Key Takeaways & Executive Findings
- •• • Ternary all-PSC with PM6:PBDTF-DTP:PYIT achieves a power conversion efficiency of 18.01%, a 16.1% relative improvement over the binary PM6:PYIT baseline (15.51%), demonstrating the efficacy of the guest donor strategy. • • The large dipole moment of the DTP-2T unit increases the dielectric constant of the active layer, which suppresses non-radiative energy loss and contributes to a higher open-circuit voltage (V_OC) in the ternary device. • • PBDTF-DTP exhibits a higher molecular electrostatic potential than the host donor, enabling fine-tuning of donor-acceptor compatibility and promoting a nanoscale fibrillar network morphology that enhances charge generation and transport while suppressing recombination. • • The guest polymer donor PBDTF-DTP deepens the highest occupied molecular orbital (HOMO) level, which is beneficial for increasing V_OC without compromising J_SC, as evidenced by the simultaneous enhancement of both parameters in the ternary device.
Abstract
All-polymer solar cells (all-PSCs) are promising for flexible and wearable electronics due to their excellent stability and mechanical stretchability. However, achieving high performance remains challenging due to difficulties in controlling the morphology of polymer blend films. In this study, a novel polymer donor, PBDTF-DTP, incorporating a weak electron-withdrawing yet large-dipole-moment dithienylphthalimide (DTP-2T) unit, was rationally designed and synthesized for ternary all-PSCs. Introducing PBDTF-DTP as a guest donor enables complementary light absorption and deepens the highest occupied molecular orbital level, simultaneously improving short-circuit current density (J_SC) and open-circuit voltage (V_OC). The large dipole moment of DTP-2T increases the dielectric constant, suppressing non-radiative energy loss and further boosting V_OC. Notably, PBDTF-DTP exhibits a relatively higher molecular electrostatic potential than the host donor, effectively tuning compatibility with both polymer donor and acceptor, regulating blend morphology, and promoting formation of a nanoscale fibrillar network. This optimized morphology facilitates efficient charge generation and transport while suppressing charge recombination. Consequently, ternary all-PSCs based on PM6:PBDTF-DTP:PYIT achieve a synergistic enhancement in J_SC, V_OC, and fill factor, yielding a remarkable power conversion efficiency of 18.01%, significantly higher than that of binary PM6:PYIT devices (15.51%). This study demonstrates that combining electrostatic potential optimization with a ternary strategy provides an effective approach to regulate morphology and achieve high-efficiency all-PSCs.
1. Introduction
All-polymer solar cells (all-PSCs) have attracted significant attention due to their excellent mechanical flexibility, stretchability, and stability, positioning them as strong candidates for flexible and wearable electronics. Despite recent advances pushing power conversion efficiencies (PCEs) to 19%, all-PSCs still lag behind small-molecule acceptor-based counterparts, which have surpassed 20%. This performance gap is primarily attributed to suboptimal phase separation and nanoscale morphology in all-polymer active layers, leading to inefficient exciton dissociation and charge transport. The large molecular dimensions, long alkyl side chains, and strong interchain entanglement of polymeric materials make achieving ideal morphology particularly challenging.
The ternary strategy has emerged as a highly effective approach to optimize the morphology of all-polymer blends by introducing an additional polymer as a third component. This approach can enhance light absorption, tune energy levels, and improve blend morphology. However, the selection of a suitable guest polymer remains critical. In this study, we introduce a novel polymer donor, PBDTF-DTP, incorporating a high-dipole-moment dithienylphthalimide unit. This design not only provides complementary absorption and deeper HOMO levels but also leverages electrostatic potential differences to regulate compatibility and morphology, addressing the long-standing bottleneck of morphology control in all-PSCs.
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Mingtao Liu, Jin Li, Feng Ding, Yuang Fu, Jinyang Yu, Peipei Zhu, Dan Liu, Meng Tao, Ruizhuo Yu, Xinhui Lu, Haiming Zhu, Xunfan Liao, Yiwang Chen (2026). Electrostatic regulation of high-dipole dithienophthalimide-based wide-bandgap polymer for efficient ternary all-polymer solar cells. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3978-0
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Frequently Asked Questions
What is the specific role of the large dipole moment of the DTP-2T unit in improving device performance?
The large dipole moment increases the dielectric constant of the active layer, which reduces exciton binding energy and suppresses non-radiative recombination losses. This leads to a higher open-circuit voltage (V_OC) and improved overall efficiency, as evidenced by the ternary device achieving 18.01% PCE compared to 15.51% for the binary device.
How does the molecular electrostatic potential of PBDTF-DTP influence blend morphology?
PBDTF-DTP exhibits a higher molecular electrostatic potential than the host donor PM6, which tunes its compatibility with both the donor and acceptor components. This promotes the formation of a nanoscale fibrillar network, enhancing charge generation and transport while suppressing recombination, as confirmed by the improved fill factor and J_SC in the ternary device.
What are the key performance metrics of the ternary all-PSC compared to the binary counterpart?
The ternary all-PSC achieves a power conversion efficiency of 18.01%, with enhanced short-circuit current density (J_SC), open-circuit voltage (V_OC), and fill factor, compared to the binary PM6:PYIT device which has a PCE of 15.51%. This represents a relative improvement of 16.1%.
What is the significance of the HOMO level deepening in PBDTF-DTP?
Deepening the HOMO level of the donor polymer increases the open-circuit voltage (V_OC) by reducing energy loss. This is achieved without compromising light absorption, as PBDTF-DTP provides complementary absorption, leading to simultaneous improvements in J_SC and V_OC.
How does the ternary strategy address the morphology challenges in all-polymer solar cells?
The ternary strategy introduces a third polymer component that can act as a compatibilizer, improving the miscibility and phase separation of the donor and acceptor polymers. In this study, PBDTF-DTP's high electrostatic potential and dipole moment facilitate the formation of a favorable nanoscale fibrillar network, which is critical for efficient exciton dissociation and charge transport, overcoming the typical limitations of all-polymer blends.
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