Interfacial and Molecular Engineering of a Helicene-Based Molecular Semiconductor for Stable and Efficient Perovskite Solar Cells,The Journal of Physical Chemistry C

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Interfacial and Molecular Engineering of a Helicene-Based Molecular Semiconductor for Stable and Efficient Perovskite Solar Cells
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2023-06-30 , DOI: 10.1021/acs.jpcc.3c02776
Zhu-Zhu Sun _{1,

2} , Run Long ₂

Affiliation

Due to the attractive optoelectronic properties and extensive application in solar cells, the design of new helicene-type molecular semiconductors is of remarkable importance for development of high-efficiency hole-transporting materials (HTMs). In this work, three helicene HTMs are constructed on the basis of the molecular conformation of experimentally reported T5H-OMeDPA by replacing the thia[5]helicene unit with a more curved π-linker of dithia[6]helicene and considering the effects of fluorine substitution. The electronic and optical properties, hole transport, and interfacial property are studied with quantum chemistry methods, and the results show that new tailored HTMs perform much better than T5H-OMeDPA in terms of the calculated HOMO levels, hole mobility, optical adsorption, solubility and stability, interfacial stability, and hole transfer. The more stable HOMO levels of new HTMs (SM31–SM33) will be beneficial for the regulation of interfacial energy alignment. Importantly, the hole mobilities of the designed HTMs are also distinctly improved due to the enhanced electronic coupling and lowered hole reorganization energies. The fluorine substitution can clearly heighten the orbital overlapping via compact molecule packing. In the meantime, dithia[6]helicene can lower the reorganization energy although the more curved π-electron system often disturbs the intermolecular π–π stacking. Moreover, our results also reveal that additional Pb–S interactions can effectually promote the interface adsorption and hole extraction. In sum, our study shows the validity of fluorine substitution and introduces helicene with a more extended structure, and three potential helicene-type HTMs are proposed.

中文翻译：

用于稳定高效钙钛矿太阳能电池的螺旋烯基分子半导体的界面和分子工程

由于具有吸引力的光电特性和在太阳能电池中的广泛应用，新型螺旋烯型分子半导体的设计对于开发高效空穴传输材料（HTM）具有重要意义。在这项工作中，基于实验报道的T5H-OMeDPA的分子构象，通过用更弯曲的二硫杂[6]螺烯的π-连接基取代硫杂[5]螺烯单元并考虑氟的影响，构建了三个螺烯HTM。代换。采用量子化学方法研究了电子和光学性质、空穴传输和界面性质，结果表明，新定制的HTM在计算的HOMO能级、空穴迁移率、光学吸附、溶解度和稳定性、界面稳定性、和空穴转移。新HTMs（SM31-SM33）更稳定的HOMO能级将有利于界面能量排列的调节。重要的是，由于电子耦合增强和空穴重组能降低，所设计的 HTM 的空穴迁移率也明显提高。氟取代可以通过紧凑的分子堆积明显提高轨道重叠。同时，二硫[6]螺烯可以降低重组能，尽管更弯曲的π电子系统经常扰乱分子间π-π堆积。此外，我们的结果还表明，额外的 Pb-S 相互作用可以有效促进界面吸附和空穴提取。总之，我们的研究证明了氟取代的有效性，并引入了具有更扩展结构的螺烯，

更新日期：2023-06-30

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