Park Su Min, Park Sang Wook, Jin Haedam, Baek Dohun, Cha Jeongbeom, Chae Weon-Sik, Lee Tae Kyung, Kim Min
School of Chemical Engineering, Clean Energy Research Center, Jeonbuk National University (JBNU), Jeonju, 54896, Republic of Korea.
Department of Materials Engineering and Convergence Technology, Gyeongsang National University (GNU), Jinju, 52828, Republic of Korea.
Small. 2024 Nov;20(46):e2404958. doi: 10.1002/smll.202404958. Epub 2024 Aug 13.
Organic-inorganic hybrid perovskites have attracted significant attention for optoelectronic applications due to their efficient photoconversion properties. However, grain boundaries and irregular crystal orientations in polycrystalline films remain issues. This study presents a method for producing crystalline-orientation-controlled perovskite single-crystal films using retarded solvent evaporation. It is shown that single-crystal films, grown via inverse temperature crystallization within a confined space, exhibit enhanced optoelectronic property. Using interfacial polymer layer, this method produces high-quality perovskite single-crystalline films with varying crystal orientations. Density functional theory calculations confirm favorable adsorption energies for (110) surfaces with methylammonium iodide and PbI terminations on poly(3-hexylthiophene), and stronger adsorption for (224) surfaces with I and methylammonium terminations on polystyrene, influenced by repulsive forces between the thiophene group and the perovskite surface. The correlation between charge transport characteristics and perovskite single-crystalline properties highlights potential advancements in perovskite optoelectronics, improving device performance and reliability.
有机-无机杂化钙钛矿因其高效的光电转换特性而在光电子应用中备受关注。然而，多晶薄膜中的晶界和不规则晶体取向仍然是问题。本研究提出了一种利用延迟溶剂蒸发制备晶体取向可控的钙钛矿单晶薄膜的方法。结果表明，通过在受限空间内进行逆温结晶生长的单晶薄膜表现出增强的光电性能。利用界面聚合物层，该方法可制备出具有不同晶体取向的高质量钙钛矿单晶薄膜。密度泛函理论计算证实，在聚（3-己基噻吩）上，甲基碘化铵和PbI端基的(110)表面具有良好的吸附能，而在聚苯乙烯上，I和甲基铵端基的(224)表面受噻吩基团与钙钛矿表面之间的排斥力影响，吸附更强。电荷传输特性与钙钛矿单晶性质之间的相关性突出了钙钛矿光电子学的潜在进展，提高了器件性能和可靠性。
