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Hole transport materials (HTMs) have greatly advanced the progress of solution-based electronic devices in the past few years. Nevertheless, most devices employing dopant-free organic HTMs can only deliver inferior performance. In this work, we introduced a novel "polymer synergy" strategy to develop versatile dopant-free polymer HTMs for quantum dot/perovskite solar cells and photodetectors. With this synergy strategy, the optical, electrical and aggregation properties of polymer HTMs can be modulated, resulting in complementary absorption, high hole mobility, favorable energy landscape and moderate aggregation. Moreover, a clear orientational transition was observed for the developed HTMs with a 9-fold increase in the face-on/edge-on ratio, providing a highway-like carrier transport for electronic devices, as revealed by in situ characterization and ultrafast transient absorption. With these benefits, the photovoltaic and photodetection performance of quantum dot devices were boosted from 11.8% to 13.5% and from 2.95 x 10(12) to 3.41 x 10(13) Jones (over a 10-fold increase), respectively. Furthermore, the developed polymer HTMs can also significantly enhance the photovoltaic and photodetection performance of perovskite devices from 15.1% to 22.7% and from 2.7 x 10(12) to 2.17 x 10(13)Jones with the same device structure, indicating their great application potential in the emerging optoelectronics.

All-polymer solar cells (APSCs) are one of the most promising types of application-oriented photovoltaic technologies because they are operationally and mechanically stable; however, their low power conversion efficiency (PCE) restricts the core competitiveness against other types of solar cells. Besides, poor insight of mechanical performance, such as ductility, has been revealed for cutting-edge APSCs. Herein, we chose two well miscible polymer donors, PM6 and J71, and achieved a PCE of 16.52% for APSCs in a ternary blend with PY-IT and 15.74% for air-processed devices. The improvement is enabled by effective energy transfer, tuned crystallinity, and improved phase separation, which resulted in faster charge transfer and more balanced charge transport, suppressed exciton recombination, and more efficient charge extraction. Furthermore, the good miscibility between two donors enabled the target to have well-maintained film morphology without damaging the initial nanoscale network, bringing comparable film ductility. Last, the inner structure-property relationship of photovoltaic and morphological parameters, and film ductility was illustrated by a correlation study.

All-polymer solar cells (All-PSCs) are one of the most promising application-oriented organic photovoltaic technologies due to their excellent operational and mechanical stability. However, the power conversion efficiency (PCEs) are mostly lower than 16%, restricting their core competitiveness. Besides, the improvement of mechanical durability was rarely paid attention to cutting-edge all-PSCs. This work deployed a low-cost “technical grade” PCBM (incompletely separated but pure mixtures containing ≥ 90% [70]PCBM or [60]PCBM), into the efficient PM6:PY-IT all-polymer blend, successfully yielding a high-performance ternary device with 16.16% PCE, among the highest PCE values for all-PSCs. Meanwhile, an excellent mechanical property (i.e., crack onset strain = 11.1%) promoted from 9.5% for the ternary system is also demonstrated. The “technical grade” PCBM slightly disrupts the crystallization of polymers, and disperses well into the amorphous polymer regions of the all-PSC blends, thus facilitating charge transport and improving film ductility simultaneously. All these results confirm introducing low-cost “technical grade” PCBM with high electron mobility into all-polymer blends can improve carrier mobility, reduce charge recombination, and optimize morphology of the amorphous polymer regions, thus yielding more efficient and mechanically durable all-PSCs.

All-polymer solar cells (APSCs) are one of the most promising types of application-oriented photovoltaic technologies because they are operationally and mechanically stable; however, their low power conversion efficiency (PCE) restricts the core competitiveness against other types of solar cells. Besides, poor insight of mechanical performance, such as ductility, has been revealed for cutting-edge APSCs. Herein, we chose two well miscible polymer donors, PM6 and J71, and achieved a PCE of 16.52% for APSCs in a ternary blend with PY-IT and 15.74% for air-processed devices. The improvement is enabled by effective energy transfer, tuned crystallinity, and improved phase separation, which resulted in faster charge transfer and more balanced charge transport, suppressed exciton recombination, and more efficient charge extraction. Furthermore, the good miscibility between two donors enabled the target to have well-maintained film morphology without damaging the initial nanoscale network, bringing comparable film ductility. Last, the inner structure-property relationship of photovoltaic and morphological parameters, and film ductility was illustrated by a correlation study.

All-polymer solar cells (All-PSCs) are one of the most promising application-oriented organic photovoltaic technologies due to their excellent operational and mechanical stability. However, the power conversion efficiency (PCEs) are mostly lower than 16%, restricting their core competitiveness. Besides, the improvement of mechanical durability was rarely paid attention to cutting-edge all-PSCs. This work deployed a low-cost “technical grade” PCBM (incompletely separated but pure mixtures containing ≥ 90% [70]PCBM or [60]PCBM), into the efficient PM6:PY-IT all-polymer blend, successfully yielding a high-performance ternary device with 16.16% PCE, among the highest PCE values for all-PSCs. Meanwhile, an excellent mechanical property (i.e., crack onset strain = 11.1%) promoted from 9.5% for the ternary system is also demonstrated. The “technical grade” PCBM slightly disrupts the crystallization of polymers, and disperses well into the amorphous polymer regions of the all-PSC blends, thus facilitating charge transport and improving film ductility simultaneously. All these results confirm introducing low-cost “technical grade” PCBM with high electron mobility into all-polymer blends can improve carrier mobility, reduce charge recombination, and optimize morphology of the amorphous polymer regions, thus yielding more efficient and mechanically durable all-PSCs.

All-polymer solar cells (APSCs) are one of the most promising types of application-oriented photovoltaic technologies because they are operationally and mechanically stable; however, their low power conversion efficiency (PCE) restricts the core competitiveness against other types of solar cells. Besides, poor insight of mechanical performance, such as ductility, has been revealed for cutting-edge APSCs. Herein, we chose two well miscible polymer donors, PM6 and J71, and achieved a PCE of 16.52% for APSCs in a ternary blend with PY-IT and 15.74% for air-processed devices. The improvement is enabled by effective energy transfer, tuned crystallinity, and improved phase separation, which resulted in faster charge transfer and more balanced charge transport, suppressed exciton recombination, and more efficient charge extraction. Furthermore, the good miscibility between two donors enabled the target to have well-maintained film morphology without damaging the initial nanoscale network, bringing comparable film ductility. Last, the inner structure-property relationship of photovoltaic and morphological parameters, and film ductility was illustrated by a correlation study.