甲脒
钙钛矿(结构)
八面体
卤化物
化学物理
碘化物
化学
铯
相(物质)
结晶学
材料科学
无机化学
晶体结构
有机化学
作者
Giuseppe Fisicaro,Antonino La Magna,Alessandra Alberti,Emanuele Smecca,Giovanni Mannino,Ioannis Deretzis
标识
DOI:10.1021/acs.jpclett.9b03763
摘要
Halide perovskites containing a mixture of formamidinium (FA+), methylammonium (MA+) and cesium (Cs+) cations are the actual standard for obtaining record-efficiency perovskite solar cells. Although the compositional tuning that brings to optimal performance of the devices has been largely established, little is understood on the role of even small quantities of MA+ or Cs+ in stabilizing the black phase of FAPbI3 while boosting its photovoltaic yield. In this paper, we use Car-Parrinello molecular dynamics in large supercells containing different ratios of FA+ and either MA+ or Cs+, in order to study the structural and kinetic features of mixed perovskites at room temperature. Our analysis shows that cation mixing relaxes the rotational disorder of FA+ molecules by preferentially aligning their axis toward ⟨100⟩ cubic directions. The phenomenon stems from the introduction of additional local minima in the energetic landscape, which are absent in pure FAPbI3 crystals. As a result, a higher structural order is achieved, characterized by a pronounced octahedral tilting and a lower vibrational activity for the inorganic framework. We show that both MA+ and Cs+ are qualified for this enhancement, with Cs+ being particularly effective when diluted within the FAPbI3 perovskite.
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