Key Takeaways & Executive Findings
- •• • THPC extends film formation kinetics by 1.4×, suppressing explosive nucleation in PM6:L8-BO-X blends and enabling ordered fibrous morphology; this translates to a PCE of 20.19% versus 18.67% for PEDOT:PSS, directly addressing the industrial need for reproducible high-throughput coating. • • Non-radiative recombination loss is reduced from 0.243 eV to 0.227 eV, and open-circuit voltage increases from 0.866 V to 0.883 V; these metrics are critical for closing the gap to the Shockley-Queisser limit and enhancing device stability under operational stress. • • THPC's deep work function of 5.32 eV increases built-in potential and reduces interfacial trap density, facilitating charge extraction; this enables broad applicability across Y-series acceptors, with D18:L8-BO achieving 20.55% PCE, demonstrating robustness for diverse material systems. • • The low surface energy of THPC improves interfacial compatibility with hydrophobic active layers, mitigating defects and vertical phase separation issues inherent to hydrophilic PEDOT:PSS; this is essential for scaling to roll-to-roll manufacturing where interfacial control dictates yield and lifetime.
Abstract
Self-assembled monolayers (SAMs) enable precise tuning of the ITO/active layer interfacial dipole, yet their impact on the crystallization kinetics of the overlying active layer remains poorly understood, limiting their potential in high-efficiency organic solar cells. This study introduces THPC, a self-assembling material with an extended carbazole core and heteroatom substitution, as a hole transport layer (HTL). Unlike the hydrophilic PEDOT:PSS, THPC exhibits low surface energy, providing a favorable template that extends the film formation kinetics of the PM6:L8-BO-X blend by nearly 1.4 times, mitigating the explosive nucleation prevalent in PM6-based active layers. This promotes a highly ordered fibrous morphology and enhances vertical phase separation. The deep work function of THPC (5.32 eV) increases the built-in potential, reduces interfacial trap density, and facilitates charge extraction. Consequently, non-radiative recombination loss decreases from 0.243 eV to 0.227 eV, and the open-circuit voltage rises from 0.866 V to 0.883 V, yielding a power conversion efficiency (PCE) of 20.19%, outperforming the PEDOT:PSS control (18.67%). This finding is confirmed across multiple Y-series acceptors, all approaching 20% PCE. Notably, the D18:L8-BO system achieves a PCE of 20.55%, demonstrating broad applicability.
1. Introduction
Conventional organic solar cells rely on PEDOT:PSS as the hole transport layer, but its high hydrophilicity and excessive surface energy disrupt interfacial compatibility with hydrophobic active layers, causing defects and poor vertical phase separation. This limits charge extraction and contributes to non-radiative recombination losses, capping power conversion efficiencies (PCEs) below 19% for PM6-based systems. The explosive nucleation kinetics of PM6:small molecule acceptor blends further exacerbate morphological disorder, hindering the formation of bicontinuous interpenetrating networks essential for efficient charge transport.
THPC, a self-assembled monolayer with an extended carbazole core and heteroatom substitution, addresses these bottlenecks by simultaneously modulating the interfacial dipole and film formation kinetics. Its low surface energy extends the film formation window by 1.4 times, promoting ordered fibrous morphology and vertical phase separation. The deep work function of 5.32 eV enhances built-in potential and reduces trap density, leading to a PCE of 20.19% and a non-radiative recombination loss of 0.227 eV, outperforming PEDOT:PSS controls. This protocol offers a scalable route to low-energy-loss organic photovoltaics with broad acceptor compatibility.
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CHEN Wei, QIU Shuwei, ZENG Xiaoya, ZHANG Qidi, ZHUANG Yunxiang, XIE Chen, YOU Peng, SHAN Tong, BAI Qing, CHEN Lu, LI Shunpu, JIA Tiekun, WANG Yufei, ZHANG Guangye (2026). Simultaneous Modulation of Interfacial Dipole and Film Kinetics via Self-Assembled Monolayers for Low-Energy-Loss Organic Photovoltaics. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-026-4391-5
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Frequently Asked Questions
What is the operational mechanism by which THPC reduces non-radiative recombination loss compared to PEDOT:PSS?
THPC's deep work function (5.32 eV) increases the built-in potential and reduces interfacial trap density, as evidenced by the decrease in non-radiative recombination loss from 0.243 eV to 0.227 eV. This is achieved through improved energy level alignment and reduced defect states at the ITO/active layer interface, facilitating charge extraction and suppressing recombination pathways.
How does the surface energy of THPC influence the crystallization kinetics of the PM6:L8-BO-X blend?
THPC's low surface energy provides a favorable template that extends the film formation kinetics by nearly 1.4 times, mitigating explosive nucleation. This allows for controlled aggregation and crystallization, resulting in a highly ordered fibrous morphology and enhanced vertical phase separation, which are critical for efficient charge transport and reduced recombination.
What are the scalability challenges for integrating THPC into roll-to-roll manufacturing, and how does its performance compare to PEDOT:PSS?
THPC's self-assembling nature and low surface energy enable uniform coating on ITO, compatible with roll-to-roll processes. It achieves a PCE of 20.19% versus 18.67% for PEDOT:PSS, with improved interfacial properties. However, long-term stability under ambient conditions and cost parity with PEDOT:PSS require further validation, particularly regarding moisture sensitivity and batch-to-batch reproducibility.
Does the use of THPC affect the thermal stability or lifetime of the organic solar cells under operational stress?
The reduced interfacial trap density and enhanced vertical phase separation suggest improved thermal stability, as fewer defects mitigate degradation pathways. However, specific degradation rates under accelerated aging (e.g., 85°C/85% RH) are not provided in the current study. The non-radiative recombination loss reduction to 0.227 eV indicates lower energy loss, which may correlate with extended lifetime, but empirical stability data are needed.
How does THPC perform with other Y-series acceptors, and what is the evidence for broad applicability?
THPC was tested with multiple Y-series acceptors, all approaching 20% PCE. Notably, the D18:L8-BO system achieved a PCE of 20.55%, demonstrating broad applicability. This suggests that THPC's interfacial modulation is effective across different donor-acceptor combinations, likely due to its universal ability to tune surface energy and work function, enabling optimized morphology and charge extraction.
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