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Journal ArticleDOI

Inorganic Lead Halide Perovskite Single Crystals: Phase-Selective Low-Temperature Growth, Carrier Transport Properties, and Self-Powered Photodetection

About: This article is published in Advanced Optical Materials.The article was published on 2017-01-01. It has received 327 citations till now. The article focuses on the topics: Perovskite (structure) & Halide.
Citations
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Journal ArticleDOI
27 Aug 2018-Nature
TL;DR: All-inorganic perovskite nanocrystals containing caesium and lead provide low-cost, flexible and solution-processable scintillators that are highly sensitive to X-ray irradiation and emit radioluminescence that is colour-tunable across the visible spectrum.
Abstract: The rising demand for radiation detection materials in many applications has led to extensive research on scintillators1–3. The ability of a scintillator to absorb high-energy (kiloelectronvolt-scale) X-ray photons and convert the absorbed energy into low-energy visible photons is critical for applications in radiation exposure monitoring, security inspection, X-ray astronomy and medical radiography4,5. However, conventional scintillators are generally synthesized by crystallization at a high temperature and their radioluminescence is difficult to tune across the visible spectrum. Here we describe experimental investigations of a series of all-inorganic perovskite nanocrystals comprising caesium and lead atoms and their response to X-ray irradiation. These nanocrystal scintillators exhibit strong X-ray absorption and intense radioluminescence at visible wavelengths. Unlike bulk inorganic scintillators, these perovskite nanomaterials are solution-processable at a relatively low temperature and can generate X-ray-induced emissions that are easily tunable across the visible spectrum by tailoring the anionic component of colloidal precursors during their synthesis. These features allow the fabrication of flexible and highly sensitive X-ray detectors with a detection limit of 13 nanograys per second, which is about 400 times lower than typical medical imaging doses. We show that these colour-tunable perovskite nanocrystal scintillators can provide a convenient visualization tool for X-ray radiography, as the associated image can be directly recorded by standard digital cameras. We also demonstrate their direct integration with commercial flat-panel imagers and their utility in examining electronic circuit boards under low-dose X-ray illumination. All-inorganic perovskite nanocrystals containing caesium and lead provide low-cost, flexible and solution-processable scintillators that are highly sensitive to X-ray irradiation and emit radioluminescence that is colour-tunable across the visible spectrum.

1,064 citations

Journal ArticleDOI
TL;DR: The promising features and challenges of halide perovskites as promising radiation detectors are shown and it is suggested that they may compete with the conventional counterparts.
Abstract: Halide lead perovskites have attracted increasing attention in recent years for ionizing radiation detection due to their strong stopping power, defect-tolerance, large mobility-lifetime (μτ) product, tunable bandgap and simple single crystal growth from low-cost solution processes. In this review, we start with the requirement of material properties for high performance ionizing radiation detection based on direct detection mechanisms for applications in X-ray imaging and γ-ray energy spectroscopy. By comparing the performances of halide perovskites radiation detectors with current state-of-the-art ionizing radiation detectors, we show the promising features and challenges of halide perovskites as promising radiation detectors.

484 citations

Journal ArticleDOI
TL;DR: It is demonstrated that polythiophene, deposited on the top of CsPbI2 Br, can significantly reduce electron-hole recombination within the perovskite, which is due to the electronic passivation of surface defect states, and the interfacial properties are improved by a simple annealing process.
Abstract: Cesium-based trihalide perovskites have been demonstrated as promising light absorbers for photovoltaic applications due to their superb composition stability. However, the large energy losses (Eloss ) observed in inorganic perovskite solar cells has become a major hindrance impairing the ultimate efficiency. Here, an effective and reproducible method of modifying the interface between a CsPbI2 Br absorber and polythiophene hole-acceptor to minimize the Eloss is reported. It is demonstrated that polythiophene, deposited on the top of CsPbI2 Br, can significantly reduce electron-hole recombination within the perovskite, which is due to the electronic passivation of surface defect states. In addition, the interfacial properties are improved by a simple annealing process, leading to significantly reduced energy disorder in polythiophene and enhanced hole-injection into the hole-acceptor. Consequently, one of the highest power conversion efficiency (PCE) of 12.02% from a reverse scan in inorganic mixed-halide perovskite solar cells is obtained. Modifying the perovskite films with annealing polythiophene enables an open-circuit voltage (VOC ) of up to 1.32 V and Eloss of down to 0.5 eV, which both are the optimal values reported among cesium-lead mixed-halide perovskite solar cells to date. This method provides a new route to further improve the efficiency of perovskite solar cells by minimizing the Eloss .

388 citations

Journal ArticleDOI
TL;DR: An improved melt growth method for cesium lead bromide and a special detector design with asymmetrical metal electrode configuration that leads to a high performance at room temperature are reported.
Abstract: Gamma-ray detection and spectroscopy is the quantitative determination of their energy spectra, and is of critical value and critically important in diverse technological and scientific fields. Here we report an improved melt growth method for cesium lead bromide and a special detector design with asymmetrical metal electrode configuration that leads to a high performance at room temperature. As-grown centimeter-sized crystals possess extremely low impurity levels (below 10 p.p.m. for total 69 elements) and detectors achieve 3.9% energy resolution for 122 keV 57Co gamma-ray and 3.8% for 662 keV 137Cs gamma-ray. Cesium lead bromide is unique among all gamma-ray detection materials in that its hole transport properties are responsible for the high performance. The superior mobility-lifetime product for holes (1.34 × 10−3 cm2 V−1) derives mainly from the record long hole carrier lifetime (over 25 μs). The easily scalable crystal growth and high-energy resolution, highlight cesium lead bromide as an exceptional next generation material for room temperature radiation detection. Detection and spectroscopic measurements of gamma-ray used to rely on expensive materials such as CdZnTe crystals. Here He et al. develop a melt method to grow large size CsPbBr3 perovskite crystals and the devices achieve low cost, high energy resolving capabilities and stability.

344 citations

Journal ArticleDOI
TL;DR: Wang et al. realize smooth and pinhole-free, small-grained inorganic perovskite films with improved photoluminescence quantum yield by introducing trifluoroacetate anions to effectively passivate surface defects and control the crystal growth.
Abstract: Quantum efficiencies of organic-inorganic hybrid lead halide perovskite light-emitting devices (LEDs) have increased significantly, but poor device operational stability still impedes their further development and application. All-inorganic perovskites show better stability than the hybrid counterparts, but the performance of their respective films used in LEDs is limited by the large perovskite grain sizes, which lowers the radiative recombination probability and results in grain boundary related trap states. We realize smooth and pinhole-free, small-grained inorganic perovskite films with improved photoluminescence quantum yield by introducing trifluoroacetate anions to effectively passivate surface defects and control the crystal growth. As a result, efficient green LEDs based on inorganic perovskite films achieve a high current efficiency of 32.0 cd A−1 corresponding to an external quantum efficiency of 10.5%. More importantly, our all-inorganic perovskite LEDs demonstrate a record operational lifetime, with a half-lifetime of over 250 h at an initial luminance of 100 cd m−2. All-inorganic cesium lead bromide perovskite based light-emitting diodes show improved operational stability but the film quality limits their performance. Here Wang et al. use trifluoroacetate anions to passivate defects and achieve excellent device performance and stability.

315 citations

References
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Journal ArticleDOI
TL;DR: This paper could serve as a general literature citation when one or more of the open-source SH ELX programs (and the Bruker AXS version SHELXTL) are employed in the course of a crystal-structure determination.
Abstract: An account is given of the development of the SHELX system of computer programs from SHELX-76 to the present day. In addition to identifying useful innovations that have come into general use through their implementation in SHELX, a critical analysis is presented of the less-successful features, missed opportunities and desirable improvements for future releases of the software. An attempt is made to understand how a program originally designed for photographic intensity data, punched cards and computers over 10000 times slower than an average modern personal computer has managed to survive for so long. SHELXL is the most widely used program for small-molecule refinement and SHELXS and SHELXD are often employed for structure solution despite the availability of objectively superior programs. SHELXL also finds a niche for the refinement of macromolecules against high-resolution or twinned data; SHELXPRO acts as an interface for macromolecular applications. SHELXC, SHELXD and SHELXE are proving useful for the experimental phasing of macromolecules, especially because they are fast and robust and so are often employed in pipelines for high-throughput phasing. This paper could serve as a general literature citation when one or more of the open-source SHELX programs (and the Bruker AXS version SHELXTL) are employed in the course of a crystal-structure determination.

81,116 citations

Journal ArticleDOI
TL;DR: New features added to the refinement program SHELXL since 2008 are described and explained.
Abstract: The improvements in the crystal structure refinement program SHELXL have been closely coupled with the development and increasing importance of the CIF (Crystallographic Information Framework) format for validating and archiving crystal structures. An important simplification is that now only one file in CIF format (for convenience, referred to simply as `a CIF') containing embedded reflection data and SHELXL instructions is needed for a complete structure archive; the program SHREDCIF can be used to extract the .hkl and .ins files required for further refinement with SHELXL. Recent developments in SHELXL facilitate refinement against neutron diffraction data, the treatment of H atoms, the determination of absolute structure, the input of partial structure factors and the refinement of twinned and disordered structures. SHELXL is available free to academics for the Windows, Linux and Mac OS X operating systems, and is particularly suitable for multiple-core processors.

28,425 citations

Journal ArticleDOI
TL;DR: OLEX2 seamlessly links all aspects of the structure solution, refinement and publication process and presents them in a single workflow-driven package, with the ultimate goal of producing an application which will be useful to both chemists and crystallographers.
Abstract: New software, OLEX2, has been developed for the determination, visualization and analysis of molecular crystal structures. The software has a portable mouse-driven workflow-oriented and fully comprehensive graphical user interface for structure solution, refinement and report generation, as well as novel tools for structure analysis. OLEX2 seamlessly links all aspects of the structure solution, refinement and publication process and presents them in a single workflow-driven package, with the ultimate goal of producing an application which will be useful to both chemists and crystallographers.

19,990 citations

Journal ArticleDOI
TL;DR: Two organolead halide perovskite nanocrystals were found to efficiently sensitize TiO(2) for visible-light conversion in photoelectrochemical cells, which exhibit strong band-gap absorptions as semiconductors.
Abstract: Two organolead halide perovskite nanocrystals, CH3NH3PbBr3 and CH3NH3PbI3, were found to efficiently sensitize TiO2 for visible-light conversion in photoelectrochemical cells. When self-assembled on mesoporous TiO2 films, the nanocrystalline perovskites exhibit strong band-gap absorptions as semiconductors. The CH3NH3PbI3-based photocell with spectral sensitivity of up to 800 nm yielded a solar energy conversion efficiency of 3.8%. The CH3NH3PbBr3-based cell showed a high photovoltage of 0.96 V with an external quantum conversion efficiency of 65%.

16,634 citations

Journal ArticleDOI
TL;DR: The use of a solid hole conductor dramatically improved the device stability compared to (CH3NH3)PbI3 -sensitized liquid junction cells.
Abstract: We report on solid-state mesoscopic heterojunction solar cells employing nanoparticles (NPs) of methyl ammonium lead iodide (CH3NH3)PbI3 as light harvesters. The perovskite NPs were produced by reaction of methylammonium iodide with PbI2 and deposited onto a submicron-thick mesoscopic TiO2 film, whose pores were infiltrated with the hole-conductor spiro-MeOTAD. Illumination with standard AM-1.5 sunlight generated large photocurrents (JSC) exceeding 17 mA/cm2, an open circuit photovoltage (VOC) of 0.888 V and a fill factor (FF) of 0.62 yielding a power conversion efficiency (PCE) of 9.7%, the highest reported to date for such cells. Femto second laser studies combined with photo-induced absorption measurements showed charge separation to proceed via hole injection from the excited (CH3NH3)PbI3 NPs into the spiro-MeOTAD followed by electron transfer to the mesoscopic TiO2 film. The use of a solid hole conductor dramatically improved the device stability compared to (CH3NH3)PbI3 -sensitized liquid junction cells.

6,751 citations

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