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Self-Assembled Perovskite Nanoislands on CH3NH3PbI3 Cuboid Single Crystals by Energetic Surface Engineering
Authors:Yurou Zhang  Dohyung Kim  Jung-Ho Yun  Jongchul Lim  Min-Cherl Jung  Xiaoming Wen  Jan Seidel  Eunyoung Choi  Mu Xiao  Tengfei Qiu  Miaoqiang Lyu  EQ Han  Mehri Ghasemi  Sean Lim  Henry J Snaith  Jae Sung Yun  Lianzhou Wang
Affiliation:1. Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology (AIBN), The University of Queensland, St. Lucia, QLD, 4027 Australia;2. Joint Institute for Advanced Materials, Department of Materials Science and Engineering, University of Tennessee, Knoxville, TN, 37996 USA

School of Materials Science and Engineering, University of New South Wales, Sydney, NSW, 2052 Australia;3. Clarendon Laboratory, Department of Physics, University of Oxford, Oxford, OX1 3PU UK

Graduate School of Energy Science and Technology (GEST), Chungnam National University, Daejeon, 34134 South Korea;4. Division of Materials Science, Faculty of Pure and Applied Sciences, University of Tsukuba, Ibaraki, 305-8577 Japan;5. Centre for Translational Atomaterials, Swinburne University of Technology, Hawthorn, VIC, 3122 Australia;6. School of Materials Science and Engineering, University of New South Wales, Sydney, NSW, 2052 Australia;7. Australian Centre for Advanced Photovoltaics (ACAP), School of Photovoltaic and Renewable Energy Engineering, University of New South Wales, Sydney, NSW, 2052 Australia;8. Electron Microscope Unit, University of New South Wales, Sydney, NSW, 2052 Australia;9. Clarendon Laboratory, Department of Physics, University of Oxford, Oxford, OX1 3PU UK

Abstract:Organometal perovskite single crystals have been recognized as a promising platform for high-performance optoelectronic devices, featuring high crystallinity and stability. However, a high trap density and structural nonuniformity at the surface have been major barriers to the progress of single crystal-based optoelectronic devices. Here, the formation of a unique nanoisland structure is reported at the surface of the facet-controlled cuboid MAPbI3 (MA = CH3NH3+) single crystals through a cation interdiffusion process enabled by energetically vaporized CsI. The interdiffusion of mobile ions between the bulk and the surface is triggered by thermally activated CsI vapor, which reconstructs the surface that is rich in MA and CsI with reduced dangling bonds. Simultaneously, an array of Cs-Pb-rich nanoislands is constructed on the surface of the MAPbI3 single crystals. This newly reconstructed nanoisland surface enhances the light absorbance over 50% and increases the charge carrier mobility from 56 to 93 cm2 V?1 s?1. As confirmed by Kelvin probe force microscopy, the nanoislands form a gradient band bending that prevents recombination of excess carriers, and thus, enhances lateral carrier transport properties. This unique engineering of the single crystal surface provides a pathway towards developing high-quality perovskite single-crystal surface for optoelectronic applications.
Keywords:CH 3NH 3PbI 3  nanoislands  perovskite single crystals  self-assembled perovskite  surface engineering
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