High-performance alloy-like ternary organic solar cells with two compatible non-fullerene acceptors

Ternary blending is one of the effective strategies to modulate the blend film morphology for achieving high efficiency organic solar cells (OSCs). In this work, high-performance ternary OSCs are fabricated by introducing a non-fullerene acceptor, namely IDTP-4F into the PM6:Y6 binary system to enhance the device performance. Detailed investigations indicate that IDTP-4F can form an alloy phase with Y6, resulting in the optimized morphology, which can facilitate the charge transport and reduce recombination, leading to enhanced open-circuit voltage (V_oc) and fill factor (FF) simultaneously. Consequently, the optimized ternary OSCs exhibit an excellent power conversion efficiency (PCE) of 17.1%, which is much higher than that of PM6:Y6 binary OSCs (15.9%). These results indicate that combining two compatible non-fullerene acceptors is an effective strategy to fabricate high efficiency ternary OSCs.     

Ternary organic solar cells with improved efficiency and stability enabled by compatible dual-acceptor strategy

To further elevate the power conversion efficiency (PCE) of organic solar cells (OSCs), ternary strategy is one of the most efficient methods via simply incorporating a suitable third component. Here, a nonfullerene small molecule acceptor MOITIC was incorporated into the state-of-art PM6:Y6 binary system to further enhance the photovoltaic performance. Detailed investigation revealed that MOITIC exhibited a good miscibility and compatibility with Y6, forming alloy-like acceptors in the ternary blends. The alloy-like phase promoted the phase separation and optimized the morphology of ternary blend, which afforded higher and more balanced carrier mobility and reduced charge recombination in devices. Moreover, the larger energy offset between PM6 and MOITIC:Y6 acceptor alloy is beneficial to enhance open-circuit voltage (V_oc) of corresponding devices. As a consequence, the optimized ternary OSC (PM6:Y6:MOITIC = 1:1:0.1) showed a significantly increased PCE of 17.1% with simultaneously enhanced V_oc of 0.882 V, short-circuit current density (J_sc) of 25.6 mA cm⁻², and fill factor (FF) of 75.7%, which has about 9% enhancement compared to the control binary PM6:Y6 (15.7%). In addition, the optimized ternary device exhibited better stability. This work indicates that ternary strategy via combining two compatible small molecule acceptors is effective to simultaneously improve the efficiency and stability of OSCs.     

Rational Mutual Interactions in Ternary Systems Enable High-Performance Organic Solar Cells

Ternary organic solar cells (TOSCs) offer a facile and efficient approach to increase the power conversion efficiencies (PCEs). However, the critical roles that guest components play in complicated ternary systems remain poorly understood. Herein, two acceptors named LA1 and LA9 with differing crystallinity are investigated. The overly crystalline LA9 induces large self-aggregates in PM6:LA9 binary system, resulting in a lower PCE (13.12%) compared to PM6:LA1 device (13.89%). Encouragingly, both acceptors are verified as efficient guest candidates into the host binary PM6:NCBDT-4Cl (PCE = 13.48%) and afford markedly improved PCEs up to 15.39% and 15.75% in LA1 and LA9 ternary devices, respectively. Interestingly, the higher crystallinity LA9 reveals smaller interaction energies with both the host acceptor and donor PM6. Compared to LA1, the appropriate mutual interactions in the LA9 ternary system not only induces the orderly crystallinity of PM6 but also better compatibility with the host acceptor, generating further optimized molecular orientations and ternary morphology. Therefore, enhanced charge transport and minimized recombination loss are detected in LA9 ternary devices, affording the most competitive performance among Y6-sbsent TOSCs. This work suggests that complicated intermolecular interactions should be seriously considered when fabricating state-of-the-art multiple components OSCs.     

Suppressing Kinetic Aggregation of Non-Fullerene Acceptor via Versatile Alloy States Enables High-Efficiency and Stable Ternary Polymer Solar Cells

Despite considerable advances devoted to improving the operational stability of organic solar cells (OSCs), the metastable morphology degradation remains a challenging obstacle for their practical application. Herein, the stabilizing function of the alloy states in the photoactive layer from the perspective of controlling the aggregation characteristics of non-fullerene acceptors (NFAs), is revealed. The alloy-like model is adopted separately into host donor and acceptor materials of the state-of-the-art binary PM6:BTP-4Cl blend with the self-stable polymer acceptor PDI-2T and small molecule donor DRCN5T as the third components, delivering the simultaneously enhanced photovoltaic efficiency and storage stability. In such ternary systems, two separate arguments can rationalize their operating principles: (1) the acceptor alloys strengthen the conformational rigidity of BTP-4Cl molecules to restrain the intramolecular vibrations for rapid relaxation of high-energy excited states to stabilize BTP-4Cl acceptor. (2) The donor alloys optimize the fibril network microstructure of PM6 polymer to restrict the kinetic diffusion and aggregation of BTP-4Cl molecules. According to the superior morphological stability, non-radiative defect trapping coefficients can be drastically reduced without forming the long-lived, trapped charge species in ternary blends. The results highlight the novel protective mechanisms of engineering the alloy-like composites for reinforcing the long-term stability of NFA-based ternary OSCs.     

19.28% Efficiency and Stable Polymer Solar Cells Enabled by Introducing an NIR-Absorbing Guest Acceptor

Here, a near-infrared (NIR)-absorbing small-molecule acceptor (SMA) Y-SeNF with strong intermolecular interaction and crystallinity is developed by combining selenophene-fused core with naphthalene-containing end-group, and then as a custom-tailor guest acceptor is incorporated into the binary PM6:L8-BO host system. Y-SeNF shows a 65 nm red-shifted absorption compared to L8-BO. Thanks to the strong crystallinity and intermolecular interaction of Y-SeNF, the morphology of PM6:L8-BO:Y-SeNF can be precisely regulated by introducing Y-SeNF, achieving improved charge-transporting and suppressed non-radiative energy loss. Consequently, ternary polymer solar cells (PSCs) offer an impressive device efficiency of 19.28% with both high photovoltage (0.873 V) and photocurrent (27.88 mA cm⁻²), which is one of the highest efficiencies in reported single-junction PSCs. Notably, ternary PSC has excellent stability under maximum-power-point tracking for even over 200 h, which is better than its parental binary devices. The study provides a novel strategy to construct NIR-absorbing SMA for efficient and stable PSCs toward practical applications.     

Real-Time Probing and Unraveling the Morphology Formation of Blade-Coated Ternary Nonfullerene Organic Photovoltaics with In Situ X-Ray Scattering

Characterizing the bulk heterojunction (BHJ) morphology of the active layer is essential for optimizing blade-coated organic solar cells (OSCs). Here, the morphology evolution of a highly efficient ternary polymer:nonfullerene blend PM6:N3:N2200 under different blade coating conditions is probed in real-time by in situ synchrotron X-ray scattering and in situ ultraviolet-visible (UV-vis) spectroscopy. Besides, the morphology of blade-coated blend films at different conditions is detailed by ex situ X-ray scattering and microscopic imaging. The ternary blend film exhibited optimized morphology, such as superior molecular stacking structure and appropriate phase separation structure, and boosted photovoltaic performance of the binary blend, as adding a second polymer component to the host polymer:nonfullerene system can balance nucleation and crystallization of polymers and small molecules, facilitating molecular rearrangement to perfect crystallization. Both binary and ternary blends obtained optimized morphology and photovoltaic properties at medium coating speed, mainly attributed to the movement of the polymer and small molecules at the long crystallization and aggregation stage. These findings help understand morphology formation under film drying and provide guidance for optimizing the morphology in blade-coated OSCs.     

High-Efficiency Organic Solar Cells Based on a Low-Cost Fully Non-Fused Electron Acceptor

A series of tetrathiophene-based fully non-fused ring acceptors (4T-1, 4T-2, 4T-3, and 4T-4), which can be paired with the star donor polymer PBDB-T to fabricate highly efficient organic solar cells are developed. Tailoring the size of lateral chains can tune the solubility and packing mode of acceptor molecules in neat and blend films. It is found that the incorporation of 2-ethylhexyl chains can effectively change the compatibility with the donor polymer PBDB-T, and an encouraging power conversion efficiency of 10.15% is accomplished by 4T-3-based organic solar cells. It also presents good compatibility with the other polymer donor and an even higher power conversion efficiency (PCE) of 12.04% is achieved based on D18:4T-3 blend, which is the champion PCE for the fully non-fused acceptors. Importantly, these inexpensive tetrathiophene fully non-fused ring acceptors provide cost-effective photovoltaic performance. The results demonstrate a high photovoltaic performance from synthetically inexpensive materials could be achieved by the rational design of non-fused ring acceptor molecules.     

Anthracene-Assisted Morphology Optimization in Photoactive Layer for High-Efficiency Polymer Solar Cells

Currently, morphology optimization methods for the fused-ring nonfullerene acceptor-based polymer solar cells (PSCs) empirically follow the treatments originally developed in fullerene-based systems, being unable to meet the diverse molecular structures and strong crystallinity of the nonfullerene acceptors. Herein, a new and universal morphology controlling method is developed by applying volatilizable anthracene as solid additive. The strong crystallinity of anthracene offers the possibility to restrict the over aggregation of fused-ring nonfullerene acceptor in the process of film formation. During the kinetic process of anthracene removal in the blend under thermal annealing, donor can imbed into the remaining space of anthracene in the acceptor matrix to form well-developed nanoscale phase separation with bi-continuous interpenetrating networks. Consequently, the treatment of anthracene additive enables the power conversion efficiency (PCE) of PM6:Y6-based devices to 17.02%, which is a significant improvement with regard to the PCE of 15.60% for the reference device using conventional treatments. Moreover, this morphology controlling method exhibits general application in various active layer systems to achieve better photovoltaic performance. Particularly, a remarkable PCE of 17.51% is achieved in the ternary PTQ10:Y6:PC₇₁BM-based PSCs processed by anthracene additive. The morphology optimization strategy established in this work can offer unprecedented opportunities to build state-of-the-art PSCs.     

Enhancing the photovoltaic performance with two similar structure polymers as donors by broadening the absorption spectrum and optimizing the molecular arrangement

Ternary organic photovoltaics (OPVs) were fabricated with two polymers (PM6 and D18) as the donor and the fullerene-free small molecule Y6 as the acceptor in an inverted structure. The blueshifted absorption spectrum of neat D18 relative to neat PM6 can enable harvesting of more short and medium wavelength photons in the ternary photoactive layer, which is beneficial to increasing the short-circuit current density (J_SC). The enhancement of the open-circuit voltage (V_OC) of the ternary OPVs can be explained by the deeper HOMO level of D18 than that of PM6, which is beneficial to broadening the energy bandgap. In addition, the combination of the cascade LUMO levels among D18, PM6 and Y6 and the enhanced crystallinity can lead to more efficient exciton dissociation and charge transport within the ternary films. As a result, the power conversion efficiency of the optimize ternary OPV is 15.85%, which is higher than those of the PM6:Y6- and D18:Y6-base binary OPVs (PCEs of 14.70% and 14.95%, respectively). The results indicate that ternary OPVs with a blend of two similar chemical structure polymers as the donor could achieve high performance by broadening the light spectrum and optimizing the phase separation and crystallinity.     

Alkoxy- and Alkyl-Side-Chain-Functionalized Terpolymer Acceptors for All-Polymer Photovoltaics Delivering High Open-Circuit Voltages and Efficiencies

A new terpolymer acceptor is presented, comprising various ratios of the same dithienothienopyrrolobenzothiadiazole (BTP) core with different side chains—alkoxy side chains (BTPO-IC) and alkyl side chains (BTP-IC)—and thiophene units, for use in all-polymer organic photovoltaics. Devices incorporating binary blends of this terpolymer and the polymer PM6 as the active layer displayed open-circuit voltages (V_OC) that increase linearly upon increasing the molar ratio of BTPO-IC. For example, the optimized device incorporating PM6:PY-0.2OBO (i.e., with 20 mol% of BTPO-IC) (1:1.2 wt.%) blend, with the smallest domain sizes but largest coherence length and combined face-on and edge-on orientation fractions among all blends, have a champion power conversion efficiency (PCE) of 16.7% (V_OC = 0.97 V; J_SC = 25.2 mA cm⁻²; FF = 0.68), whereas the device containing a similar blend ratio of the PM6:PY-OD:PY-OBO ternary blend (1:0.96:0.24 wt.%) displayed a PCE of 8.6% (V_OC = 0.969 V; J_SC = 18.7 mA cm⁻²; FF = 0.48). The device with PM6:PY-0.2OBO displays better thermal stability than the devices with PM6: PY-OD or PY-OBO. Thus, employing terpolymer acceptors with differently functionalized side-chain units can be an effective approach for simultaneously optimizing the aggregation domain and enhancing the PCEs and thermal stabilities of all-polymer devices.     

Realizing an Unprecedented Fill Factor of 82.2% in Ternary Organic Solar Cells via Co-Crystallization of Non-Fullerene Acceptors

Ternary strategy is demonstrated as an efficient approach to achieve high short-circuit current and open-circuit voltage to boost the performance of organic solar cells (OSCs), however, the realization of high fill-factor (FF) in ternary OSCs has been rare. In this study, three thiophene terminated non-fullerene acceptors (NFAs) with methyl or chlorine substitutions on their end-groups are designed and synthesized, and further incorporated into the state-of-the-art PM6:L8-BO system to construct ternary OSCs. Subtle changes in their chemical structures significantly modify the molecular packings of these thiophene terminated NFAs. While BTP-ThMe and BTP-ThCl have limited forms of dimer, versatile molecular dimers, including “Z” shaped D-D, “S” shaped A-A, and “F” shaped A-D packings exist in BTP-ThMeCl, which lead to the formation of compact 3D honey-comb network and this is analogous to the host acceptor L8-BO. This synergetic molecular packing between BTP-ThMeCl and L8-BO contributes to maintain the 3D charge transport network in the ternary system via the formation of NFA co-crystals at the molecular level, and consequently realizing a maximum power conversion efficiency of 19.1% with a superior FF of 82.2%, which is the highest FF reported so far for OSCs.     

18.9% Efficiency Ternary Organic Solar Cells Enabled by Isomerization Engineering of Chlorine-Substitution on Small Molecule Donors

Ternary organic solar cells (OSCs) represent an efficient and facile strategy to further boost the device performance. However, the selection criteria and rational design of the third guest small molecule (SM) material still remain less understood. In this study, two new SM donor isomers, with α-chlorinated thiophene (αBTCl) and β-chlorinated thiophene (βBTCl) as side chains, are systematically designed, synthesized and incorporated as a third component in PM6:L8-BO binary blends. It is noticed that introducing the SM donors guest has extended the absorption of photo-active layer, induced desired component distribution vertically with enhanced crystallinity and reduced recombination process, leading to increased short-circuit current (J_SC) and improved fill factor. Moreover, due to the synergetic suppressed nonradiative loss and preferable morphology, the ternary OSCs feature improves open-circuit voltage (V_OC). Consequently, an impressive champion power conversion efficiency of 18.96% and 18.55% is achieved by αBTCl-based and βBTCl-based ternary OSCs, respectively. Furthermore, a record efficiency of 17.46% is obtained with a 330 nm thickness of αBTCl-based ternary OSCs. This study demonstrates that molecular isomerization can be a promising design approach for SM donors to construct high-performance ternary OSCs with simultaneous enhancement of all photovoltaic parameters.     

Efficient ternary polymer solar cells by optimizing photogenerated exciton dissociation and photon harvesting with a short wavelength absorption polymer acceptor as the third component

Ternary blend films, obtained by introducing a third component (a second acceptor as the third component) to a binary polymer solar cell (PSC), are a promising ternary strategy because the light absorption range, surface morphology, and charge carrier transport of the photoactive layer may be optimized, as can the energy level alignment between the donor and the acceptor. In this work, acceptors such as the short-wavelength-absorption polymer N2200 and the long-wavelength-absorption small molecule FOIC were combined with the donor PBDB-T-2F to construct ternary blends. The optimized ternary PSC could achieve a power conversion efficiency (PCE) of 13.98%, which is higher than the efficiencies of binary PSCs based on PBDB-T-2F:FOIC (12.65%) and PBDB-T-2F:N2200 (9.36%). The enhanced PCE of the ternary PSC is based on the high electron mobility, balanced charge transport, optimized surface morphology and charge carrier kinetics and the extended light absorption of the ternary photoactive layer, realized by adjusting the ratio of FOIC:N2200. Our results indicate that mixing a polymer acceptor into a binary photoactive layer to form a ternary blend photoactive layer is a valuable strategy for improving photovoltaic performance.     

Air Processing of Thick and Semitransparent Laminated Polymer:Non-Fullerene Acceptor Blends Introduces Asymmetric Current–Voltage Characteristics

Non-fullerene acceptors have recently revolutionized indoor organic photovoltaics (OPVs) with power conversion efficiencies exceeding 30% in laboratory scale. Nevertheless, transferring their superior performance to larger-scale prototyping, i.e., air-processing via roll-to-roll compatible techniques, still shows severe challenges. Herein, the industrial potential of the PM6:IO4Cl blend, which is one of the most successful indoor OPV photoactive layers (PALs), is thoroughly investigated. The corresponding thick and semitransparent laminated devices are fabricated entirely in air, by blade and slot-die coating. Their current–voltage (J–V) characteristics show anomalous features depending on the illumination side, with the cathode side generally outperforming the anode counterpart. Electrical and optical modeling reveal that a plausible cause of such a phenomenon is a dead layer that forms at the PAL/anode contact interface that does not contribute to the photocurrent. Said layer becomes undetectable when the PALs are made thin enough (<35 nm each) leading to symmetric J–V curves and improved light utilization efficiency. By screening the photovoltaic performance of multiple donor:acceptor blends, certain all-polymer and polymer:fullerene PALs are identified as adequately symmetric candidates for thick device up-scaling. Finally, ternary blends based on PM6:IO4Cl:fullerene may constitute a viable route to mitigate the electrical asymmetry detected on conventional binary blends.     

Subtle Polymer Donor and Molecular Acceptor Design Enable Efficient Polymer Solar Cells with a Very Small Energy Loss

A new wide bandgap polymer donor, PNDT‐ST, based on naphtho[2,3‐b:6,7‐b′]dithiophene (NDT) and 1,3‐bis(thiophen‐2‐yl)‐5,7‐bis(2‐ ethylhexyl)benzo[1,2‐c:4,5‐c′]dithiophene‐4,8‐dione (BDD) is developed for efficient nonfullerene polymer solar cells. To better match the energy levels, a new near infrared small molecule of Y6‐T is also developed. The extended π‐conjugation and less twist of PNDT‐ST provides it with higher crystallinity and stronger aggregation than the PBDT‐ST counterpart. The higher lowest occupied molecular orbital level of Y6‐T than Y6 favors the better energy level match with these polymers, resulting in improved open circuit voltage (V_oc) and power conversion efficiency (PCE). The high crystallinity and strong aggregation of PNDT‐ST also induces large phase separation with poorer morphology, leading to lower fill factor and reduced PCE than PBDT‐ST. To mediate the crystallinity and optimize the morphology, PNDT‐ST and PBDT‐ST are blended together with Y6‐T, forming the ternary blend devices. As expected, the two compatible polymers allow continual optimization of the morphology by varying the blend ratio. The optimized ternary blend devices deliver a champion PCE as high as 16.57% with a very small energy loss (E_loss) of 0.521 eV. Such small E_loss is the best record for polymer solar cells with PCEs over 16% to date.     

Small-molecule acceptors with long alkyl chains for high-performance as-cast nonfullerene organic solar cells

Three fused-ring small-molecule electron acceptors, IDTC16-IC, IDTC16-Th, and IDTC16-4F, were designed and synthesized by introducing indacenodithiophene (IDT) as the electron-donating core and 2-(3-oxo-2,3-dihydro-1H-inden-1-ylidene)malononitrile (IC), fluorinated IC, and a thiophene-based unit as the electron-withdrawing end group. Here, instead of the commonly used n-hexyl or n-hexylphenyl side chains, n-hexadecyl peripheral substituents were employed at the IDT core to study the influence of alkyl groups on photovoltaic performance of the nonfullerene acceptors. The introduction of flexible n-hexadecyl group endowed the three acceptors with excellent solubility in common organic solvents. All the three acceptors presented strong absorption ranging from 450 nm to 720 nm in solution with high molar extinction coefficients. As a result, the as-cast organic solar cells (OSCs) based on IDTC16-IC and the wide bandgap polymer donor PM6 exhibited a power conversion efficiency (PCE) of 5.12%. The OSCs based on PM6:IDTC16-Th and PM6:IDTC16-4F showed much better photovoltaic performance with PCEs of 8.76% and 8.55%, respectively. The PCE values were improved to 5.89%, 9.09%, and 9.42% for the PM6:IDTC16-IC, PM6:IDTC16-Th, and PM6:IDTC16-4F OSCs, respectively, with the addition of the solvent additive 1,8-diiodooctane. These findings demonstrate that the combination of alkyl chains at the fused rings and fluorination or aromatic structure change of the terminal groups leads to greatly enhanced photovoltaic performance of nonfullerene acceptors through improving the photophysical, molecular orbital, and film morphological properties.     

Efficient PTB7-Th:Y6:PC71BM ternary organic solar cell with superior stability processed by chloroform

Blend morphology is crucial for the efficiency and stability of organic solar cells. Exploring and understanding the correlations between is meaningful and greatly desired. In this work, based on polymer donor (PTB7-Th), fullerene and non-fullerene acceptors (PC₇₁BM and Y6), we systematically study the influence of ternary strategy and solvent system on device performance and stability. It is found that insufficient and excessive phase separation of blend could result in the depressed performance of corresponding devices. Appropriate phase separation/blend morphology can be achieved by utilizing a ternary strategy or suitable solvent. Chloroform-processed ternary blend PTB7-Th:Y6:PC₇₁BM delivers efficiency of 9.55%, with dramatically enhanced J_SC of 24.68 mA cm⁻² due to optimized absorption, blend morphology and optoelectronic properties. More importantly, superior device stability is demonstrated for the optimal ternary device under both thermal stress and maximum power point operation, by maintaining 80% of initial efficiency at 85 °C for 880 h and presenting almost zero efficiency decay in 200 h under MPP operation.     

Asymmetric Isomer Effects in Benzo[c ][1,2,5]thiadiazole-Fused Nonacyclic Acceptors: Dielectric Constant and Molecular Crystallinity Control for Significant Photovoltaic Performance Enhancement

Herein, asymmetric isomer effects are systematically explored by designing and synthesizing two benzo[c][1,2,5]thiadiazole (BT)-fused nonacyclic electron acceptors. By changing from BP6T-4F to asymmetric ABP6T-4F, significantly enhanced dielectric constant and inhibited excessive molecular aggregation and unfavorable edge-on orientation could be achieved. The reduced exciton binding energy also facilitates a more efficient dissociation process in PM6:ABP6T-4F compared to PM6:BP6T-4F with the same energy offset. Moreover, the weaker crystallization behavior enables a significantly enhanced miscibility between PM6 and ABP6T-4F than that between PM6 and BP6T-4F, which leads to an optimized micromorphology with smooth surface, suitable domain size, and ordered π–π stacking. Organic solar cells (OSCs) based on PM6:ABP6T-4F achieve a 15.8% power conversion efficiency (PCE), which is remarkably higher than that of PM6:BP6T-4F-based OSCs (6.4%). Furthermore, ternary devices are also fabricated considering good compatibility between ABP6T-4F and CH1007 to deliver a PCE over 17%. This study reveals the effectiveness and great potential of asymmetric isomerization strategy in regulating molecular properties, which will provide guidance for the future design of non-fullerene acceptors.     

High-Performance Ternary Organic Solar Cells Enabled by Integrating a 3D-Shaped Guest Acceptor Derived from Perylene Diimide

Integrating a third component into the binary system is considered to be one of the most effective strategies to further enhance the power conversion efficiency (PCE) in organic solar cells (OSCs). Here, a novel perylene diimide (PDI) derivative featuring 3D structure, TPA-4PDI, with tetraphenyladamantane central core is developed as a guest electron acceptor to be incorporated into the PM6:Y6 binary system. The champion PCE of ternary OSC is recorded to be 18.29% by adding 7.5 wt.% of TPA-4PDI in the ternary blend, which photovoltaic performance is enhanced with synergistically increased open-circuit voltage (V_oc) of 0.849 V, short-circuit current density (J_sc) of 27.55 mA cm⁻², and fill factor (FF) of 78.21%. TPA-4PDI exhibits a complementary absorption band with PM6 and Y6 while its lowest unoccupied molecular orbital (LUMO) energy level falls between the two host materials. The addition of TPA-4PDI can effectively suppress the recombination behavior, inhibit the excessive aggregation of Y6 and improve the morphology of PM6:Y6 blend. All these effects function synergistically and then lead to the enhancement of V_oc, J_sc, and FF in ternary OSCs. This study suggests that developing PDI derivatives as the third component is an effective method to further improve the performance of ternary OSCs.     

High-Performance Green Thick-Film Ternary Organic Solar Cells Enabled by Crystallinity Regulation

The power conversion efficiency (PCE) of organic solar cells (OSCs) has reached high values of over 19%. However, most of the high-efficiency OSCs are fabricated by spin-coating with toxic solvents and the optimal photoactive layer thickness is limited to 100 nm, limiting practical development of OSCs. It is a great challenge to obtain ideal morphology for high-efficiency thick-film OSCs when using non-halogenated solvents due to the unfavorable film formation kinetics. Herein, high-efficiency ternary thick-film (300 nm) OSCs with PCE of 15.4% based on PM6:BTR-Cl:CH1007 are fabricated by hot slot-die coating using non-halogenated solvent (o-xylene) in the air. Compared to PM6:BTR-Cl:Y6 blends, the stronger pre-aggregation of CH1007 in solution induces the earlier aggregation of CH1007 molecules and longer aggregation time, and thus results in high and balanced crystallinity of donors and acceptor in CH1007-based ternary film, which led to high-carrier mobility and suppressed charge recombination. The ternary strategy is further used to fabricate high-efficiency, thick-film, large-area, and flexible devices processed from non-halogenated solvents, paving the way for industrial development of OSCs.