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Vol. 18 (2026)

High-Efficiency Perovskite/Silicon Tandem Solar Cells Based on Wide-Bandgap Perovskite Solar Cells with Unprecedented Fill Factor

https://doi.org/10.1007/s40820-025-01959-y
Li‑Chun Chang
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
The Duong
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Viqar Ahmad
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Hualin Zhan
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Anh Dinh Bui
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Jana‑Isabelle Polzin
Division Photovoltaics, Fraunhofer Institute for Solar Energy Systems ISE, Heidenhofstrasse 2, 79110 Freiburg, Germany
Armin Richter
Division Photovoltaics, Fraunhofer Institute for Solar Energy Systems ISE, Heidenhofstrasse 2, 79110 Freiburg, Germany
Gabriel Bartholazzi
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Keqing Huang
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Zhongshu Yang
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Wei Wang
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Yihui Hou
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Li Li
Research School of Physics, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Qian Cui
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Rabin Basnet
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Jianfei Yang
State Key Laboratory of New Ceramics & Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, People’s Republic of China
Hong Lin
State Key Laboratory of New Ceramics & Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, People’s Republic of China
Guozheng Du
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Khoa Nguyen
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Dang‑Thuan Nguyen
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Lachlan E. Black
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Daniel MacDonald
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Daniel Walter
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Klaus J. Weber
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Kylie R. Catchpole
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia
Heping Shen
School of Engineering, The Australian National University, Canberra, Australian Capital Territory 2601, Australia

Corresponding Author: Heping Shen

Heping.Shen@anu.edu.au

Nano-Micro Letters, Vol. 18 (2026), Article Number: 122

Abstract

Recent progress in inverted perovskite solar cells (iPSCs) highlights the critical role of interface engineering between the charge transport layer and perovskite. Self-assembled monolayers (SAM) on transparent conductive oxide electrodes serve effectively as hole transport layers, though challenges such as energy mismatches and surface inhomogeneities remain. Here, a blended self-assembled monolayer of (2-(9H-carbazol-9-yl)ethyl)phosphonic acid (2PACz) and (4-(3,6-Dimethyl-9H-carbazol-9-yl)butyl)phosphonic acid (Me-4PACz) is developed, offering improved surface potential uniformity and interfacial energy alignment compared to individual SAMs. Interactions between the SAMs and ionic species are investigated with simulation analysis conducted, revealing the elimination of interfacial energy barriers through precise energy-level tuning. This strategy enables wide-bandgap (1.67 eV) perovskite solar cells with inverted structures with over 24% efficiency, an open-circuit voltage (Voc) of 1.268 V, and a certified fill factor (FF) of 86.8%, leading to a certified efficiency of 23.42%. The approach also enables high-efficiency semi-transparent devices and a mechanically stacked four-terminal perovskite/silicon tandem solar cell reaching 30.97% efficiency.


Highlights:
1 By mixing 2PACz and Me-4PACz, an energetically homogeneous buried interface is formed, enabling preferential energy alignment at the hole transport layer/perovskite (1.67 eV) interface, which delivers a certified fill factor of 86.8% and a power conversion efficiency of 23.42%.
2 Simulations indicate that at lower interface defect densities (1 × 108–1 × 1011 cm−2), improvements in FF dominate the device performance, whereas at higher defect densities (1 × 1012–1 × 1013 cm−2), Voc is the key factor.

Keywords

Inverted perovskite solar cells Self-assembled monolayers Interface energy-level alignment Wide-bandgap perovskite Tandem solar cells
Chang, Li‑Chun, The Duong, Viqar Ahmad, Hualin Zhan, Anh Dinh Bui, Jana‑Isabelle Polzin, Armin Richter, Gabriel Bartholazzi, Keqing Huang, Zhongshu Yang, Wei Wang, Yihui Hou, Li Li, Qian Cui, Rabin Basnet, Jianfei Yang, Hong Lin, Guozheng Du, Khoa Nguyen, Dang‑Thuan Nguyen, Lachlan E. Black, Daniel MacDonald, Daniel Walter, Klaus J. Weber, Kylie R. Catchpole, and Heping Shen. 2026. “High-Efficiency Perovskite/Silicon Tandem Solar Cells Based on Wide-Bandgap Perovskite Solar Cells With Unprecedented Fill Factor”. Nano-Micro Letters 18 (January):122. https://doi.org/10.1007/s40820-025-01959-y.
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