Project description:Pockels and Kerr effects are linear and nonlinear electro-optical effects, respectively, used in many applications. The modulation of the refractive index is employed in different photonic circuits. However, the greatest challenge is in photonic elements for quantum computing at room temperature. For this aim, materials with strong Pockels/Kerr effects and χ(2)/χ(3) nonlinear susceptibilities are necessary. Here, we demonstrate composition-modulated strong electro-optical response in epitaxial films of (Ba,Ca)(Ti,Zr)O3 perovskite titanate. These films are grown by pulsed laser deposition on SrTiO3. Depending on the ratios of Ca/Ba and Ti/Zr, films show high Pockels or Kerr optical nonlinearities. We relate the variable electro-optic response to the occurrence of nanopolar domains with different symmetries in a selected composition range. These findings open the route to easily implement nonlinear optical elements in integrated photonic circuits.
Project description:Lead-free double perovskites have been considered as a potential environmentally friendly photovoltaic material for substituting the hybrid lead halide perovskites due to their high stability and nontoxicity. Here, lead-free double perovskite Cs2AgBiBr6 films are initially fabricated by single-source evaporation deposition under high vacuum condition. X-ray diffraction and scanning electron microscopy characterization show that the high crystallinity, flat, and pinhole-free double perovskite Cs2AgBiBr6 films were obtained after post-annealing at 300 °C for 15 min. By changing the annealing temperature, annealing time, and film thickness, perovskite Cs2AgBiBr6 solar cells with planar heterojunction structure of FTO/TiO2/Cs2AgBiBr6/Spiro-OMeTAD/Ag achieve an encouraging power conversion efficiency of 0.70%. Our preliminary work opens a feasible approach for preparing high-quality double perovskite Cs2AgBiBr6 films wielding considerable potential for photovoltaic application.
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:Charge transport in three-dimensional metal-halide perovskite semiconductors is due to a complex combination of ionic and electronic contributions, and its study is particularly relevant in light of their successful applications in photovoltaics as well as other opto- and microelectronic applications. Interestingly, the observation of field effect at room temperature in transistors based on solution-processed, polycrystalline, three-dimensional perovskite thin films has been elusive. In this work, we study the time-dependent electrical characteristics of field-effect transistors based on the model methylammonium lead iodide semiconductor and observe the drastic variations in output current, and therefore of apparent charge carrier mobility, as a function of the applied gate pulse duration. We infer this behavior to the accumulation of ions at the grain boundaries, which hamper the transport of carriers across the FET channel. This study reveals the dynamic nature of the field effect in solution-processed metal-halide perovskites and offers an investigation methodology useful to characterize charge carrier transport in such emerging semiconductors.
Project description:In recent years, hybrid organic-inorganic halide perovskites have been widely studied for the low-cost fabrication of a wide range of optoelectronic devices, including impressive perovskite-based solar cells. Amongst the key factors influencing the performance of these devices, recent efforts have focused on tailoring the granularity and microstructure of the perovskite films. Albeit, a cost-effective technique allowing to carefully control their microstructure in ambient environmental conditions has not been realized. We report on a solvent-antisolvent ambient processed CH3NH3PbI3-xClx based thin films using a simple and robust solvent engineering technique to achieve large grains (>5 µm) having excellent crystalline quality and surface coverage with very low pinhole density. Using optimized treatment (75% chlorobenzene and 25% ethanol), we achieve highly-compact perovskite films with 99.97% surface coverage to produce solar cells with power conversion efficiencies (PCEs) up-to 14.0%. In these planar solar cells, we find that the density and size of the pinholes are the dominant factors that affect their overall performances. This work provides a promising solvent treatment technique in ambient conditions and paves the way for further optimization of large area thin films and high performance perovskite solar cells.
Project description:Photodetectors based on three dimensional organic-inorganic lead halide perovskites have recently received significant attention. As a new type of light-harvesting materials, formamidinium lead iodide (FAPbI3) is known to possess excellent optoelectronic properties even exceeding those of methylammonium lead iodide (MAPbI3). To date, only a few photoconductor-type photodetectors based on FAPbI3 single crystals and polycrystalline thin films in a lateral structure have been reported. Here, we demonstrate low-voltage, high-overall-performance photodiode-type photodetectors in a sandwiched geometry based on polycrystalline α-FAPbI3 thin films synthesized by a one-step solution processing method and post-annealing treatment. The photodetectors exhibit a broadband response from the near-ultraviolet to the near-infrared (330-800 nm), achieving a high on/off current ratio of 8.6 × 104 and fast response times of 7.2/19.5 μs. The devices yield a photoresponsivity of 0.95 AW-1 and a high specific detectivity of 2.8 × 1012 Jones with an external quantum efficiency (EQE) approaching 182% at -1.0 V under 650 nm illumination. The photodiode-type photodetectors based on polycrystalline α-FAPbI3 thin films with superior performance consequently show great promise for future optoelectronic device applications.
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:Perovskite thin films are at the forefront of highly promising photovoltaic technologies due to their remarkable optoelectronic properties. Herein, we explore a low-cost, reproducible, and industry-scalable methodology to synthesize an all-inorganic CsPbI1.5Br1.5 perovskite thin film with additional incorporation of copper and chloride ions into the lattice structure. The synthesis process involves chemical bath deposition of PbS, followed by a gas-solid iodination reaction to yield PbI2. Subsequently, dip-coating incorporates Cs+, Cu2+, Br-, and Cl- ions into PbI2, and annealing at 270 °C produces perovskite thin films. The results show a large coverage area and a uniform thickness of each perovskite thin film. Comprehensive characterization, including X-ray diffraction, Raman spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy, and photoluminescence, provides the structural, chemical, and optical properties of the synthesized thin films. To evaluate the practical implications of our methodology, we fabricated photodetectors employing CsPbI1.5Br1.5 and (Cs0.95:Cu0.01)PbI1.5Br1.3Cl0.1 perovskite films. A comparative analysis unequivocally demonstrates a significant increase in photodetector performance when utilizing (Cs0.95:Cu0.01)PbI1.5Br1.3Cl0.1 perovskite films. While our findings quantitatively assess the tangible enhancement in photocurrent, we acknowledge the potential for improvement in device fabrication to enhance the overall performance. This study not only affirms the successful low-cost synthesis of perovskite thin films but also emphasizes the pivotal role of Cu2+ and Cl- ions in enhancing the performance of perovskite-based optoelectronic devices.
Project description:Reversible optical property changes in lead-free perovskites have recently received great interest due to their potential applications in smart windows, sensors, data encryption, and various on-demand devices. However, it is challenging to achieve remarkable color changes in their thin films. Here, methylamine gas (CH3 NH2 , MA0 ) induced switchable optical bleaching of bismuth (Bi)-based perovskite films is demonstrated for the first time. By exposure to an MA0 atmosphere, the color of Cs2 AgBiBr6 (CABB) films changes from yellow to transparent, and the color of Cs3 Bi2 I9 (CBI) films changes from dark red to transparent. More interestingly, the underlying reason is found to be the interactions between MA0 and Bi3+ with the formation of an amorphous liquefied transparent intermediate phase, which is different from that of lead-based perovskite systems. Moreover, the generality of this approach is demonstrated with other amine gases, including ethylamine (C2 H5 NH2 , EA0 ) and butylamine (CH3 (CH2 )3 NH2 , BA0 ), and another compound, Cs3 Sb2 I9 , by observing a similar reversible optical bleaching phenomenon. The potential for the application of CABB and CBI films in switchable smart windows is investigated. This study provides valuable insights into the interactions between amine gases and lead-free perovskites, opening up new possibilities for high-efficiency optoelectronic and stimuli-responsive applications of these emerging Bi-based materials.
Project description:Metal halide perovskite solar cells (PSCs) have raised considerable scientific interest due to their high cost-efficiency potential for photovoltaic solar energy conversion. As PSCs already are meeting the efficiency requirements for renewable power generation, more attention is given to further technological barriers as environmental stability and reliability. However, the most major obstacle limiting commercialization of PSCs is the lack of a reliable and scalable process for thin film production. Here, a generic crystallization strategy that allows the controlled growth of highly qualitative perovskite films via a one-step blade coating is reported. Through rational ink formulation in combination with a facile vacuum-assisted precrystallization strategy, it is possible to produce dense and uniform perovskite films with high crystallinity on large areas. The universal application of the method is demonstrated at the hand of three typical perovskite compositions with different band gaps. P-i-n perovskite solar cells show fill factors up to 80%, underpinning the statement of the importance of controlling crystallization dynamics. The methodology provides important progress toward the realization of cost-effective large-area perovskite solar cells for practical applications.