Properties of three organic hole transport materials (HTMs), FDT, PEH-2, and SNE (See Scheme 1) are investigated by combination of molecular dynamics and first principle calculations. Besides the isolated molecules, the interfacial properties of HTMs adsorbed on CH₃NH₃PbI₃ (110) surface are firstly theoretically investigated in detail to evaluate the HTM performance. The overall performance of isolated HTMs is evaluated in terms of frontier molecular orbital, absorption spectrum, and hole mobility. After HTMs are adsorbed on CH₃NH₃PbI₃ (110) surface, the significantly reduced band gap of SNE can improve the light harvesting ability of perovskite solar cells (PSCs). Moreover, the energy difference between HOMO energy level of HTM and valence band of CH₃NH₃PbI₃ (110) surface for SNE is the smallest in three studied molecules indicating the largest V_oc of PSCs. Although HTM-CH₃NH₃PbI₃ system is closer to the real environment than isolated HTMs, the adsorbed HTM-CH₃NH₃PbI₃ is rarely considered because of its expensive computational cost and structural complexity. We expected that this work would be helpful to deeply understand the property of HTMs applied in PSCs.

通过结合分子动力学和第一性原理计算研究了三种有机空穴传输材料（HTM），FDT，PEH-2和SNE（参见方案1）的性能。除分离的分子外，首先在理论上详细研究了吸附在CH ₃ NH ₃ PbI ₃（110）表面上的HTM的界面性质，以评估HTM性能。孤立的HTM的整体性能是根据前沿的分子轨道，吸收光谱和空穴迁移率来评估的。HTMs吸附在CH ₃ NH ₃ PbI ₃（110）表面后，SNE的带隙显着减小可以提高钙钛矿太阳能电池（PSC）的光收集能力。此外，HTM的HOMO能级和CH的价带之间的能量差₃ NH ₃碘化铅₃（110）面为SNE是在表示最大v三个研究分子的最小_OC的PSC。尽管HTM-CH ₃ NH ₃ PbI ₃系统比分离的HTM更接近真实环境，但吸附的HTM-CH ₃ NH ₃ PbI ₃由于其昂贵的计算成本和结构复杂性，很少考虑使用这种方法。我们希望这项工作将有助于深入了解应用于PSC的HTM的属性。