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Solution processability is one of the advantages of organic solar cells (OSCs). However, most high-efficiency OSCs are prepared using hazardous chlorinated solvents for the deposition of photoactive layers. The replacement of non-halogenated solvents with eco-friendly green solvents for photoactive materials is urgently required. Herein, we have developed a novel asymmetric T2-OEHRH, which is modified from the symmetric T2-ORH. The introduction of asymmetric alkyl side chains onto rhodanine end groups can effectively suppress excessive self-aggregation/crystallization and substantially improve solubility without sacrificing optoelectrical properties. Therefore, ternary-blend OSCs based on PTB7-Th:EH-IDTBR:T2-OEHRH processed using a non-halogenated solvent system exhibit a uniform and favorable morphology and give a high power conversion efficiency (PCE) of 12.10%. More importantly, we demonstrate an impressive PCE of 9.32% for large-area NFA-OSCs (substrate size = 100 cm2 and aperture size = 55.5 cm2) prepared via D-bar coating in air. To our knowledge, this PCE is the highest reported to date for NFA-based large-area OSC modules processed from a non-halogenated solvent. This asymmetric alkyl-chain engineering strategy can be exploited to develop high-performance large-area NFA-OSCs with eco-friendly solvent processing.

A simple-structured nonfullerene acceptor (NFA), T2-ORH, consisting of a bithiophene core and octyl-substituted rhodanine ends is utilized as the third component in ternary-blend solar cells with PTB7-Th and EH-IDTBr as host materials. T2-ORH is a wide band gap NFA and specially contributes to light absorption, which provides complimentary absorption with a low band gap acceptor, EH-IDTBR. In the ternary device, a PCE of 11.55%, a short circuit current (JSC) of 17.51 mA cm−2, a fill factor (FF) of 63% and an open circuit voltage (VOC) of 1.05 V were achieved with a 1 : 1 : 1 blend ratio. In this ternary system, it is estimated that the two NFAs work as one alloy-like acceptor and energy transfer model from T2-ORH to EH-IDTBR for efficient ternary-blend organic solar cells (OSCs). On conducting thermal, light, and air-process stability tests, the ternary-blend systems show superior stability performance owing to the formation of a stable and robust morphology. Finally, we fabricated a large-scale device (5 cm × 5 cm substrate, 13.5 cm2 aperture size, and a geometric FF of 54%) with the same ternary system. The sub-module ternary-blend OSCs displayed the highest PCE of 10.08% with JSC = 2.83 mA cm−2, VOC = 6.36 V and FF = 56%. As a result, ternary-blend OSCs show tremendous promise for use in actual applications.

A novel series of benzodithiophene-4,8-dione (BDD)-based copolymers, poly[(4,4,9,9-tetrakis(4-hexylphenyl)-4,9-dihydro-s-indacenodithiophene-2,7-diyl)-alt-(1,3-bis(2-ethylhexyl)-5,7-di(thiophene2-yl)benzodithiophene-4,8-dione)] (P1) and poly[(5,5,11,11-tetrakis(4-hexylphenyl)dithieno[2,3-d: 2',3'-d']-s-indacenodithiophene-3,9-diyl)-alt-(1,3-bis(2-ethylhexyl)-5,7-di(thiophene-2-yl)benzodithiophene-4,8-dione)] (P2), which have the same acceptor moiety but different donor segments, have been designed and synthesized for use as donor materials in solution-processable polymer solar cells (PSCs). The optical and photovoltaic properties of the copolymers were investigated. The band gaps of the copolymers were in the range 1.91-1.92 eV. Under optimized conditions, the BDD-based polymers showed power conversion efficiencies (PCEs) for the PSCs in the range 2.52-2.92% under AM 1.5 illumination (100 mW/cm2). Among the copolymers, P1, which contained an indacenodithiophene donor unit, showed a power conversion efficiency of 2.92% with a short circuit current of 7.30 mA/cm2, open circuit voltage of 0.92 V, and a fill factor of 0.43, under AM 1.5 illumination (100 mW/cm2).

A newly synthesized small molecule donor, BDTT-2DPPBFu, is designed for incorporation into the photo-active layer in solution-processed small molecule organic photovoltaics (SM-OPVs). The effects of a solvent additive (1-chloronaphthalene, CN) on the bulk heterojunction morphology of a BDTT-2DPPBFu donor:fullerene derivative acceptor (PC71BM) are investigated and correlated with the device performance. A TEM analysis revealed that the nanomorphology of the SM-OPVs evolved dramatically with increasing solvent additive volume. With an optimum concentration of 2.5 vol% CN, a nanomorphology with a fibrillar and interpenetrating network on the order of exciton diffusion length (∼10–15 nm) is formed, resulting in improvement of the short-circuit current density, fill factor, and power conversion efficiency. Further GIWAXS studies have shown that the π–π stacking distance of BDTT-2DPPBFu small molecules is reduced and the inter-mixing of PC71BM within the BDTT-2DPPBFu-rich phase in the photo-active layer processed from 2.5 vol% CN is increased, leading to enhanced charge transport and reduced charge recombination and transfer resistance. The present work provides important progress in the nanomorphology of the photo-active layer, which can be effectively tuned via the use of a solvent additive in SM-OPVs.

We performed systematic experiments based on a small molecule donor and a polymer acceptor containing a naphthalene diimide (NDI)-based polymer as compared with fullerene-based acceptor (PC71BM) solar cells. Among polymer acceptors, the NDI-based polymer (PNDI-2T) shows good properties such as broad light absorbance with a strong absorption co-efficient and a well oriented crystalline structure leading to high electron mobility. We monitored the photovoltaic properties of both PNDI-2T and PC71BM acceptors with a BDT2TR donor. Although the BDT2TR:PC71BM device showed a higher PCE of 8.20%, the BDT2TR:PNDI-2T device also showed remarkable photovoltaic results with a PCE of 4.43%, VOC of 0.86 V, JSC of 7.26 mA cm−2, and FF of 71% indicating one of the highest efficiencies for small molecule donor and non-fullerene polymer acceptor systems. In particular, the PNDI-2T acceptor showed excellent thermal stability and intrinsic mechanical performance as compared with the PC71BM acceptor. To demonstrate the potential of the polymer acceptor for solar devices, we fabricated a device for testing thermal stability, high thickness tolerance, and the flexibility of the solar cell with bending stress. As a result, the PNDI-2T-based solar cell exhibited excellent thermal stability at 150 °C for 15 h and the PCE of the BDT2TR:PNDI-2T device with a thick active layer (around 610 nm) maintained 80% of its initial value. Moreover, the flexible device with the BDT2TR:PNDI-2T system retained its homogeneous morphology and showed maintained photovoltaic performance even after 100 bending cycles. Therefore, PNDI-2T based organic solar cells have good potential for application as flexible and portable real energy generators.

Most non-fullerene acceptors (NFAs) are designed in a complex planar molecular conformation containing fused aromatic rings in high-efficiency organic solar cells (OSCs). To obtain the final molecules, however, numerous synthetic steps are necessary. In this work, a novel simple-structured NFA containing alkoxy-substituted benzothiadiazole and a rhodanine end group (BTDT2R) is designed and synthesized. We also investigate the photovoltaic properties of BTDT2R-based OSCs employing representative polymer donors (wide band gap and high-crystalline P3HT, medium band gap and semicrystalline PPDT2FBT, and narrow band gap and low-crystalline PTB7-Th) to compare the performance capabilities of fullerene acceptor-based OSCs, which are well matched with various polymer donors. OSCs based on P3HT:BTDT2R, PPDT2FBT:BTDT2R, and PTB7-Th:BTDT2R achieved efficiency as high as 5.09, 6.90, and 8.19%, respectively. Importantly, photoactive films incorporating different forms of optical and molecular ordering characteristics exhibit favorable morphologies by means of solvent vapor annealing. This work suggests that the new n-type organic semiconductor developed here is highly promising as a universal NFA that can be paired with various polymer donors with different optical and crystalline properties.

A non-fullerene small molecule acceptor, SF-HR composed of 3D-shaped spirobifluorene and hexyl rhodanine, was synthesized for use in bulk heterojunction organic solar cells (OSCs). It possesses harmonious molecular aggregation between the donor and acceptor, due to the interesting diagonal molecular shape of SF-HR. Furthermore, the energy level of SF-HR matches well with that of the donor polymer, poly(3-hexyl thiophene) (P3HT) in this system which can affect efficient charge transfer and transport properties. As a result, OSCs made from a P3HT:SF-HR photoactive layer exhibited a power conversion efficiency rate of 4.01% with a high VOC of 1.00 V, a JSC value of 8.23 mA cm−2, and a FF value of 49%. Moreover, the P3HT:SF-HR film showed superior thermal and photo-stability to P3HT:PC71BM. These results indicate that SF-HR is specialized as a non-fullerene acceptor for use in high-performance OSCs.

We studied fullerene-free organic solar cells based on electron-donating (BDT3TR) and -accepting (O-IDTBR) small molecules. Bulk heterojunction devices comprising BDT3TR:O-IDTBR showed an excellent power conversion efficiency exceeding 7% and much better thermal stability than BDT3TR:PC70BM devices after ageing at 120 °C for 300 hours.

The molecular self-organization of organic semiconductors, which is mainly determined by the structural design, film processing, and device configuration, is one of the crucial factors for achieving high-performance organic photovoltaics (OPVs) and perovskite solar cells (PvSCs). In this study, we newly synthesized and developed strongly self-organized small molecules via alkyl side-chain engineering. Replacing “H” to “C6H13” on the thienyl group, SM2 showed a well-ordered face-on orientation. Due to favorable self-organization leading to effective charge carrier dynamics, including enhanced charge transfer/transport and suppressed recombination, SM2-based OPVs and PvSCs exhibited improved device performance compared to the devices based on SM1 without an additional hexyl side-chain. The best fullerene-based OPV and planar PvSC with SM2 as a small-molecule donor and as a hole transport layer (HTL) achieved an unprecedentedly high efficiency of 9.38% and 20.56%, in contrast with SM1-based devices showing lower efficiency of 8.70% and 15.37%. Furthermore, the planar PvSCs based on undoped-SM2 HTL exhibited comparable efficiency but provided excellent heat and humidity stability compared with doped spiro-OMeTAD-based devices. These results clearly indicated that SM2 with highly-ordered and favorable self-organization is a promising organic semiconductor for future applications of high-performance organic and inorganic-organic hybrid electronics.

A series of four donor-acceptor alternating copolymers based on dialkyloxy-benzothiadiazole (ROBT) as an acceptor and thienoacenes as donor units were synthesized and tested for polymer solar cells (PSCs). These new polymers had different donor units with varied electron-donating ability (thieno[3,2-b]thiophene (TT), dithieno[3,2-b:2',3'-d]thiophene (DTT), benzo[1,2-b:4,5-b']dithiophene (BDT), and naphtha[1,2-b:5,6-b']dithiophene (NDT)) in the polymer backbone. To understand the effect of these thienoacenes on the optoelectronic and photovoltaic properties of the copolymers, we systematically analyzed and compared the energy levels, crystallinity, morphology, charge recombination, and charge carrier mobility in the resulting polymers. In this series, optimized photovoltaic cells yielded power conversion efficiency (PCE) values of 6.25% (TT), 9.02% (DTT), 6.34% (BDT), and 2.29% (NDT) with different thienoacene donors. The introduction of DTT into the thienoacene-ROBT polymer enabled the generation of well-ordered molecular packings with a π-π stacking distance of 3.72 Å, high charge mobilities, and an interconnected nanofibrillar morphology in blend films. As a result, the PSC employing the polymer with DTT exhibited the highest PCE of 9.02%. Thus, our structure-property relationship studies of thienoacene-ROBT-based polymers emphasize that the molecular design of the polymers must be carefully optimized to develop high efficient PSCs. These findings will help us to understand the impact of the donor thienoacene on the optoelectronic and photovoltaic performance of polymers.

Solution-processed organic solar cells are promising owing to their light weight, ease of processability, low cost, flexibility, and large-area fabrication. Particularly, small-molecule active materials have been recently developed using straightforward synthesizing methods, exhibiting the least batch-to-batch variation in physical and optoelectronic properties and highly reproducible efficiency. A series of 2D-BDT-based active materials with various numbers of benzodithiophene (BDT) units and how the number of 2D-BDT units influences the construction of a well-defined interconnected structure are reported. The systematically controlled morphology of the 2D-BDT material helps achieve a high power-conversion efficiency (PCE) of 8.56% and a high fill factor of 0.73 without the use of additives. The reduced charge recombination and well-constructed morphology of this material facilitate a PCE of 7.45% in a 77.8 cm2 rigid module, which is the outstanding performance in large-area modules.