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      Structural and Chemical Changes to CH 3 NH 3 PbI 3 Induced by Electron and Gallium Ion Beams

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          Organometal halide perovskites as visible-light sensitizers for photovoltaic cells.

          Two organolead halide perovskite nanocrystals, CH(3)NH(3)PbBr(3) and CH(3)NH(3)PbI(3), were found to efficiently sensitize TiO(2) for visible-light conversion in photoelectrochemical cells. When self-assembled on mesoporous TiO(2) films, the nanocrystalline perovskites exhibit strong band-gap absorptions as semiconductors. The CH(3)NH(3)PbI(3)-based photocell with spectral sensitivity of up to 800 nm yielded a solar energy conversion efficiency of 3.8%. The CH(3)NH(3)PbBr(3)-based cell showed a high photovoltage of 0.96 V with an external quantum conversion efficiency of 65%.
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            Iodide management in formamidinium-lead-halide–based perovskite layers for efficient solar cells

            The formation of a dense and uniform thin layer on the substrates is crucial for the fabrication of high-performance perovskite solar cells (PSCs) containing formamidinium with multiple cations and mixed halide anions. The concentration of defect states, which reduce a cell's performance by decreasing the open-circuit voltage and short-circuit current density, needs to be as low as possible. We show that the introduction of additional iodide ions into the organic cation solution, which are used to form the perovskite layers through an intramolecular exchanging process, decreases the concentration of deep-level defects. The defect-engineered thin perovskite layers enable the fabrication of PSCs with a certified power conversion efficiency of 22.1% in small cells and 19.7% in 1-square-centimeter cells.
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              Semiconducting tin and lead iodide perovskites with organic cations: phase transitions, high mobilities, and near-infrared photoluminescent properties.

              A broad organic-inorganic series of hybrid metal iodide perovskites with the general formulation AMI3, where A is the methylammonium (CH3NH3(+)) or formamidinium (HC(NH2)2(+)) cation and M is Sn (1 and 2) or Pb (3 and 4) are reported. The compounds have been prepared through a variety of synthetic approaches, and the nature of the resulting materials is discussed in terms of their thermal stability and optical and electronic properties. We find that the chemical and physical properties of these materials strongly depend on the preparation method. Single crystal X-ray diffraction analysis of 1-4 classifies the compounds in the perovskite structural family. Structural phase transitions were observed and investigated by temperature-dependent single crystal X-ray diffraction in the 100-400 K range. The charge transport properties of the materials are discussed in conjunction with diffuse reflectance studies in the mid-IR region that display characteristic absorption features. Temperature-dependent studies show a strong dependence of the resistivity as a function of the crystal structure. Optical absorption measurements indicate that 1-4 behave as direct-gap semiconductors with energy band gaps distributed in the range of 1.25-1.75 eV. The compounds exhibit an intense near-IR photoluminescence (PL) emission in the 700-1000 nm range (1.1-1.7 eV) at room temperature. We show that solid solutions between the Sn and Pb compounds are readily accessible throughout the composition range. The optical properties such as energy band gap, emission intensity, and wavelength can be readily controlled as we show for the isostructural series of solid solutions CH3NH3Sn(1-x)Pb(x)I3 (5). The charge transport type in these materials was characterized by Seebeck coefficient and Hall-effect measurements. The compounds behave as p- or n-type semiconductors depending on the preparation method. The samples with the lowest carrier concentration are prepared from solution and are n-type; p-type samples can be obtained through solid state reactions exposed in air in a controllable manner. In the case of Sn compounds, there is a facile tendency toward oxidation which causes the materials to be doped with Sn(4+) and thus behave as p-type semiconductors displaying metal-like conductivity. The compounds appear to possess very high estimated electron and hole mobilities that exceed 2000 cm(2)/(V s) and 300 cm(2)/(V s), respectively, as shown in the case of CH3NH3SnI3 (1). We also compare the properties of the title hybrid materials with those of the "all-inorganic" CsSnI3 and CsPbI3 prepared using identical synthetic methods.
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                Author and article information

                Contributors
                (View ORCID Profile)
                (View ORCID Profile)
                Journal
                Advanced Materials
                Adv. Mater.
                Wiley
                0935-9648
                1521-4095
                June 15 2018
                June 2018
                April 26 2018
                June 2018
                : 30
                : 25
                : 1800629
                Affiliations
                [1 ]Department of Materials Science and EngineeringMonash University Victoria 3800 Australia
                [2 ]ARC Centre of Excellence in Exciton ScienceMonash University Victoria 3800 Australia
                [3 ]Department of Chemical EngineeringMonash University Victoria 3800 Australia
                [4 ]Department of Applied PhysicsThe Hong Kong Polytechnic University Hung Hom Kowloon Hong Kong
                [5 ]Monash Centre for Electron MicroscopyMonash University Victoria 3800 Australia
                [6 ]School of Physics and AstronomyMonash University Victoria 3800 Australia
                [7 ]State Key Laboratory of Advanced Technology for Materials Synthesis and ProcessingWuhan University of Technology Wuhan 430070 China
                [8 ]Commonwealth Scientific and Industrial Research OrganizationManufacturing Flagship Clayton Victoria 3168 Australia
                [9 ]Melbourne Centre for Nano fabrication 151 Wellington Road Clayton VIC 3168 Australia
                [10 ]State Key Laboratory of Silicate Materials for ArchitecturesWuhan University of Technology Wuhan 430070 China
                Article
                10.1002/adma.201800629
                e958a0da-fcfe-4a4f-b04a-e367e4f7c380
                © 2018

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                http://doi.wiley.com/10.1002/tdm_license_1.1

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