Insights Into Preaggregation Control of Y-Series Nonfullerene Acceptors in Liquid State for Highly Efficient Binary Organic Solar Cells.

Leveraging breakthroughs in Y-series nonfullerene acceptors (NFAs), organic solar cells (OSCs) have achieved impressive power conversion efficiencies (PCEs) exceeding 19%. However, progress in advancing OSCs has decelerated due to constraints in realizing the full potential of the Y-series NFAs. Herein, a simple yet effective solid additive-induced preaggregation control method employing 2-chloro-5-iodopyridine (PDCI) is reported to unlock the full potential of the Y-series NFAs. Specifically, PDCI interacts predominantly with Y-series NFAs enabling enhanced and ordered phase-aggregation in solution. This method leads to a notable improvement and a redshifted absorption of the acceptor phase during film formation, along with improved crystallinity. Moreover, the PDCI-induced preaggregation of NFAs in the solution enables ordered molecule packing during the film-formation process through delicate intermediate states transition. Consequently, the PDCI-induced preaggregated significantly improves the PCE of PM6:Y6 OSCs from 16.12% to 18.12%, among the best values reported for PM6:Y6 OSCs. Importantly, this approach is universally applicable to other Y-series NFA-based OSCs, achieving a champion PCE of 19.02% for the PM6:BTP-eC9 system. Thus, the preaggregation control strategy further unlocks the potential of Y-series NFAs, offering a promising avenue for enhancing the photovoltaic performance of Y-series NFA-based OSCs.

Designing a Novel Wide Bandgap Small Molecule Guest for Enhanced Stability and Morphology Mediation in Ternary Organic Solar Cells with over 19.3% Efficiency.

In this study, a novel wide-bandgap small molecule guest material, ITOA, designed and synthesized for fabricating efficient ternary organic solar cells (OSCs) ITOA complements the absorbance of the PM6:Y6 binary system, exhibiting strong crystallinity and modest miscibility. ITOA optimizes the morphology by promoting intensive molecular packing, reducing domain size, and establishing a preferred vertical phase distribution. These features contribute to improved and well-balanced charge transport, suppressed carrier recombination, and efficient exciton dissociation. Consequently, a significantly enhanced efficiency of 18.62% for the ternary device is achieved, accompanied by increased short-circuit current density (JSC), fill factor (FF), and open-circuit voltage (VOC). Building on this success, replacing Y6 with BTP-eC9 leads to an outstanding PCE of 19.33% for the ternary OSCs. Notably, the introduction of ITOA expedites the formation of the optimized morphology, resulting in an impressive PCE of 18.04% for the ternary device without any postprocessing. Moreover, the ternary device exhibits enhanced operational stability under maximum power point (MPP) tracking. This comprehensive study demonstrates that a rationally designed guest molecule can optimize morphology, reduce energy loss, and streamline the fabrication process, essential for achieving high efficiency and stability in OSCs, paving the way for practical commercial applications.

Rational molecular and device design enables organic solar cells approaching 20% efficiency.

For organic solar cells to be competitive, the light-absorbing molecules should simultaneously satisfy multiple key requirements, including weak-absorption charge transfer state, high dielectric constant, suitable surface energy, proper crystallinity, etc. However, the systematic design rule in molecules to achieve the abovementioned goals is rarely studied. In this work, guided by theoretical calculation, we present a rational design of non-fullerene acceptor o-BTP-eC9, with distinct photoelectric properties compared to benchmark BTP-eC9. o-BTP-eC9 based device has uplifted charge transfer state, therefore significantly reducing the energy loss by 41 meV and showing excellent power conversion efficiency of 18.7%. Moreover, the new guest acceptor o-BTP-eC9 has excellent miscibility, crystallinity, and energy level compatibility with BTP-eC9, which enables an efficiency of 19.9% (19.5% certified) in PM6:BTP-C9:o-BTP-eC9 based ternary system with enhanced operational stability.

19.31% binary organic solar cell and low non-radiative recombination enabled by non-monotonic intermediate state transition.

Non-fullerene acceptors based organic solar cells represent the frontier of the field, owing to both the materials and morphology manipulation innovations. Non-radiative recombination loss suppression and performance boosting are in the center of organic solar cell research. Here, we developed a non-monotonic intermediate state manipulation strategy for state-of-the-art organic solar cells by employing 1,3,5-trichlorobenzene as crystallization regulator, which optimizes the film crystallization process, regulates the self-organization of bulk-heterojunction in a non-monotonic manner, i.e., first enhancing and then relaxing the molecular aggregation. As a result, the excessive aggregation of non-fullerene acceptors is avoided and we have achieved efficient organic solar cells with reduced non-radiative recombination loss. In PM6:BTP-eC9 organic solar cell, our strategy successfully offers a record binary organic solar cell efficiency of 19.31% (18.93% certified) with very low non-radiative recombination loss of 0.190 eV. And lower non-radiative recombination loss of 0.168 eV is further achieved in PM1:BTP-eC9 organic solar cell (19.10% efficiency), giving great promise to future organic solar cell research.

Artificial Intelligence Designer for Highly-Efficient Organic Photovoltaic Materials.

Designing efficient organic photovoltaic (OPV) materials purposefully is still challenging and time-consuming. It is of paramount importance in material development to identify basic functional units that play the key roles in material performance and subsequently establish the substructure-property relationship. Herein, we describe an automatic design framework based on an in-house designed La FREMD Fingerprint and machine learning (ML) algorithms for highly efficient OPV donor molecules. The key building blocks are identified, and a library consisting of 18 960 new molecules is generated within this framework. Through investigating the chemical structures of materials with different performance, a guidance on designing efficient OPV materials is proposed. Furthermore, the most promising candidates exhibit a predicted power conversion efficiency (PCE) value of over 15% when combined with acceptor Y6. Density functional theory (DFT) studies show these candidate materials possess exceptional potential for efficient charge carrier transport. The proposed framework demonstrates the ability to design new materials based on the substructure-property relationship built by ML, which provides an alternative methodology for applying ML in new material discovery.

15.3% Efficiency All-Small-Molecule Organic Solar Cells Achieved by a Locally Asymmetric F, Cl Disubstitution Strategy.

Single junction binary all-small-molecule (ASM) organic solar cells (OSCs) with power conversion efficiency (PCE) beyond 14% are achieved by using non-fullerene acceptor Y6 as the electron acceptor, but still lag behind that of polymer OSCs. Herein, an asymmetric Y6-like acceptor, BTP-FCl-FCl, is designed and synthesized to match the recently reported high performance small molecule donor BTR-Cl, and a record efficiency of 15.3% for single-junction binary ASM OSCs is achieved. BTP-FCl-FCl features a F,Cl disubstitution on the same end group affording locally asymmetric structures, and so has a lower total dipole moment, larger average electronic static potential, and lower distribution disorder than those of the globally asymmetric isomer BTP-2F-2Cl, resulting in improved charge generation and extraction. In addition, BTP-FCl-FCl based active layer presents more favorable domain size and finer phase separation contributing to the faster charge extraction, longer charge carrier lifetime, and much lower recombination rate. Therefore, compared with BTP-2F-2Cl, BTP-FCl-FCl based devices provide better performance with FF enhanced from 71.41% to 75.36% and J sc increased from 22.35 to 24.58 mA cm-2, leading to a higher PCE of 15.3%. The locally asymmetric F, Cl disubstitution on the same end group is a new strategy to achieve high performance ASM OSCs.

Molecular Lock Induced by Chloroplatinic Acid Doping of PEDOT:PSS for High-Performance Organic Photovoltaics.

In organic photovoltaics (OPVs), the mechanical contact between charge transport layers and photoactive layer can influence the electrical contact that facilitates carrier collection. Unfortunately, the mechanical contact at the interface is rarely discussed in the OPV context. Herein, we report a distinct molecular locking effect that occurs between the donor molecules in the photoactive layer and the hole transport layer (HTL). This is achieved by doping chloroplatinic acid into poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate). The "molecular lock" at the interface leads to denser distribution and more ordered assembling of PM6 donor molecules close to the HTL. Consequently, the trap-assisted recombination in the cell is greatly suppressed, and the carrier lifetime is prolonged by more than 2 times. Together with the elevated charge carrier collection probability, a high fill factor of 77% and a power conversion efficiency of 16.5% are achieved in the PM6:Y6-based OPVs. This study provides a feasible way to boost the device performance by reinforcing the interfacial interaction between the HTL and photoactive layer.

An asymmetric end-capping strategy enables a new non-fullerene acceptor for organic solar cells with efficiency over 10.

Two different terminal groups, rhodanine-flanked benzo[c][1,2,5]thiadiazole (BR) and 2-(5,6-difluoro-3-oxo-2,3-dihydro-1H-inden-1-ylidene)malononitrile (IM2F), were connected to an indaceno[1,2-b:5,6-b']dithiophene (IDT) core to construct a new non-fullerene acceptor (IDTBF). Solar cells based on this acceptor exhibited promising photovoltaic performances with a power conversion efficiency (PCE) of up to 10.43%.

A "σ-Hole"-Containing Volatile Solid Additive Enabling 16.5% Efficiency Organic Solar Cells.

Here we introduce a σ-hole-containing volatile solid additive, 1, 4-diiodotetrafluorobenzene (A3), in PM6:Y6-based OSCs. Aside from the appropriate volatility of A3 additive, the synergetic halogen interactions between A3 and photoactive matrix contribute to more condensed and ordered molecular arrangement in the favorable interpenetrating donor/acceptor domains. As a result, greatly accelerated charge transport process with suppressed charge recombination possibility is observed and ultimately a champion PCE value of 16.5% is achieved. Notably, the A3 treated OSCs can maintain a high efficiency of over 16.0% in a wide concentration range of A3 additive between 10 and 35 mg/mL. The A3-treated device shows excellent stability with an efficiency of 15.9% after 360-h storage. This work demonstrates that the σ-hole interaction can be applied to enhance the OSC performance and highlights the importance of non-covalent interactions in the optoelectronic materials.

Simple near-Infrared Nonfullerene Acceptors Enable Organic Solar Cells with >9% Efficiency.

Nonfullerene acceptors (NFAs) based on calamitic-shaped small molecules are being developed rapidly to improve the photoelectron conversion efficiencies (PCEs) of organic solar cells. NFAs with light absorption extended to the near-infrared (NIR) region are of interest because they play a pivotal role in both organic tandem cells and semitransparent devices. In this work, two simple acceptor-donor-acceptor-structured NFAs (CPDT-4Cl and CPDT-4F) have been designed and synthesized. Featured with dimerized 4H-cyclopenta[1,2-b:5,4-b']dithiophene (CPDT) as the electron-donating core and Cl- or F-substituted 2-(3-oxo-2,3-dihydro-1H-inden-1-ylidene)malononitrile as the electron-accepting unit, the absorption spectra of two NFAs are extended to the NIR region with an absorption edge at approximately 910 nm. In conjunction with the polymer donor material PBDB-T, a PCE of 9.47% was achieved by using a CPDT-4F-based device with a short-circuit current density of up to 20.1 mA/cm2, which slightly outperforms its counterpart CPDT-4Cl (PCE = 9.28%) under the same condition. This work broadens the scope of developing new NIR NFAs with both high efficiency and easy accessibility.

Impact of ZnO Photoluminescence on Organic Photovoltaic Performance.

ZnO is a widely used electron transport material in third generation solar cells. Intrinsic defects arising from different synthetic methods and conditions lead to different fluorescent colors. The defect mechanisms have been explored in the literature, but their impact on organic photovoltaic (OPV) cell performance is rarely reported. Herein, three different ZnO nanoparticles showing blue, green, and yellow emission colors are synthesized and incorporated into OPV cells. The as-cast ZnO films result in vastly different OPV performances. It is found the sodium acetate as the byproduct of the synthesis can significantly influence the interfacial contact. After removing the impurity via rinsing with polar organic solvents, the different ZnO nanoparticles can deliver similar power conversion efficiencies (PCEs) in three representative OPV systems. The PCEs reached 4, 8, and 10% in P3HT:PC61BM-, PTB7-Th:PC71BM-, and PBDB-T-SF:IT-4F-based OPV cells, respectively. A series of characterizations indicate that the intrinsic defect types do not affect the optical and electrical properties of the ZnO film, including photon transmittance, electrical conductivity, and charge extraction from the active layer as well as electron mobility. The results together suggest that the intrinsic defect in ZnO nanoparticles has little impact on OPV performance. Thus, it might be necessary to revisit the strategies for defect engineering or passivation in oxide-based interfacial materials.

Inverted Planar Perovskite Solar Cells with a High Fill Factor and Negligible Hysteresis by the Dual Effect of NaCl-Doped PEDOT:PSS.

The performance of inverted perovskite solar cells is highly dependent on hole extraction and surface properties of hole transport layers. To highlight the important role of hole transport layers, a facile and simple method is developed by adding sodium chloride (NaCl) into poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS). The average power conversion efficiency of the perovskite solar cells prepared on NaCl-doped PEDOT:PSS is 17.1% with negligible hysteresis, compared favorably to the control devices (15.1%). Particularly, they exhibit markedly improved Voc and fill factor (FF), with the best FF as high as 81.9%. The enhancement of photovoltaic performance is ascribed to two effects. Better conductivity and hole extraction of PEDOT:PSS are observed after NaCl doping. More intriguingly, the perovskite polycrystalline film shows a preferred orientation along the (001) direction on NaCl-doped PEDOT:PSS, leading to a more uniform thin film. The comparison of the crystal structure between NaCl and MAPbCl3 indicates a lattice constant mismatch less than 2% and a matched chlorine atom arrangement on the (001) surface, which implies that the NaCl crystallites on the top surface of PEDOT:PSS might serve as seeds guiding the growth of perovskite crystals. This simple method is fully compatible with printing technologies to mass-produce perovskite solar cells with high efficiency and tunable crystal orientations.