Citation: Shantao Zhang, TianAo Hou, Yandong Wang, Zhimin Fang, Yu Wu, Haolin Wang, Tao Chen, Shuang Chen, Wenhua Zhang, Shengzhong (Frank) Liu, Shangfeng Yang. π-Conjugation-extended dinaphthocarbazole phosphonic acid as a hole-selective layer for inverted perovskite solar cells[J]. Acta Physico-Chimica Sinica, ;2026, 42(3): 100194. doi: 10.1016/j.actphy.2025.100194 shu

π-Conjugation-extended dinaphthocarbazole phosphonic acid as a hole-selective layer for inverted perovskite solar cells

1.
State Key Laboratory of Precision and Intelligent Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Materials Science and Engineering, University of Science and Technology of China, Hefei 230026, Anhui Province, China;
2.
Institute of Technology for Carbon Neutralization, Yangzhou University, Yangzhou 225127, Jiangsu Province, China;
3.
Key Laboratory of Photoelectric Conversion and Utilization of Solar Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning Province, China;
4.
Yunnan Key Laboratory of Carbon Neutrality and Green, Low-carbon Technologies, School of Materials and Energy, Yunnan University, Kunming 650000, Yunnan Province, China;
5.
Kuang Yaming Honors School, Nanjing University, Nanjing 210023, Jiangsu Province, China

Corresponding author: Zhimin Fang, Shengzhong (Frank) Liu, Shangfeng Yang,
Received Date: 17 July 2025
Revised Date: 13 September 2025
Accepted Date: 23 September 2025

In the rapidly evolving field of photovoltaic technology, self-assembled monolayers (SAMs) have become essential hole-selective layers (HSLs) for inverted perovskite solar cells (PSCs). SAMs not only determine interfacial hole extraction but also significantly influence the film quality of the atop perovskite layers, consequently affecting the efficiency and stability of perovskite solar cells. Among various SAMs, carbazole-based SAMs, exemplified by 4PACZ, have emerged as prominent due to their electron-rich characteristics, making them some of the most prevalent HSLs in modern inverted PSCs. Nevertheless, 4PACZ exhibits significant limitations: one major issue is its limited molecular dipole, which leads to insufficient energy level alignment between the treated substrate and the perovskite, causing substantial interfacial energy loss. Another critical challenge is the flat structure of the carbazole unit, which often promotes molecular stacking, resulting in incomplete substrate coverage and non-uniform film formation, thereby compromising both device performance and stability. In this study, we designed a novel SAM based on a polycyclic aromatic hydrocarbon derivative, (4-(8H-dinaphtho[2,3-c:2',3'-g]carbazol-8-yl)butyl)phosphonic acid (4PADNC), with the aim of optimizing hole transport in inverted PSCs. This SAM incorporates the structurally extended dinaphtho[2,3-c:2',3'-g]carbazole (DNC) as the functional terminal group, replacing the single carbazole unit in the traditional material 4PACZ. The key structural difference is that the DNC group provides a significantly expanded π-conjugated skeleton and enhanced electron-rich characteristics. These features not only greatly enhance hole extraction and transport at the interface but also induce a significant increase in the molecular dipole moment, which is crucial for effectively adjusting the work function of ITO, ensuring proper alignment with the perovskite layer. Additionally, there is an intramolecular dihedral angle of approximately 34.62° in the DNC unit at the core of 4PADNC. This non-planar configuration contrasts sharply with the planar carbazole structure. The larger dihedral angle effectively suppresses excessive π-π stacking between molecules, which not only aids in forming a denser and more ordered molecular layer on the ITO surface but also provides a more favorable and defect-free substrate for the growth of the upper perovskite. With these upgrades, the inverted PSCs based on 4PADNC achieved a PCE as high as 24.32%, compared to 22.89% for the control devices based on 4PACZ. Furthermore, the 4PADNC-based devices also exhibited superior thermal stability and operational stability.
- Perovskite solar cells,
- Hole-selective layer,
- Self-assembled monolayer,
- Dinaphtho carbazole,
- π-conjugation
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沈阳化工大学材料科学与工程学院沈阳 110142