Project description:Inorganic semiconductor ferroelectrics such as BiFeO3 have shown great potential in photovoltaic and other applications. Currently, semiconducting properties and the corresponding application in optoelectronic devices of hybrid organo-plumbate or stannate are a hot topic of academic research; more and more of such hybrids have been synthesized. Structurally, these hybrids are suitable for exploration of ferroelectricity. Therefore, the design of molecular ferroelectric semiconductors based on these hybrids provides a possibility to obtain new or high-performance semiconductor ferroelectrics. Here we investigated Pb-layered perovskites, and found the layer perovskite (benzylammonium)2PbCl4 is ferroelectric with semiconducting behaviours. It has a larger ferroelectric spontaneous polarization Ps=13 μC cm(-2) and a higher Curie temperature Tc=438 K with a band gap of 3.65 eV. This finding throws light on the new properties of the hybrid organo-plumbate or stannate compounds and provides a new way to develop new semiconductor ferroelectrics.
Project description:Lead halide perovskite nanocrystals of the formula CsPbBr3 have recently been identified as potential time taggers in scintillating heterostructures for time-of-flight positron emission tomography (TOF-PET) imaging thanks to their ultrafast decay kinetics. This study investigates the potential of this material experimentally. We fabricated CsPbBr3 thin films on scintillating GGAG:Ce (Gd2.985Ce0.015Ga2.7Al2.3O12) wafer as a model structure for the future sampling detector geometry. We focused this study on the radioluminescence (RL) response of this composite material. We compare the results of two spin-coating methods, namely the static and the dynamic process, for the thin film preparation. We demonstrated enhanced RL intensity of both CsPbBr3 and GGAG:Ce scintillating constituents of a composite material. This synergic effect arises in both the RL spectra and decays, including decays in the short time window (50 ns). Consequently, this study confirms the applicability of CsPbBr3 nanocrystals as efficient time taggers for ultrafast timing applications, such as TOF-PET.
Project description:Organic-inorganic hybrid perovskites (OIHPs) have been intensively studied due to their fascinating optoelectronic performance. Electron microscopy and related characterization techniques are powerful to figure out their structure-property relationships at the nanoscale. However, electron beam irradiation usually causes damage to these beam-sensitive materials and thus deteriorates the associated devices. Taking a widely used CH3NH3PbI3 film as an example, here, we carry out a comprehensive study on how electron beam irradiation affects its properties. Interestingly, our results reveal that photoluminescence (PL) intensity of the film can be significantly improved along with blue-shift of emission peak at a specific electron beam dose interval. This improvement stems from the reduction of trap density at the CH3NH3PbI3 surface. The knock-on effect helps expose a fresh surface assisted by the surface defect-induced lowering of displacement threshold energy. Meanwhile, the radiolysis process consistently degrades the crystal structure and weaken the PL emission with the increase of electron beam dose. Consequently, the final PL emission comes from a balance between knock-on and radiolysis effects. Taking advantage of the defect regulation, we successfully demonstrate a patterned CH3NH3PbI3 film with controllable PL emission and a photodetector with enhanced photocurrent. This work will trigger the application of electron beam irradiation as a powerful tool for perovskite materials processing in micro-LEDs and other optoelectronic applications.
Project description:In this article, we used a two-step chemical vapor deposition (CVD) method to synthesize methylammonium lead-tin triiodide perovskite films, MAPb1-xSnxI3, with x varying from 0 to 1. We successfully controlled the concentration of Sn in the perovskite films and used Rutherford backscattering spectroscopy (RBS) to quantify the composition of the precursor films for conversion into perovskite films. According to the RBS results, increasing the SnCl2 source amount in the reaction chamber translate into an increase in Sn concentration in the films. The crystal structure and the optical properties of perovskite films were examined by X-ray diffraction (XRD) and UV-Vis spectrometry. All the perovskite films depicted similar XRD patterns corresponding to a tetragonal structure with I4cm space group despite the precursor films having different crystal structures. The increasing concentration of Sn in the perovskite films linearly decreased the unit volume from about 988.4 Å3 for MAPbI3 to about 983.3 Å3 for MAPb0.39Sn0.61I3, which consequently influenced the optical properties of the films manifested by the decrease in energy bandgap (Eg) and an increase in the disorder in the band gap. The SEM micrographs depicted improvements in the grain size (0.3-1 µm) and surface coverage of the perovskite films compared with the precursor films.
Project description:Recently, several studies have investigated dielectric properties as a possible origin of the exceptional optoelectronic properties of metal halide perovskites (MHPs). In this study we investigated the temperature-dependent dielectric behavior of different MHP films at different frequencies. In the gigahertz regime, dielectric losses in methylammonium-based samples are dominated by the rotational dynamics of the organic cation. Upon increasing the temperature from 160 to 300 K, the rotational relaxation time, τ, decreases from 400 (200) to 6 (1) ps for MAPb-I3 (-Br3). By contrast, we found negligible temperature-dependent variations in τ for a mixed cation/mixed halide FA0.85MA0.15Pb(I0.85Br0.15)3. From temperature-dependent time-resolved microwave conductance measurements we conclude that the dipolar reorientation of the MA cation does not affect charge carrier mobility and lifetime in MHPs. Therefore, charge carriers do not feel the relatively slow-moving MA cations, despite their great impact on the dielectric constants.
Project description:We show that pristine thin films made of tin halide perovskite have external photoluminescence quantum yield comparable to that of lead halide perovskite, i.e., the material in use to prepare state-of-the-art perovskite solar cells.
Project description:Miniaturized photonic sources based on semiconducting two-dimensional (2D) materials offer new technological opportunities beyond the modern III-V platforms. For example, the quantum-confined 2D electronic structure aligns the exciton transition dipole moment parallel to the surface plane, thereby outcoupling more light to air which gives rise to high-efficiency quantum optics and electroluminescent devices. It requires scalable materials and processes to create the decoupled multi-quantum-well superlattices, in which individual 2D material layers are isolated by atomically thin quantum barriers. Here, we report decoupled multi-quantum-well superlattices comprised of the colloidal quantum wells of lead halide perovskites, with unprecedentedly ultrathin quantum barriers that screen interlayer interactions within the range of 6.5 Å. Crystallographic and 2D k-space spectroscopic analysis reveals that the transition dipole moment orientation of bright excitons in the superlattices is predominantly in-plane and independent of stacking layer and quantum barrier thickness, confirming interlayer decoupling.
Project description:We apply the contactless quasi-steady-state photoconductance (QSSPC) method to co-evaporated methyl ammonium lead iodide (MAPbI3) perovskite thin-films. Using an adapted calibration for ultralow photoconductances, we extract the injection-dependent carrier lifetime of the MAPbI3 layer. The lifetime is found to be limited by radiative recombination at the high injection densities applied during the QSSPC measurement, enabling the extraction of the electron and hole mobility sum in the MAPbI3 using the known coefficient of radiative recombination of MAPbI3. Combining the QSSPC measurement with transient photoluminescence measurements, performed at much lower injection densities, we obtain the injection-dependent lifetime curve over several orders of magnitude. From the resulting lifetime curve, we determine the achievable open-circuit voltage of the examined MAPbI3 layer.
Project description:Lead halide perovskite microlasers have been very promising for versatile optoelectronic applications. However, most perovskite microlasers are linearly polarized with uniform wavefront. The structured laser beams carrying orbital angular momentum have rarely been studied and the applications of perovskites in next-generation optical communications are thus hindered. Herein, we experimentally demonstrate the perovskite vortex microlasers with highly directional outputs and well-controlled topological charges. High quality gratings have been experimentally fabricated in perovskite film and the subsequent vertical cavity surface emitting lasers (VCSELs) with divergent angles of 3o are achieved. With the control of Archimedean spiral gratings, the wavefront of the perovskite VCSELs has been switched to be helical with topological charges of q = -4 to 4. This research is able to expand the potential applications of perovskite microlasers in hybrid integrated photonic networks, as well as optical computing.
Project description:In this letter, methylammonium lead iodide (MAPbI3) thin films were examined via piezoresponse force microscopy (PFM) and nanoindentation (NI) to determine if long-range atomic order existed across the full width and depth of the apparent grains. From the PFM, the piezoelectric response of the films was strongly correlated with low-index planes of the crystal structure and ferroelastic domains in macroscale solution-grown MAPbI3 crystals, which implied long-range order near the top surface. From the NI, it was found that the induced cracks were straight and extended across the full width of the apparent grains, which indicated that the long-range order was not limited to the near-surface region, but extended through the film thickness. Interestingly, the two MAPbI3 processes examined resulted in subtle differences in the extracted electro-mechanical and fracture properties, but exhibited similar power conversion efficiencies of >17% in completed devices.