Key Takeaways & Executive Findings
- •• TbCl3 doping improves the buried interface between Me-4PACz and CsPbI3, enhancing crystallinity and passivating defects. • Inverted CsPbI3 PSCs achieve a remarkable efficiency of 18.68% with enhanced ambient stability. • Efficiencies of 29.40% (4T) and 25.44% (2T) are achieved in all-inorganic perovskite/silicon tandem devices, among the highest reported. • This work provides a novel metal halide doping strategy for high-performance and stable inverted all-inorganic PSCs and tandem solar cells.
Abstract
All-inorganic perovskite materials exhibit exceptional thermal stability and promising candidates for tandem devices, while their application is still in the initial stage. Here, a metal halide doping strategy was implemented to enhance device performance and stability for inverted CsPbI3 perovskite solar cells (PSCs), which are ideal for integration into perovskite/silicon tandem solar cells. The lanthanide compound terbium chloride (TbCl3) was employed to improve buried interface between [4-(3,6-Dimethyl-9H-carbazol-9-yl) butyl] phosphonic acid (Me-4PACz) and perovskite layer, thereby enhancing the crystallinity of CsPbI3 films and passivating non-radiative recombination defects. Thus, the inverted CsPbI3 PSCs achieved an efficiency of 18.68% and demonstrated excellent stability against water and oxygen. Meanwhile, remarkable efficiencies of 29.40% and 25.44% were, respectively, achieved in four-terminal (4T) and two-terminal (2T) perovskite/silicon mechanically tandem devices, which are higher efficiencies among reported all-inorganic perovskite-based tandem solar cells. This study presents a novel approach for fabricating highly efficient and stable inverted all-inorganic PSCs and perovskite/silicon tandem solar cells.
1. Introduction
All-inorganic CsPbI3−xBrx (0 ≤ x ≤ 3) perovskites demonstrate exceptional thermal stability (> 300 °C) and possess an adjustable optical bandgap ranging from 1.7 to 2.3 eV, offering significant potential for integration into tandem devices with silicon and organic solar cells [1–5]. The efficiency of single-junction CsPbI3−xBrx perovskite solar cells (PSCs) has rapidly surpassed 22% [6–9]. However, the commonly used hole transport layer (HTL) of 2,2′,7,7′-tetrakis [N,N-di(4-methoxyphenyl)amino]-9,9′-spirobifluorene (spiro-OMeTAD) exhibits high parasitic absorption, which hinders its application in tandem devices. Additionally, the 4-tert-butylpyridine (t-BP) and Li-bis(trifluoromethanesulfonyl) imide (Li-TFSI) dopants could absorb moisture from the air, negatively impacting device stability [10–12]. Compared to the conventional structure, the electron transport layer (ETL) of inverted structure can protect the perovskite layer, exhibiting superior moisture stability and reduced hysteresis effects [13, 14]. Consequently, inverted PSCs have become a focal point of research in the photovoltaic field.
Inverted all-inorganic PSCs primarily utilize CsPbI3 and CsPbI2Br perovskite materials. Snaith et al. [15] first reported inverted CsPbI3 PSCs with an efficiency of 1.7%, which has since rapidly increased to achieve a record efficiency of 20.6% [16]. Compared to conventional structures, inverted all-inorganic PSCs exhibit inferior photovoltaic performance and larger open-circuit voltage (VOC) losses due to mismatched energy level alignment. Among common hole transport materials (HTMs), the hydrophilicity and acidity of PEDOT reduce interface stability, consequently decreasing the VOC [17–19]. The wettability of precursor on the surfaces of poly[bis(4-phenyl) (2,4,6-trimethylphenyl) amine] (PTAA) is low, deteriorating the growth of perovskite films. The high annealing temperature restricts the application of organic HTLs in all-inorganic PSCs [20]. And, nickel oxide (NiOx) possesses low conductivity and high surface defects (Ni3+), which could hinder hole transfer, increase non-radiative recombination and accelerate perovskite degradation [14, 21]. Moreover, there is a detrimental reaction between NiOx and dimethylammonium iodide (DMAI) in CsPbI3, which adversely affects device performance [22]. The energy mismatch between the all-inorganic perovskite film and the HTL/ETL also results in lower efficiency of inverted devices [19]. Tremendous efforts have been dedicated to optimizing the interface between perovskite and charge transport layers for synchronously enhanced PCE and stability of PSCs, such as bilayer homojunctions, ion-modulated radical doping [10–12, 23, 24]. Therefore, excellent charge transport materials can improve the crystallization of perovskite films and facilitate charge extraction at the interface.
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Wenming Chai, Weidong Zhu, He Xi, Dazheng Chen, Hang Dong, Long Zhou, Hailong You, Jincheng Zhang, Chunfu Zhang, Chunxiang Zhu, Yue Hao (2025). Buried Interface Regulation with TbCl3 for Highly-Efficient All-Inorganic Perovskite/Silicon Tandem Solar Cells. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01763-8
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Frequently Asked Questions
What is the main contribution of this paper?
The paper introduces a metal halide doping strategy using TbCl3 to regulate the buried interface in inverted CsPbI3 perovskite solar cells, achieving high efficiency and stability, and demonstrates record efficiencies in all-inorganic perovskite/silicon tandem devices.
What efficiency was achieved for the inverted CsPbI3 PSCs?
The inverted CsPbI3 PSCs achieved an efficiency of 18.68% with enhanced stability against water and oxygen.
What are the efficiencies of the tandem devices?
The four-terminal (4T) and two-terminal (2T) perovskite/silicon mechanically tandem devices achieved efficiencies of 29.40% and 25.44%, respectively.
How does TbCl3 improve device performance?
TbCl3 improves the wettability of Me-4PACz, enhances crystallization of CsPbI3 films, passivates iodine vacancies with Cl− ions, and improves energy level alignment at the buried interface, reducing non-radiative recombination.
What is the significance of this work for tandem solar cells?
This work provides a novel approach for fabricating highly efficient and stable inverted all-inorganic PSCs, which are ideal for integration into perovskite/silicon tandem solar cells, achieving among the highest efficiencies reported for all-inorganic perovskite-based tandems.
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