High-Performance Hard X-Ray Imaging Detector Using Facet-Dependent Bismuth Vanadate.

Bismuth vanadate (BiVO4) exhibits large absorption efficiency for hard X-rays, which endows it with a robust capacity to attenuate X-ray radiation across a broad energy range. The anisotropic properties of BiVO4 allow for the manipulation of their physical and chemical characteristics through crystallographic orientation and exposed facets. In this study, the issue of heavy recombination caused by sluggish electron transport in BiVO4 is successfully addressed by enhancing the abundance of the (040) crystal face ratio using a Co2+ crystal face exposure agent. The facet-dependent modifications exhibit excellent and balanced intrinsic charge transport properties, and finely optimize both the sensitivity and detection limit of BiVO4 X-ray detectors. As a result, ultra-stable BiVO4 metal oxide X-ray detectors demonstrate a high sensitivity of 3164 µC Gyair -1 cm-2 and a low detection limit of 20.76 nGyair s-1 under 110 kVp hard X-rays, establishing a new benchmark for X-ray detectors based on polycrystalline Bi-halides and metal oxides. These findings highlight the significance of crystal orientation in optimizing materials for X-ray detection, setting a new sensitivity record for X-ray detectors based on polycrystalline Bi-halides and metal oxides, which paves the way for the development of advanced, low-dose, and highly stable imaging systems specifically for hard X-rays.

High-Performance Flat-Panel Perovskite X-ray Detectors Enabled by Defect Passivation in Ruddlesden-Popper Perovskites.

Halide perovskites have emerged as promising candidates in X-ray detection due to their strong X-ray absorption and excellent optoelectronic properties. The development of sensitive and stable flat-panel X-ray detectors with high resolution is crucial for practical applications. In this paper, we introduce a novel flat-panel X-ray detector that integrates quasi-two-dimensional (2D) Ruddlesden-Popper (RP) perovskite with a pixeled thin film transistor (TFT) backplane. We incorporate 2,5-dibromopyrimidine (DBPM) as an additive to passivate the Lewis acid defects in the quasi-2D RP perovskite. This modification results in suppressed ion migration, improved optoelectronic performance, and enhanced operational stability of the device. Impressively, the activation energy of the RP perovskite increases from 0.96 to 1.35 eV with the DBPM additive. As a result, X-ray detectors exhibit a high sensitivity of ∼13,600 µC Gyair-1 cm-2, a low detection limit of 6.56 nGyair s-1, and excellent operational stability. Moreover, the flat-panel detectors demonstrate a high spatial resolution of 3.7 line pairs per millimeter and excellent X-ray imaging properties under a remarkably low X-ray dose of ∼50 µGyair, which is just half of the X-ray dose typically used in commercial equipment. This study opens new avenues for the development of flat-panel perovskite X-ray detectors with significant potential for various applications.

Halide perovskites for sensitive, stable and scalable X-ray detection and imaging.

Halide perovskites have attracted significant research interests in the X-ray detection and imaging field. Their strong X-ray attenuating ability and good carrier transportation endow them with high sensitivity, which is better than those of commercialized amorphous selenium (a-Se) and CdZnTe (CZT). However, ion migration has been identified as a critical factor that deteriorates the performance of three-dimensional (3D) lead-based halide perovskite detectors. Moreover, large dark current has hindered their application in low-dose X-ray detection. Another major challenge is to fabricate large area, high-quality thick perovskites that can be integrated with commercial electronic readout backplanes, such as thin-film transistors (TFTs) and complementary metal-oxide-semiconductor (CMOS) transistors, to produce multipixel flat-panel detectors for X-ray imaging. Bismuth-based halide perovskites have been demonstrated to be competitive candidates due to their low ionic migration and small dark current. Fabrication methods, including pressing, membrane filling, blade coating, spray coating etc., will be summarized and discussed in detail. This feature article discusses the potential and challenges in perovskite X-ray detection and imaging, providing new research directions for future development.

Additive-Induced Synergies of Ion Migration Inhibition and Defect Passivation toward Sensitive Perovskite X-ray Detectors.

Two-dimensional (2D) Ruddlesden-Popper (RP) metal halide perovskites have emerged as a promising material for X-ray detection. However, defects and ion migration generated nonradiative recombination and high dark current could cause severe performance degradation, which hinders their application. Herein, rubrene was added to the precursor solution of BA2MA3Pb4I13 to modulate the performance of the 2D RP perovskite X-ray detectors. The cation-π interaction between rubrene and perovskite could passivate the defects and inhibit the ion migration, resulting in improved performance and stability. The detectors made with rubrene exhibited a sensitivity of 354.30 µC·Gyair-1 cm-2 and a detection limit of 112.85 nGyair s-1. This work highlights the synergistic effect of rubrene in defect passivation and ion migration inhibition, providing a facile approach toward sensitive perovskite X-ray detectors.

A-Site Cation Engineering of Ruddlesden-Popper Perovskites for Stable, Sensitive, and Portable Direct Conversion X-ray Imaging Detectors.

Perovskite flat-panel X-ray detectors are promising products for realizing low-dose medical imaging, a nondestructive test, and security inspection. However, the perovskite X-ray imager still faces intractable problems such as severe baseline drift, a low signal-to-noise ratio, and rapid performance degradation, which were involved by the notorious intrinsic ion migration of the perovskite functional layer. In this work, sensitive, stable, and portable pixel quasi-two-dimensional (2D) Ruddlesden-Popper (RP) perovskite X-ray imagers were obtained by an advanced solvent-free laminated fabrication approach. A-Site cation engineering of RP perovskites provides a hint for solving the trade-off between stability and detection performance, resulting in a stable pixel X-ray imager that shows a sensitivity of ∼7000 µC Gyair-1 cm-2, a detection limit of 7.8 nGyair s-1, and good 2D multipixel X-ray imaging. This work demonstrates both a high-performance, stable X-ray imager and its robust fabrication, paving the way for adopting a RP perovskite imager as novel flat-panel X-ray detectors.

High-Efficiency Perovskite Solar Cells Enabled by Anatase TiO2 Nanopyramid Arrays with an Oriented Electric Field.

One-dimensional (1D) nanostructured oxides are proposed as excellent electron transport materials (ETMs) for perovskite solar cells (PSCs); however, experimental evidence is lacking. A facile hydrothermal approach was employed to grow highly oriented anatase TiO2 nanopyramid arrays and demonstrate their application in PSCs. The oriented TiO2 nanopyramid arrays afford sufficient contact area for electron extraction and increase light transmission. Moreover, the nanopyramid array/perovskite system exhibits an oriented electric field that can increase charge separation and accelerate charge transport, thereby suppressing charge recombination. The anatase TiO2 nanopyramid array-based PSCs deliver a champion power conversion efficiency of approximately 22.5 %, which is the highest power conversion efficiency reported to date for PSCs consisting of 1D ETMs. This work demonstrates that the rational design of 1D ETMs can achieve PSCs that perform as well as typical mesoscopic and planar PSCs.

Defect mitigation using d-penicillamine for efficient methylammonium-free perovskite solar cells with high operational stability.

Trap-dominated non-radiative charge recombination is one of the key factors that limit the performance of perovskite solar cells (PSCs), which was widely studied in methylammonium (MA) containing PSCs. However, there is a need to elucidate the defect chemistry of thermally stable, MA-free, cesium/formamidinium (Cs/FA)-based perovskites. Herein, we show that d-penicillamine (PA), an edible antidote for treating heavy metal ions, not only effectively passivates the iodine vacancies (Pb2+ defects) through coordination with the -SH and -COOH groups in PA, but also finely tunes the crystallinity of Cs/FA-based perovskite film. Benefiting from these merits, a reduction of non-radiative recombination and an increase in photoluminescence lifetime have been achieved. As a result, the champion MA-free device exhibits an impressive power conversion efficiency (PCE) of 22.4%, an open-circuit voltage of 1.163 V, a notable fill factor of 82%, and excellent long-term operational stability. Moreover, the defect passivation strategy can be further extended to a mini module (substrate: 4 × 4 cm2, active area: 7.2 cm2) as well as a wide-bandgap (∼1.73 eV) Cs/FA perovskite system by delivering PCEs of 16.3% and 20.2%, respectively, demonstrating its universality in defect passivation for efficient PSCs.

Defect Passivation in Hybrid Perovskite Solar Cells by Tailoring the Electron Density Distribution in Passivation Molecules.

Commercialization of perovskite solar cells (PSCs) requires developing high-efficiency devices with good stability. Ionic defects existing in the perovskite layer can serve as nonradiative recombination centers to deteriorate the performance of PSCs and can introduce chemical degradation of the perovskite material introducing instability issues. Here, passivation molecules with various electron density distributions (EDD) are employed as an ideal model to reveal the role of EDD on defect passivation in perovskite thin films. Power conversion efficiency (PCE) exceeding 21% with good stability in humid air was obtained for planar PSCs with the 4-aminobenzonitrile (ABN) additive, higher than the reference PSCs with a PCE of 20.22%. The improved stability and performance features are attributed to the efficient passivation for charged defects in perovskites by adding ABN, which guarantees a smaller Urbach energy, longer carrier lifetime, and less traps in the perovskite films.

Crystalline Copper Phosphide Nanosheets as an Efficient Janus Catalyst for Overall Water Splitting.

Hydrogen is essential to many industrial processes and could play an important role as an ideal clean energy carrier for future energy supply. Herein, we report for the first time the growth of crystalline Cu3P phosphide nanosheets on conductive nickel foam (Cu3P@NF) for electrocatalytic and visible light-driven overall water splitting. Our results show that the Cu3P@NF electrode can be used as an efficient Janus catalyst for both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER). For OER catalysis, a current density of 10 mA/cm2 requires an overpotential of only ∼320 mV and the slope of the Tafel plot is as low as 54 mV/dec in 1.0 M KOH. For HER catalysis, the overpotential is only ∼105 mV to achieve a catalytic current density of 10 mA cm-2. Moreover, overall water splitting can be achieved in a water electrolyzer based on the Cu3P@NF electrode, which showed a catalytic current density of 10 mA/cm2 under an applied voltage of ∼1.67 V. The same current density can also be obtained using a silicon solar cell under ∼1.70 V for both the HER and the OER. This new Janus Cu3P@NF electrode is made of inexpensive and nonprecious metal-based materials, which opens new possibilities based on copper to exploit overall water splitting for hydrogen production. To the best of our knowledge, such high performance of a copper-based water oxidation and overall water splitting catalyst has not been reported to date.