Browse
Submit Data
Databases
API
Help

Dataset Information

26 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

High-Resolution In-Situ Synchrotron X-Ray Studies of Inorganic Perovskite CsPbBr₃ : New Symmetry Assignments and Structural Phase Transitions.

ABSTRACT: Perovskite photovoltaic ABX₃ systems are being studied due to their high energy-conversion efficiencies with current emphasis placed on pure inorganic systems. In this work, synchrotron single-crystal diffraction measurements combined with second harmonic generation measurements reveal the absence of inversion symmetry below room temperature in CsPbBr₃ . Local structural analysis by pair distribution function and X-ray absorption fine structure methods are performed to ascertain the local ordering, atomic pair correlations, and phase evolution in a broad range of temperatures. The currently accepted space group assignments for CsPbBr₃ are found to be incorrect in a manner that profoundly impacts physical properties. New assignments are obtained for the bulk structure: Im3¯ (above ≈410 K), P2₁ /m (between ≈300 K and ≈410 K), and the polar group Pm (below ≈300 K), respectively. The newly observed structural distortions exist in the bulk structure consistent with the expectation of previous photoluminescence and Raman measurements. High-pressure measurements reveal multiple low-pressure phases, one of which exists as a metastable phase at ambient pressure. This work should help guide research in the perovskite photovoltaic community to better control the structure under operational conditions and further improve transport and optical properties.

SUBMITTER: Liu S

PROVIDER: S-EPMC8456275 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Sr-Doping All-Inorganic CsPbBr3 Perovskite Thick Film for Self-Powered X-ray Detectors.

Project description:The all-inorganic perovskite cesium lead bromine (CsPbBr3) has attracted much attention in the field of X-ray detectors because of its high X-ray absorption coefficient, high carrier collection efficiency, and easy solution preparation. The low-cost anti-solvent method is the main method to prepare CsPbBr3; during this process, solvent volatilization will bring a large number of holes to the film, leading to the increase of defects. Based on the heteroatomic doping strategy, we propose that Pb2+ should be partially replaced by Sr2+ to prepare leadless all-inorganic perovskite. The introduction of Sr2+ promoted the ordered growth of CsPbBr3 in the vertical direction, increased the density and uniformity of the thick film, and achieved the goal of CsPbBr3 thick film repairing. In addition, the prepared CsPbBr3 and CsPbBr3:Sr X-ray detectors were self-powered without external bias, maintaining a stable response during on and off states at different X-ray dose rates. Furthermore, the detector base on 160 µm CsPbBr3:Sr had a sensitivity of 517.02 µC Gyair-1 cm-3 at zero bias under the dose rate of 0.955 µGy ms-1 and it obtained a fast response speed of 0.053-0.148 s. Our work provides a new opportunity to produce cost-effective and highly efficient self-powered perovskite X-ray detectors in a sustainable way.

| S-EPMC10003980 | biostudies-literature

Photon Recycling in CsPbBr3 All-Inorganic Perovskite Nanocrystals.

Project description:Photon recycling, the iterative process of re-absorption and re-emission of photons in an absorbing medium, can play an important role in the power-conversion efficiency of photovoltaic cells. To date, several studies have proposed that this process may occur in bulk or thin films of inorganic lead-halide perovskites, but conclusive proof of the occurrence and magnitude of this effect is missing. Here, we provide clear evidence and quantitative estimation of photon recycling in CsPbBr3 nanocrystal suspensions by combining measurements of steady-state and time-resolved photoluminescence (PL) and PL quantum yield with simulations of photon diffusion through the suspension. The steady-state PL shows clear spectral modifications including red shifts and quantum yield decrease, while the time-resolved measurements show prolonged PL decay and rise times. These effects grow as the nanocrystal concentration and distance traveled through the suspension increase. Monte Carlo simulations of photons diffusing through the medium and exhibiting absorption and re-emission account quantitatively for the observed trends and show that up to five re-emission cycles are involved. We thus identify 4 quantifiable measures, PL red shift, PL QY, PL decay time, and PL rise time that together all point toward repeated, energy-directed radiative transfer between nanocrystals. These results highlight the importance of photon recycling for both optical properties and photovoltaic applications of inorganic perovskite nanocrystals.

| S-EPMC8603385 | biostudies-literature

Ultra-stable CsPbBr3 Perovskite Nanosheets for X-Ray Imaging Screen.

Project description:Wet chemistry methods, including hot-injection and precipitation methods, have emerged as major synthetic routes for high-quality perovskite nanocrystals in backlit display and scintillation applications. However, low chemical yield hinders their upscale production for practical use. Meanwhile, the labile nature of halide-based perovskite poses a major challenge for long-term storage of perovskite nanocrystals. Herein, we report a green synthesis at room temperature for gram-scale production of CsPbBr3 nanosheets with minimum use of solvent, saving over 95% of the solvent for the unity mass nanocrystal production. The perovskite colloid exhibits record stability upon long-term storage for up to 8 months, preserving a photoluminescence quantum yield of 63% in solid state. Importantly, the colloidal nanosheets show self-assembly behavior upon slow solidification, generating a crack-free thin film in a large area. The uniform film was then demonstrated as an efficient scintillation screen for X-ray imaging. Our findings bring a scalable tool for synthesis of high-quality perovskite nanocrystals, which may inspire the industrial optoelectronic application of large-area perovskite film.

| S-EPMC7770729 | biostudies-literature

In Situ Imaging of Ferroelastic Domain Dynamics in CsPbBr3 Perovskite Nanowires by Nanofocused Scanning X-ray Diffraction.

Project description:The interest in metal halide perovskites has grown as impressive results have been shown in solar cells, light emitting devices, and scintillators, but this class of materials have a complex crystal structure that is only partially understood. In particular, the dynamics of the nanoscale ferroelastic domains in metal halide perovskites remains difficult to study. An ideal in situ imaging method for ferroelastic domains requires a challenging combination of high spatial resolution and long penetration depth. Here, we demonstrate in situ temperature-dependent imaging of ferroelastic domains in a single nanowire of metal halide perovskite, CsPbBr3. Scanning X-ray diffraction with a 60 nm beam was used to retrieve local structural properties for temperatures up to 140 °C. We observed a single Bragg peak at room temperature, but at 80 °C, four new Bragg peaks appeared, originating in different real-space domains. The domains were arranged in periodic stripes in the center and with a hatched pattern close to the edges. Reciprocal space mapping at 80 °C was used to quantify the local strain and lattice tilts, revealing the ferroelastic nature of the domains. The domains display a partial stability to further temperature changes. Our results show the dynamics of nanoscale ferroelastic domain formation within a single-crystal perovskite nanostructure, which is important both for the fundamental understanding of these materials and for the development of perovskite-based devices.

| S-EPMC7690043 | biostudies-literature

Rapid Crystallization of All-Inorganic CsPbBr3 Perovskite for High-Brightness Light-Emitting Diodes.

Project description:Research into perovskite-based light-emitting diodes (PeLEDs) has been rapidly gaining momentum since the initial reports of green-emitting methylammonium lead bromide (CH3NH3PbBr3)-based devices were published. However, issues pertaining to its stability and morphological control still hamper progress toward high performing devices. Solvent engineering, a technique typically employed to modulate film crystallization, offers little opportunity for scale-up due to the tendency for inhomogeneous film growth and low degree of reproducibility. Here, we propose and show a simple gas-facilitated process to deposit a stable, all-inorganic perovskite CsPbBr3 film. The formation of smaller and less percolated grains, which gives rise to enhanced optical properties, highlights the importance of spatial charge confinement in the film. Consequently, the performance of our PeLEDs shows great improvement, with luminance as high as 8218 cd m-2 and turn-on voltage as low as 2.4 V. Concomitantly, the current efficiency and EQE of our device were increased to 0.72 cd A-1 and 0.088%, respectively. High reproducibility in the performance of PeLEDs fabricated using this process opens the path for large-area devices.

| S-EPMC6640975 | biostudies-literature

Efficient Carbon-Based CsPbBr3 Inorganic Perovskite Solar Cells by Using Cu-Phthalocyanine as Hole Transport Material.

Project description:Metal halide perovskite solar cells (PSCs) have attracted extensive research interest for next-generation solution-processed photovoltaic devices because of their high solar-to-electric power conversion efficiency (PCE) and low fabrication cost. Although the world's best PSC successfully achieves a considerable PCE of over 20% within a very limited timeframe after intensive efforts, the stability, high cost, and up-scaling of PSCs still remain issues. Recently, inorganic perovskite material, CsPbBr3, is emerging as a promising photo-sensitizer with excellent durability and thermal stability, but the efficiency is still embarrassing. In this work, we intend to address these issues by exploiting CsPbBr3 as light absorber, accompanied by using Cu-phthalocyanine (CuPc) as hole transport material (HTM) and carbon as counter electrode. The optimal device acquires a decent PCE of 6.21%, over 60% higher than those of the HTM-free devices. The systematic characterization and analysis reveal a more effective charge transfer process and a suppressed charge recombination in PSCs after introducing CuPc as hole transfer layer. More importantly, our devices exhibit an outstanding durability and a promising thermal stability, making it rather meaningful in future fabrication and application of PSCs.

| S-EPMC6199080 | biostudies-literature

Thin Layer Buckling in Perovskite CsPbBr3 Nanobelts.

Project description:Flexible semiconductor materials, where structural fluctuations and transformation are tolerable and have low impact on electronic properties, focus interest for future applications. Two-dimensional thin layer lead halide perovskites are hailed for their unconventional optoelectronic features. We report structural deformations via thin layer buckling in colloidal CsPbBr3 nanobelts adsorbed on carbon substrates. The microstructure of buckled nanobelts is determined using transmission electron microscopy and atomic force microscopy. We measured significant decrease in emission from the buckled nanobelt using cathodoluminescence, marking the influence of such mechanical deformations on electronic properties. By employing plate buckling theory, we approximate adhesion forces between the buckled nanobelt and the substrate to be Fadhesion ∼ 0.12 μN, marking a limit to sustain such deformation. This work highlights detrimental effects of mechanical buckling on electronic properties in halide perovskite nanostructures and points toward the capillary action that should be minimized in fabrication of future devices and heterostructures based on nanoperovskites.

| S-EPMC8397391 | biostudies-literature

How lasing happens in CsPbBr3 perovskite nanowires.

Project description:Lead halide perovskites are emerging as an excellent material platform for optoelectronic processes. There have been extensive discussions on lasing, polariton formation, and nonlinear processes in this material system, but the underlying mechanism remains unknown. Here we probe lasing from CsPbBr3 perovskite nanowires with picosecond (ps) time resolution and show that lasing originates from stimulated emission of an electron-hole plasma. We observe an anomalous blue-shifting of the lasing gain profile with time up to 25 ps, and assign this as a signature for lasing involving plasmon emission. The time domain view provides an ultra-sensitive probe of many-body physics which was obscured in previous time-integrated measurements of lasing from lead halide perovskite nanowires.

| S-EPMC6335413 | biostudies-literature

Electrochemical p-Doping of CsPbBr3 Perovskite Nanocrystals.

Project description:Lead halide perovskite nanocrystals have drawn attention as active light-absorbing or -emitting materials for opto-electronic applications due to their facile synthesis, intrinsic defect tolerance, and color-pure emission ranging over the entire visible spectrum. To optimize their application in, e.g., solar cells and light-emitting diodes, it is desirable to gain control over electronic doping of these materials. However, predominantly due to the intrinsic instability of perovskites, successful electronic doping has remained elusive. Using spectro-electrochemistry and electrochemical transistor measurements, we demonstrate here that CsPbBr3 nanocrystals can be successfully and reversibly p-doped via electrochemical hole injection. From an applied potential of ∼0.9 V vs NHE, the emission quenches, the band edge absorbance bleaches, and the electronic conductivity quickly increases, demonstrating the successful injection of holes into the valence band of the CsPbBr3 nanocrystals.

| S-EPMC8294022 | biostudies-literature

CsPbBr3-CdS heterostructure: stabilizing perovskite nanocrystals for photocatalysis.

Project description:The instability of cesium lead bromide (CsPbBr3) nanocrystals (NCs) in polar solvents has hampered their use in photocatalysis. We have now succeeded in synthesizing CsPbBr3-CdS heterostructures with improved stability and photocatalytic performance. While the CdS deposition provides solvent stability, the parent CsPbBr3 in the heterostructure harvests photons to generate charge carriers. This heterostructure exhibits longer emission lifetime (τ ave = 47 ns) than pristine CsPbBr3 (τ ave = 7 ns), indicating passivation of surface defects. We employed ethyl viologen (EV2+) as a probe molecule to elucidate excited state interactions and interfacial electron transfer of CsPbBr3-CdS NCs in toluene/ethanol mixed solvent. The electron transfer rate constant as obtained from transient absorption spectroscopy was 9.5 × 1010 s-1 and the quantum efficiency of ethyl viologen reduction (Φ EV+˙) was found to be 8.4% under visible light excitation. The Fermi level equilibration between CsPbBr3-CdS and EV2+/EV+˙ redox couple has allowed us to estimate the apparent conduction band energy of the heterostructure as -0.365 V vs. NHE. The insights into effective utilization of perovskite nanocrystals built around a quasi-type II heterostructures pave the way towards effective utilization in photocatalytic reduction and oxidation processes.

| S-EPMC8597851 | biostudies-literature