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      Environmentally Stable Room Temperature Continuous Wave Lasing in Defect-passivated Perovskite

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          Abstract

          Metal halide perovskites have emerged as promising gain materials for on-chip lasers in photonic integrated circuits (PICs). However, stable continuous wave (CW) lasing behavior under optical pumping at room temperature - a prerequisite for electrically pumped lasing - has not yet been demonstrated. To achieve stable CW operation, we introduce a multiplex of strategies that include morphological, structural and interfacial engineering of CH3NH3PbBr3 (MAPbBr3) thin films to improve perovskite's intrinsic stability, as well as high quality cavity design to reduce the operational power. We demonstrate for the first time, over 90-minute-long green CW lasing with 9.4W/cm2 threshold from a polycarbonate (PC)-defect-passivated, directly patterned MAPbBr3 two-dimensional photonic crystal (PhC) cavity without any substrate cooling. We also show our approach's effectiveness on the performance of MAPbBr3 under electrical excitation: we observe a seven-fold current efficiency enhancement by applying our strategies to a MAPbBr3 LED. This work paves the way to the realization of electrically pumped lasing in perovskites.

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          Most cited references 31

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          Long-range balanced electron- and hole-transport lengths in organic-inorganic CH3NH3PbI3.

          Low-temperature solution-processed photovoltaics suffer from low efficiencies because of poor exciton or electron-hole diffusion lengths (typically about 10 nanometers). Recent reports of highly efficient CH3NH3PbI3-based solar cells in a broad range of configurations raise a compelling case for understanding the fundamental photophysical mechanisms in these materials. By applying femtosecond transient optical spectroscopy to bilayers that interface this perovskite with either selective-electron or selective-hole extraction materials, we have uncovered concrete evidence of balanced long-range electron-hole diffusion lengths of at least 100 nanometers in solution-processed CH3NH3PbI3. The high photoconversion efficiencies of these systems stem from the comparable optical absorption length and charge-carrier diffusion lengths, transcending the traditional constraints of solution-processed semiconductors.
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            Solar cells. Impact of microstructure on local carrier lifetime in perovskite solar cells.

            The remarkable performance of hybrid perovskite photovoltaics is attributed to their long carrier lifetimes and high photoluminescence (PL) efficiencies. High-quality films are associated with slower PL decays, and it has been claimed that grain boundaries have a negligible impact on performance. We used confocal fluorescence microscopy correlated with scanning electron microscopy to spatially resolve the PL decay dynamics from films of nonstoichiometric organic-inorganic perovskites, CH3NH3PbI3(Cl). The PL intensities and lifetimes varied between different grains in the same film, even for films that exhibited long bulk lifetimes. The grain boundaries were dimmer and exhibited faster nonradiative decay. Energy-dispersive x-ray spectroscopy showed a positive correlation between chlorine concentration and regions of brighter PL, whereas PL imaging revealed that chemical treatment with pyridine could activate previously dark grains. Copyright © 2015, American Association for the Advancement of Science.
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              High Photoluminescence Efficiency and Optically Pumped Lasing in Solution-Processed Mixed Halide Perovskite Semiconductors.

              The study of the photophysical properties of organic-metallic lead halide perovskites, which demonstrate excellent photovoltaic performance in devices with electron- and hole-accepting layers, helps to understand their charge photogeneration and recombination mechanism and unravels their potential for other optoelectronic applications. We report surprisingly high photoluminescence (PL) quantum efficiencies, up to 70%, in these solution-processed crystalline films. We find that photoexcitation in the pristine CH3NH3PbI3-xClx perovskite results in free charge carrier formation within 1 ps and that these free charge carriers undergo bimolecular recombination on time scales of 10s to 100s of ns. To exemplify the high luminescence yield of the CH3NH3PbI3-xClx perovskite, we construct and demonstrate the operation of an optically pumped vertical cavity laser comprising a layer of perovskite between a dielectric mirror and evaporated gold top mirrors. These long carrier lifetimes together with exceptionally high luminescence yield are unprecedented in such simply prepared inorganic semiconductors, and we note that these properties are ideally suited for photovoltaic diode operation.
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                Author and article information

                Journal
                22 September 2019
                2019-09-24
                1909.10097

                http://arxiv.org/licenses/nonexclusive-distrib/1.0/

                Custom metadata
                14 pages, 4 figures. arXiv admin note: ... => ... physics.app-ph
                physics.optics

                Optical materials & Optics

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