摘要
为了研究卤化物钙钛矿材料的去质子化效应,以甲铵碘基钙钛矿的超胞结构为对象,设置不同H空位缺陷,利用第一性原理计算和从头算分子动力学模拟探究其去质子化效应.结果表明:去质子化产生的缺陷结构对材料结构稳定性、态密度和激发电荷分布有显著影响,会破坏结构稳定性,影响光电性能.分子动力学模拟显示,去质子化的结构会引发结构中其他MA(MA=CH_(3)NH_(3)^(+))去质子化,降低热稳定性;用FA(FA=CH(NH_(2))_(2)^(+))替换MA后,发现由于FA共轭体系大,能抑制去质子化,提升动力学稳定性.该研究揭示了去质子化效应的微观机制,为开发高稳定性卤化物钙钛矿材料及相关光电器件提供理论指导.
To investigate the deprotonation effect in halide perovskite materials,the methylammonium lead iodide perovskite was taken as the research object,according to the supercells with different H vacancy defects,the first-principles and AIMD methods were introduced to explore the deprotonation effect.The results from the first-principles calculations showed that defect structures generated by deprotonation significantly affected the material′s structural stability,density of states and charge distributions of excited states,leading to reduced structure stability and photoelectric performance.The results from the AIMD simulations revealed that deprotonated structures could trigger deprotonation of other MA(MA=CH_(3)NH_(3)^(+)),which in turn reduced the thermal stability.Replacing MA with FA(FA=CH(NH_(2))_(2)^(+))inhibited deprotonation and improved dynamic stability due to the larger conjugate system of FA.The simulation results revealed the microscopic mechanism of the deprotonation effect,providing theoretical guidance for the development of stable halide perovskite materials and related optoelectronic devices.
作者
吴燕
南广军
WU Yan;NAN Guangjun(College of Physics and Electronic Information Engineering,Zhejiang Normal University,Jinhua 321004,China)
出处
《浙江师范大学学报(自然科学版)》
2026年第1期55-62,共8页
Journal of Zhejiang Normal University:Natural Sciences
基金
国家自然科学基金资助项目(22273088)。
关键词
卤化物钙钛矿
去质子化效应
第一性原理计算
分子动力学模拟
材料稳定性
halide perovskite
deprotonation effect
first-principles calculation
molecular dynamics simulation
material stability
