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In contrast to classical bulk heterojunction (BHJ) in organic solar cells (OSCs), the quasi-homojunction (QHJ) with extremely low donor content (≤10 wt.%) is unusual and generally yields much lower device efficiency. Here, representative polymer donors and nonfullerene acceptors are selected to fabricate QHJ OSCs, and a complete picture for the operation mechanisms of high-efficiency QHJ devices is illustrated. PTB7-Th:Y6 QHJ devices at donor:acceptor (D:A) ratios of 1:8 or 1:20 can achieve 95% or 64% of the efficiency obtained from its BHJ counterpart at the optimal D:A ratio of 1:1.2, respectively, whereas QHJ devices with other donors or acceptors suffer from rapid roll-off of efficiency when the donors are diluted. Through device physics and photophysics analyses, it is observed that a large portion of free charges can be intrinsically generated in the neat Y6 domains rather than at the D/A interface. Y6 also serves as an ambipolar transport channel, so that hole transport as also mainly through Y6 phase. The key role of PTB7-Th is primarily to reduce charge recombination, likely assisted by enhancing quadrupolar fields within Y6 itself, rather than the previously thought principal roles of light absorption, exciton splitting, and hole transport., (© 2022 Wiley-VCH GmbH.)

The terminal electron-withdrawing group is thought to strongly influence π-π stacking interactions and thereby the charge transport properties of fused-ring electron acceptors (FREAs). In this work, we designed and synthesized three asymmetric/symmetric small molecule FREAs ( LC301 , LC302 , and LC303 ), in which three electron-withdrawing functional groups with different polarities (phenyl-fused indanone < thienyl-fused indanone < F-modified phenyl-fused indanone) were selected as the terminal groups. Photophysical properties, electrochemistry, charge transport, and crystalline properties of the materials were studied to investigate the effect of electron-withdrawing abilities of the terminal groups on the properties of FREAs. Starting from the symmetric LC302 (two thienyl-fused indanone terminal groups), we have found that by simply replacing only one thienyl-fused indanone terminal group in symmetric LC302 with one difluorinated phenyl-fused indanone terminal group, the asymmetric LC301 -based organic solar cells (OSCs) can yield a high power conversion efficiency (PCE) of 17.21% and a promising fill factor (FF) of 78.1%, which are higher than those of symmetric LC302 -based OSCs (PCE = 15.18%, FF = 73.3%) and the asymmetric LC303 -based OSCs bearing one thienyl-fused indanone terminal group and one nonfluorinated phenyl-fused indanone terminal group (PCE = 14.28%, FF = 70.3%). The results indicate that the rational selection of terminal groups with different electron-withdrawing capabilities is highly desirable for designing high-performance asymmetric FREAs.

Asymmetric fused-ring electron acceptors (a-FREAs) have proved to be a promising type of electron acceptor for high-performance organic solar cells (OSCs). However, the relationship among molecular structures of a-FREAs and their nanoscale morphology, charge-carrier dynamics, and device performance remains unclear. In this contribution, two FREAs differing in conjugated backbone geometry with an asymmetric conformation (IPT-2F) or symmetric one (INPIC-2F) are selected to systematically explore the superiorities of the asymmetric conformation. Despite the frailer extinction coefficient and weaker crystallinity, IPT-2F shows stronger dipole interactions in the asymmetrical backbone, which would induce a closer lamellar packing than that of the symmetrical counterpart. Using PBDB-T as the electron donor, the IPT-2F-based OSCs achieve the best power conversion efficiency of 14.0%, which is ca. 67% improvement compared to the INPIC-2F-based ones (8.37%), resulting from a simultaneously increased short-circuited current density ( J sc ) and fill factor. Systematical investigations on optoelectronic and morphological properties show that the asymmetric conformation-structured IPT-2F exhibits better miscibility with the polymer donor to induce a favorable blend ordering with small domain sizes and suitable phase separation compared to the INPIC-2F symmetric molecule. This facilitates an efficient charge generation and transport, inhibits charge-carrier recombination, and promotes valid charge extraction in IPT-2F-based devices.

The ternary strategy has been widely used in high-efficiency organic solar cells (OSCs). Herein, we successfully incorporated a mid-band-gap star-shaped acceptor, FBTIC, as the third component into the PM6/Y6 binary blend film, which not only achieved a panchromatic absorption but also significantly improved the open-circuit voltage ( V OC ) of the devices due to the high-lying lowest unoccupied molecular orbital (LUMO) of the FBTIC. Morphology characterizations show that star-shaped FBTIC molecules are amorphously distributed in the ternary system, and the finely tuned ternary film morphology facilitates the exciton dissociation and charge collection in ternary devices. As a result, the best PM6/Y6/FBTIC-based ternary OSCs achieved a power conversion efficiency (PCE) of 16.7% at a weight ratio of 1.0:1.0:0.2.

Three fused-ring electron acceptors (FXIC-1, FXIC-2, and FXIC-3) were designed and synthesized. This FXIC series has similar electron-rich central units and the same electron-poor termini. Due to the different steric structures of fluorene, bifluorenylidene, and spirobifluorene, FXIC-1 is a one-dimensional (1D) crystal, while FXIC-2 and FXIC-3 are multidimensional (MD) amorphous materials. The conformations of the FXIC series have a slight impact on their absorption and energy levels. FXIC-1 has higher electron mobility than FXIC-2 and FXIC-3. When blending with different polymer donors (PTB7-Th, J71, and PM7), the FXIC-1-based organic solar cells have efficiencies higher than those of the FXIC-2/FXIC-3-based cells. Meanwhile, the ternary-blend cells based on PTB7-Th:F8IC with FXIC-1, FXIC-2, and FXIC-3 show similar efficiencies, which are all better than those of the binary-blend devices.

Selecting suitable outermost aromatic rings of the central cores is of particular importance for the design of fused-ring electron acceptors (FREAs) because the direct electronic communication between the outermost aromatic rings and termini exerts a strong impact on the optoelectronic properties of FREAs. In most cases, the outermost rings of the FREA cores are thiophene. This work reported the first example of using pyrrole as the outermost rings of the core. Fused hexacyclic electron acceptor, P6IC, using pyrrole in place of the often-used thiophene as the outermost rings of the central core was synthesized. Compared with its structural analogue F6IC with thiophene as the outermost rings, P6IC exhibits a remarkably upshifted highest occupied molecular orbital energy level (P6IC: -5.43 eV, F6IC: -5.71 eV), a slightly upshifted lowest unoccupied molecular orbital energy level (P6IC: -3.94 eV, F6IC: -4.00 eV), 54 nm red-shifted absorption, a narrower band gap (P6IC: 1.30 eV, F6IC: 1.37 eV), and an enhanced mobility (P6IC: 8.8 × 10 -4 cm 2 V -1 s -1 , F6IC: 7.4 × 10 -4 cm 2 V -1 s -1 ). Organic photovoltaic cells using PTB7-Th/P6IC as a photoactive layer exhibit an efficiency of 12.2%, far surpassing that based on PTB7-Th/F6IC active layer (5.57%). The semitransparent devices using PTB7-Th/P6IC as the active layer yield efficiency of 10.2% with an average visible transmittance (AVT) of 17.0%, far surpassing that based on PTB7-Th/F6IC (5.26% with an AVT of 18.4%).

A new fused-chrysene electron-donating core is synthesized, where chrysene is condensed with two thiophenes via two dihydrobenzene rings. Based on this building block coupled with two electron-accepting end groups of 1,1-dicyanomethylene-3-indanone, a new Z-shaped fused-ring electron acceptor, FCIC, is designed and synthesized. FCIC shows intense absorption in the 500-850 nm region, with a maximum molar absorptivity of 1.5 × 10 5 M -1 cm -1 , a bandgap of 1.50 eV, and a charge mobility of 2.5 × 10 -4 cm 2 V -1 s -1 . The ternary organic photovoltaic cells based on PTB7-Th/F8IC/FCIC yield an efficiency of 12.6%, higher than that of the binary cells of PTB7-Th/F8IC (10.7%) and PTB7-Th/FCIC (7.21%). Relative to the PTB7-Th/F8IC binary blend, the addition of FCIC leads to improvement in the open-circuit voltage, short-circuit current, and fill factor.

In order to utilize the near-infrared (NIR) solar photons like silicon-based solar cells, extensive research efforts have been devoted to the development of organic donor and acceptor materials with strong NIR absorption. However, single-junction organic solar cells (OSCs) with photoresponse extending into >1000 nm and power conversion efficiency (PCE) >11% have rarely been reported. Herein, three fused-ring electron acceptors with varying core size are reported. These three molecules exhibit strong absorption from 600 to 1000 nm and high electron mobility (>1 × 10 -3 cm 2 V -1 s -1 ). It is proposed that core engineering is a promising approach to elevate energy levels, enhance absorption and electron mobility, and finally achieve high device performance. This approach can maximize both short-circuit current density (  J SC ) and open-circuit voltage (V OC ) at the same time, differing from the commonly used end group engineering that is generally unable to realize simultaneous enhancement in both V OC and J SC . Finally, the single-junction OSCs based on these acceptors in combination with the widely polymer donor PTB7-Th yield J SC as high as 26.00 mA cm -2 and PCE as high as 12.3%., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Much effort has been devoted to the development of new donor materials for small-molecule organic solar cells due to their inherent advantages of well-defined molecular weight, easy purification, and good reproducibility in photovoltaic performance. Herein, we report two small-molecule donors that are compatible with both fullerene and nonfullerene acceptors. Both molecules consist of an (E)-1,2-di(thiophen-2-yl)ethane-substituted (TVT-substituted) benzo[1,2-b:4,5-b']dithiophene (BDT) as the central unit, and two rhodanine units as the terminal electron-withdrawing groups. The central units are modified with either alkyl side chains (DRBDT-TVT) or alkylthio side chains (DRBDT-STVT). Both molecules exhibit a medium bandgap with complementary absorption and proper energy level offset with typical acceptors like PC 71 BM and IDIC. The optimized devices show a decent power conversion efficiency (PCE) of 6.87% for small-molecule organic solar cells and 6.63% for nonfullerene all small-molecule organic solar cells. Our results reveal that rationally designed medium-bandgap small-molecule donors can be applied in high-performance small-molecule organic solar cells with different types of acceptors.