In recent years, methylammonium lead halide (MAPbX3, where X = Cl, Br, and I) perovskites have attracted tremendous interest caused by their outstanding photovoltaic performance. Mixed halides have been frequently used as the active layer of solar cells, as a result of their superior physical properties as compared to those of traditionally used pure iodide. Herein, we report a remarkable finding of reversible halide-exchange reactions of MAPbX3, which facilitates the synthesis of a series of mixed halide perovskites. We synthesized MAPbBr3 plate-type nanocrystals (NCs) as a starting material by a novel solution reaction using octylamine as the capping ligand. The synthesis of MAPbBr(3-x)Clx and MAPbBr(3-x)Ix NCs was achieved by the halide exchange reaction of MAPbBr3 with MACl and MAI, respectively, in an isopropyl alcohol solution, demonstrating full-range band gap tuning over a wide range (1.6-3 eV). Moreover, photodetectors were fabricated using these composition-tuned NCs; a strong correlation was observed between the photocurrent and photoluminescence decay time. Among the two mixed halide perovskite series, those with I-rich composition (x = 2), where a sole tetragonal phase exists without the incorporation of a cubic phase, exhibited the highest photoconversion efficiency. To understand the composition-dependent photoconversion efficiency, first-principles density-functional theory calculations were carried out, which predicted many plausible configurations for cubic and tetragonal phase mixed halides.
Light-matter interactions in inorganic perovskite nanolasers are investigated using single-crystalline cesium lead halide (CsPbX3, X = Cl, Br, and I) nanowires synthesized by the chemical vapor transport method. The perovskite nanowires exhibit a uniform growth direction, smooth surfaces, straight end facets, and homogeneous composition distributions. Lasing occurs in the perovskite nanowires at low thresholds (3 μJ/cm(2)) with high quality factors (Q = 1200-1400) under ambient atmospheric environments. The wavelengths of the nanowire lasers are tunable by controlling the stoichiometry of the halide, allowing the lasing of the inorganic perovskite nanowires from blue to red. The unusual spacing of the Fabry-Pérot modes suggests strong light-matter interactions in the reduced mode volume of the nanowires, while the polarization of the lasing indicates that the Fabry-Pérot modes belong to the same fundamental transverse mode. The dispersion curve of the exciton-polariton model suggests that the group refractive index of the polariton is significantly enhanced.
To investigate the effect of seed layer on the growth of ZnO nanorods during hydrothermal synthesis, different types of sputter-deposited ZnO films were used. The changes in growth rate, diameter, density, and surface area of highly oriented ZnO nanorods on each seed layer were examined. The growth rate of ZnO nanorods has a strong relationship with the intensity of (0001) orientation. The density of nanorods per unit area is larger if the diameter of the nanorods is smaller. The total surface area of ZnO nanorods is determined by the growth rate and density per unit area. It was found that the morphology of the ZnO nanorods is strongly influenced by the thickness of the seed layer and the corresponding crystal size. A thinner ZnO seed layer provides a higher surface area of ZnO nanorods because of the smaller crystal size of the seed layer. The orientation of the ZnO seed layer significantly affects the crystallinity of the nanorods.
This Letter describes size-controlled photocatalytic activity of ZnO nanoparticles coated with glutathione-protected gold nanoparticles with diameters of 1.1, 1.6, and 2.8 nm. The photocatalytic activity of the ZnO–Au composites was found to increase with increasing gold size for both oxidative and reductive catalytic reactions. Photoluminescence decay dynamics of the composites showed that the electron-transfer rate from the photoexcited ZnO to gold nanoparticle also increased as the gold size increased. These results demonstrate that the photogenerated electron transfer and the resulting catalytic activity of the composites can be controlled by the size of the mediating gold capacitors.
Femtosecond fluorescence anisotropy measurements for a variety of cyclic porphyrin arrays such as Zn(II)porphyrin m-trimer and hexamer are reported along with o-dimer and monomer as reference molecules. In the porphyrin arrays, a pair of porphyrin moieties are joined together via triphenyl linkage to ensure cyclic and rigid structures. Anisotropy decay times of the porphyrin arrays can be well described by the Förster incoherent excitation hopping process between the porphyrin units. Exciton coupling strengths of 74 and 264 cm(-1) for the m-trimer and hexamer estimated from the observed excitation energy hopping rates are close to those of B800 and B850, respectively, in the LH2 bacterial light-harvesting antenna. Thus, these cyclic porphyrin array systems have proven to be useful in understanding energy migration processes in a relatively weak interaction regime in light of the similarity in overall structures and constituent chromophores to natural light-harvesting arrays.
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