Spiro-OMeTAD remains a prominent hole-transport material in perovskite and solid-state dye-sensitized solar cells. However, an understanding of its intrinsic hole-transport properties is still limited. Here, hole transport in spiro-OMeTAD is systematically characterized on the basis of the recently reported X-ray single-crystal data. An approach combining density functional theory calculations, tight-binding modeling, and kinetic Monte Carlo simulations are exploited to describe the key parameters governing hole transport and to investigate the transport mechanism and hole mobilities in the spiro-OMeTAD single crystal. The results provide insight into: (i) why an anisotropic hole-transport mechanism, with an upper range of intrinsic hole mobilities on the order of ~10⁻³ cm²/Vs, can be expected in the single crystal; and (ii) how detrimental factors, related to the presence of the spiro motif and of the 4,4′-dimethoxydiphenylamine substituents, limit the intrinsic hole mobilities of the system.

Spiro-OMeTAD仍然是钙钛矿和固态染料敏化太阳能电池中一种重要的空穴传输材料。然而，对其内在的空穴传输性质的理解仍然是有限的。这里，基于最近报道的X射线单晶数据，系统地表征了螺-OMeTAD中的空穴传输。利用一种结合了密度泛函理论计算，紧密结合模型和动力学蒙特卡洛模拟的方法来描述控制空穴传输的关键参数，并研究螺-​​OMeTAD单晶中的传输机理和空穴迁移率。结果提供了以下方面的见解：（i）为什么各向异性空穴传输机制的固有空穴迁移率上限在〜10 ^-3  cm ^{2的数量级}/ Vs，可以在单晶中预期；（ii）与螺旋基序和4，4′-二甲氧基二苯胺取代基的存在有关的有害因素如何限制体系的固有空穴迁移率。