Molecular Insights into Early Nuclei and Interfacial Mismatch during Vapor Deposition of Hybrid Perovskites on Titanium Dioxide Substrate
Molecular Insights into Early Nuclei and Interfacial Mismatch during Vapor Deposition of Hybrid Perovskites on Titanium Dioxide Substrate
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DOI：
10.1021/acs.cgd.7b00626
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发表时间：
2017-11
影响因子：
3.8
通讯作者：
Jingfan Wang;Lingling Zhao;Mingchao Wang;Shangchao Lin
中科院分区：
文献类型：
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作者：
Jingfan Wang;Lingling Zhao;Mingchao Wang;Shangchao Lin
对杂化钙钛矿（例如典型的三碘化铅甲基铵（MAPbI3））的核结构的理论理解可以极大地提高沉积薄膜的质量和由此产生的光电器件性能。在本文中，我们报告了在不同离子前体（PbI2 和 MAI 盐）组成和温度下 MAPbI3 在 TiO2 基底上气相沉积过程中成核和界面失配的系统分子动力学模拟研究。尽管存在显着的各向异性晶格失配，但由于 I 和 Ti 原子之间的中间静电引力，在 TiO2/[MAI]0 界面处观察到了小缺陷，而 Pb 和 O 原子之间非常强的静电引力导致 TiO2/[PbI2]0 界面处存在显着缺陷。从气相沉积模拟中，我们确定 PbI42- 四面体、PbI53- 金字塔和 PbI64- 八面体是早期 MAPbI3 核的主要多面体构建块。具体来说，PbI53-金字塔......
Theoretical understanding of the nucleus structures of hybrid perovskites, such as those of the prototypical methylammonium lead triiodide (MAPbI3), can greatly improve the deposited thin film quality and the resulting optoelectronic device performance. In this paper, we report a systematic molecular dynamics simulation study on nucleation and interfacial mismatch during the vapor deposition of MAPbI3 on the TiO2 substrate under different ionic precursor (PbI2 and MAI salts) compositions and temperatures. Despite significant anisotropic lattice mismatches, small defects are observed at the TiO2/[MAI]0 interface due to intermediate electrostatic attractions between I and Ti atoms, while very strong electrostatic attractions between Pb and O atoms lead to significant defects at the TiO2/[PbI2]0 interface. From the vapor deposition simulations, we identify PbI42– tetrahedra, PbI53– pyramids, and PbI64– octahedra as dominant polyhedral building blocks of early MAPbI3 nuclei. Specifically, the PbI53– pyramids ...