Achieving 20% Toluene-Processed Binary Organic Solar Cells via Secondary Regulation of Donor Aggregation in Sequential Processing

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Achieving 20% Toluene-Processed Binary Organic Solar Cells via Secondary Regulation of Donor Aggregation in Sequential Processing
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Achieving 20% Toluene-Processed Binary Organic Solar Cells via Secondary Regulation of Donor Aggregation in Sequential Processing - Nano-Micro Letters

Sequential processing (SqP) of the active layer offers independent optimization of the donor and acceptor with more targeted solvent design, which is considered the most promising strategy for achieving efficient organic solar cells (OSCs). In the SqP method, the favorable interpenetrating network seriously depends on the fine control of the bottom layer swelling. However, the choice of solvent(s) for both the donor and acceptor have been mostly based on a trial-and-error manner. A single solvent often cannot achieve sufficient yet not excessive swelling, which has long been a difficulty in the high efficient SqP OSCs. Herein, two new isomeric molecules are introduced to fine-tune the nucleation and crystallization dynamics that allows judicious control over the swelling of the bottom layer. The strong non-covalent interaction between the isomeric molecule and active materials provides an excellent driving force for optimize the swelling-process. Among them, the molecule with high dipole moment promotes earlier nucleation of the PM6 and provides extended time for crystallization during SqP, improving bulk morphology and vertical phase segregation. As a result, champion efficiencies of 17.38% and 20.00% (certified 19.70%) are achieved based on PM6/PYF-T-o (all-polymer) and PM6/BTP-eC9 devices casted by toluene solvent.

Researchers from Shenzhen Technology University and collaborative institutions, led by Professor Guangye Zhang, have achieved a major milestone in organic solar cell (OSC) technology. Their latest work, published in Nano-Micro Letters, introduces a novel additive engineering strategy that enables 20.0% power conversion efficiency (PCE) in binary OSCs processed entirely with non-halogenated solvents. This advancement not only sets a new benchmark for toluene-processed OSCs but also offers a scalable and eco-friendly approach aligned with industrialization needs.

Why This Innovation Matters

  • Certified 20% Efficiency with Toluene: A remarkable PCE of 20.0% (certified at 19.7%) is achieved in PM6/BTP-eC9 OSCs, surpassing many halogen-solvent-processed devices.
  • Green and Scalable Fabrication: The entire process uses toluene—a non-halogen, high-boiling solvent—avoiding toxic solvents like chloroform, which are unsuitable for large-scale manufacturing.
  • Universal Additive Strategy: The strategy is shown to be effective across multiple systems, including PM6/PYF-T-o, PM6/L8-BO, and PM6/PJ1-γ, offering wide applicability.

Key Innovation: Additive-Guided Secondary Nucleation Control

To address the longstanding challenge of morphology control in sequentially processed OSCs (SqP), the team introduced two isomeric additives, ODBC and PDBC, into either the donor or acceptor layers. These additives regulate the swelling and aggregation behaviors of the active materials through non-covalent interactions, allowing for precise modulation of film morphology.

  • Dipole-Driven Control: ODBC, with a higher dipole moment, promotes earlier nucleation and tighter π–π stacking, leading to enhanced crystallinity and exciton dissociation.
  • Additive Placement Matters: Adding the additive into the acceptor layer rather than the donor layer produces significantly better morphology and charge transport properties.
  • Drying Kinetics Optimization: The high boiling points of ODBC/PDBC extend the drying window, promoting homogeneous phase separation and vertical phase segregation.

Unprecedented Device Performance

  • PM6/PYF-T-o Devices: Achieved a champion PCE of 38%, surpassing chloroform-casted blend devices (16.81%) and marking the highest efficiency for this binary system.
  • PM6/BTP-eC9 Devices: With ODBC and 2PACZ as a hole transport layer, a certified PCE of 19.7% is reached—the highest ever for non-halogenated solvent-processed binary OSCs.
  • Improved Charge Dynamics:
    • High short-circuit current (JSC) up to 2 mAcm-2.
    • Balanced and enhanced carrier mobilities (μe≈ μh ≈ 7.7 × 10⁻4 cm2 V-1 s-1).
    • Reduced bimolecular recombination and improved charge extraction, validated through photo-CELIV and transient photovoltage measurements.

Mechanistic Insights and Morphology Control

  • In Situ Absorption and AFM: Extended drying times and smaller RMS roughness confirm finer microstructures.
  • GIWAXS Analysis: Improved π–π stacking (d-spacing ~3.67 Å, CCL ~11.14 Å) supports better charge transport.
  • Vertical Composition Profiling: FDDLAS and FLAS analyses reveal more uniform donor/acceptor distribution, promoting efficient exciton dissociation and charge collection.
  • Ultrafast Spectroscopy: Transient absorption experiments indicate enhanced hole transfer and stronger interfacial charge generation in ODBC-treated devices.

Robust Stability and Broad Applicability

  • Stability: Devices with ODBC show superior light and thermal stability, retaining over 88% of PCE after 500 hours of continuous illumination.
  • Universality: The additive strategy was extended to various binary OSC systems, consistently improving performance:
    • PM6/L8-BO: Increased from 16.95% to 16%.
    • PM6/PJ1-γ: Increased from 14.36% to 41%.

Future Outlook

This study establishes a practical, scalable pathway toward high-efficiency, halogen-free OSCs by leveraging additive-induced secondary nucleation control in the SqP framework. The use of isomeric additives like ODBC offers a powerful handle for morphology tuning, enabling enhanced crystallinity, charge transport, and long-term stability. With compatibility across multiple systems and processing conditions, this strategy holds promise for industrial-scale, environmentally friendly production of organic photovoltaics.

Stay tuned for more from Professor Guangye Zhang’s team as they continue to push the frontiers of green, high-performance organic solar technologies!

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Materials Chemistry
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  • Nano-Micro Letters Nano-Micro Letters

    Nano-Micro Letters is a peer-reviewed, international, interdisciplinary and open-access journal that focus on science, experiments, engineering, technologies and applications of nano- or microscale structure and system in physics, chemistry, biology, material science, and pharmacy.