Key Takeaways & Executive Findings
- •• • D4PA-based small-area PSCs achieved a record PCE of 26.83% (certified 26.72%), surpassing the previous Me-4PACz-based certified efficiency of 26.15%, demonstrating a tangible efficiency gain for commercial viability. • • Mini-modules with an effective area of 10.86 cm2 reached a PCE of 23.37% and a certified MPPT efficiency of 22.66%, indicating scalability potential for industrial manufacturing. • • D4PA-based devices retained 97.2% of initial efficiency after 2500 hours of continuous operation at MPP under one-sun illumination, far outperforming reference devices, addressing operational stability concerns critical for long-term deployment. • • EQE-EL of D4PA-based devices was 15.25% versus 6.23% for Me-4PACz, indicating superior defect passivation and reduced non-radiative recombination, which directly translates to higher open-circuit voltage and efficiency.
Abstract
Metal halide perovskites have significantly improved solar cell performance due to their excellent optoelectronic properties. Recently, p-type small molecules such as Me-4PACz, assisted by dual-functional passivation, have enabled perovskite solar cells (PSCs) to achieve certified power conversion efficiencies (PCEs) up to 26.15%. However, issues such as molecular aggregation during solution processing limit the storage stability of precursor solutions and lead to poor molecular distribution within the film, hindering device efficiency and operational stability. Zhu's group enacted the co-deposition of a new p-type small molecule, D4PA, with perovskite. Density functional theory (DFT) investigations revealed that D4PA exhibits strong dual-terminal anchoring interactions with indium tin oxide (ITO) via two phosphonic acid groups, stabilized by intramolecular hydrogen bonding, ensuring robust adhesion and improved interface uniformity. Additionally, D4PA forms stable coordination with Pb2+ ions, suppressing defects and facilitating efficient charge transfer. Temperature-dependent Fourier-transform infrared (FTIR) spectroscopy confirmed strong binding between D4PA and perovskite, contrasting with the weaker binding of Me-4PACz. This stable interaction improves perovskite crystallinity and promotes uniform distribution of D4PA, resulting in superior photovoltaic performance. D4PA-based PSCs achieved a record PCE of 26.83% in small-area devices (certified 26.72%), and a mini-module (10.86 cm2) achieved a PCE of 23.37% with a certified MPPT efficiency of 22.66%. Devices retained 97.2% of initial efficiency after 2500 h of continuous operation at MPP under one-sun illumination. Reduced and homogeneous photoluminescence intensity indicated efficient and uniform hole extraction, and electroluminescence quantum efficiency (EQE-EL) reached 15.25%, significantly higher than 6.23% for Me-4PACz-based devices. This molecular engineering strategy provides a promising route for high-performance and high-durability inverted PSCs.
1. Introduction
The commercialization of perovskite solar cells (PSCs) has been hindered by the trade-off between efficiency and operational stability. While p-type small molecules like Me-4PACz have enabled certified efficiencies exceeding 26%, their solution processing suffers from molecular aggregation, leading to poor film uniformity and limited precursor solution storage stability. These issues compromise device performance and accelerate degradation under operational stress, posing a critical bottleneck for industrial scale-up.
Zhu's group addresses this friction by introducing a co-depositable p-type small molecule, D4PA, which features dual phosphonic acid anchoring groups that bind strongly to both the ITO substrate and the perovskite layer. This design not only suppresses molecular aggregation but also enhances interfacial adhesion and passivates deep defects. The result is a record PCE of 26.83% in small-area devices and exceptional operational stability, retaining 97.2% of initial efficiency after 2500 hours. This molecular engineering strategy offers a practical pathway to overcome the stability-efficiency trade-off, making PSCs more viable for commercial deployment.
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Shangfeng Yang (2026). Efficient Perovskite Solar Cells Enabled by Co-Depositable p-Type Small Molecules. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3636-9
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Frequently Asked Questions
What is the specific mechanism by which D4PA suppresses molecular aggregation compared to Me-4PACz, and how does this affect precursor solution storage stability?
D4PA is a chemically bonded dimer formed via C–C coupling, which inherently prevents molecular aggregation due to its rigid, extended structure. This contrasts with Me-4PACz, which aggregates during solution processing. The co-deposition method ensures uniform distribution within the perovskite film, as confirmed by reduced and homogeneous PL intensity. While the text does not provide quantitative storage stability data, the improved film uniformity and strong binding to perovskite suggest enhanced precursor stability, as aggregation is a primary cause of degradation.
How does the dual-terminal anchoring of D4PA to ITO and perovskite influence charge extraction and device efficiency?
D4PA's two phosphonic acid groups anchor to ITO via strong dual-terminal interactions, stabilized by intramolecular hydrogen bonding, ensuring robust adhesion and uniform interface. Simultaneously, D4PA coordinates with Pb2+ ions in the perovskite, passivating defects and facilitating efficient charge transfer. This dual anchoring reduces non-radiative recombination, as evidenced by a high EQE-EL of 15.25% (vs. 6.23% for Me-4PACz), leading to higher open-circuit voltage and overall PCE of 26.83%.
What are the scalability limitations of D4PA-based PSCs, and what performance metrics are achieved in larger-area devices?
Scalability is demonstrated by a mini-module with an effective area of 10.86 cm2, achieving a PCE of 23.37% and a certified MPPT efficiency of 22.66%. While this is lower than the small-area PCE due to increased series resistance and non-uniformities, the performance is among the highest reported for mini-modules, indicating that the co-deposition method can be scaled with minimal efficiency loss.
What is the operational stability of D4PA-based devices under continuous illumination, and what degradation mechanisms are mitigated?
D4PA-based devices retained 97.2% of their initial efficiency after 2500 hours of continuous operation at MPP under one-sun illumination. This exceptional stability is attributed to the strong binding of D4PA to the perovskite, which suppresses defect formation and ion migration, and the uniform distribution of D4PA, which prevents localized degradation. In contrast, reference devices with Me-4PACz degrade faster due to weaker binding and aggregation.
How does the co-deposition of D4PA with perovskite affect the crystallization process and film quality?
Temperature-dependent FTIR spectroscopy confirmed that D4PA binds strongly to the perovskite during grain growth and crystallization, with the P=O vibration peak remaining consistent. This stable interaction improves perovskite crystallinity and promotes uniform distribution of D4PA within the film, as evidenced by reduced and homogeneous PL intensity. This results in superior photovoltaic performance and stability.
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