin vacancies, structural deformation of SnI6- octahedra and oxidation of Sn2+ states, are the major challenge to achieve high-performance CsSnI3-based photoelectric devices with good stability. In this work, defect passivation method is adopted to solve the above issues, and the ultra-stable and high-performance CsSnI3 nanowires (NWs) photodetectors (PDs) are fabricated via incorporating 1-butyl-2,3-dimethylimidazolium chloride salt (BMIMCl) into perovskites. Through materials analysis and theoretical calculations, BMIM+ ions can effectively passivate the Sn-related defects and reduce the dark current of CsSnI3 NW PDs. To further reduce the dark current of the devices, the polymethyl methacrylate is introduced, and finally, the dual passivated CsSnI3 NWPDs show ultra-high performance with an ultra-low dark current of 2 × 10-11 A, a responsivity of up to 0.237 A W-1, a high detectivity of 1.18 × 1012 Jones and a linear dynamic range of 180 dB. Furthermore, the unpackaged devices exhibit ultra-high stability in device performance after 60 days of storage in air (25 °C, 50% humidity), with the device performance remaining above 90%.