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      Resolving spatial and energetic distributions of trap states in metal halide perovskite solar cells

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          Abstract

          We report the profiling of spatial and energetic distributions of trap states in metal halide perovskite single-crystalline and polycrystalline solar cells. The trap densities in single crystals varied by five orders of magnitude, with a lowest value of 2 × 10 11 per cubic centimeter and most of the deep traps located at crystal surfaces. The charge trap densities of all depths of the interfaces of the polycrystalline films were one to two orders of magnitude greater than that of the film interior, and the trap density at the film interior was still two to three orders of magnitude greater than that in high-quality single crystals. Suprisingly, after surface passivation, most deep traps were detected near the interface of perovskites and hole transport layers, where a large density of nanocrystals were embedded, limiting the efficiency of solar cells.

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          Most cited references31

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          Solar cells. Electron-hole diffusion lengths > 175 μm in solution-grown CH3NH3PbI3 single crystals.

          Long, balanced electron and hole diffusion lengths greater than 100 nanometers in the polycrystalline organolead trihalide compound CH3NH3PbI3 are critical for highly efficient perovskite solar cells. We found that the diffusion lengths in CH3NH3PbI3 single crystals grown by a solution-growth method can exceed 175 micrometers under 1 sun (100 mW cm(-2)) illumination and exceed 3 millimeters under weak light for both electrons and holes. The internal quantum efficiencies approach 100% in 3-millimeter-thick single-crystal perovskite solar cells under weak light. These long diffusion lengths result from greater carrier mobility, longer lifetime, and much smaller trap densities in the single crystals than in polycrystalline thin films. The long carrier diffusion lengths enabled the use of CH3NH3PbI3 in radiation sensing and energy harvesting through the gammavoltaic effect, with an efficiency of 3.9% measured with an intense cesium-137 source.
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            Solar cells. Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals.

            The fundamental properties and ultimate performance limits of organolead trihalide MAPbX3 (MA = CH3NH3(+); X = Br(-) or I(-)) perovskites remain obscured by extensive disorder in polycrystalline MAPbX3 films. We report an antisolvent vapor-assisted crystallization approach that enables us to create sizable crack-free MAPbX3 single crystals with volumes exceeding 100 cubic millimeters. These large single crystals enabled a detailed characterization of their optical and charge transport characteristics. We observed exceptionally low trap-state densities on the order of 10(9) to 10(10) per cubic centimeter in MAPbX3 single crystals (comparable to the best photovoltaic-quality silicon) and charge carrier diffusion lengths exceeding 10 micrometers. These results were validated with density functional theory calculations.
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              Origin and elimination of photocurrent hysteresis by fullerene passivation in CH3NH3PbI3 planar heterojunction solar cells.

              The large photocurrent hysteresis observed in many organometal trihalide perovskite solar cells has become a major hindrance impairing the ultimate performance and stability of these devices, while its origin was unknown. Here we demonstrate the trap states on the surface and grain boundaries of the perovskite materials to be the origin of photocurrent hysteresis and that the fullerene layers deposited on perovskites can effectively passivate these charge trap states and eliminate the notorious photocurrent hysteresis. Fullerenes deposited on the top of the perovskites reduce the trap density by two orders of magnitude and double the power conversion efficiency of CH(3)NH(3)PbI(3) solar cells. The elucidation of the origin of photocurrent hysteresis and its elimination by trap passivation in perovskite solar cells provides important directions for future enhancements to device efficiency.
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                Author and article information

                Contributors
                Journal
                Science
                Science
                American Association for the Advancement of Science (AAAS)
                0036-8075
                1095-9203
                March 19 2020
                March 20 2020
                March 19 2020
                March 20 2020
                : 367
                : 6484
                : 1352-1358
                Affiliations
                [1 ]Department of Applied Physical Sciences, University of North Carolina, Chapel Hill, NC 27599, USA.
                [2 ]Department of Mechanical and Materials Engineering and Nebraska Center for Materials and Nanoscience, University of Nebraska–Lincoln, Lincoln, NE 68588, USA.
                [3 ]School of Electrical, Computer, and Energy Engineering, Arizona State University, Tempe, AZ 85287, USA.
                Article
                10.1126/science.aba0893
                32193323
                19a4949e-bf66-41b3-b653-87bc5759482f
                © 2020

                http://www.sciencemag.org/about/science-licenses-journal-article-reuse

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