A novel alcohol-soluble n-type conjugated polyelectrolyte (n-CPE) poly-2,5-bis(2-octyldodecyl)-3,6-bis(thiophen-2-yl)-pyrrolo [3,4-c]pyrrole-1,4-dione-alt-2,5-bis [6-(N,N,N-trimethylammonium)hexyl]-3,6-bis(thiophen-2-yl)-pyrrolo[3,4-c]pyrrole-1,4-dione (PDPPNBr) is synthesized for applications as an electron transport layer (ETL) in an inverted polymer solar cells (PSCs) device. Because of the electron-deficient nature of diketopyrrolopyrrole (DPP) backbone and its planar structure, PDPPNBr is endowed with high conductivity and electron mobility. The interfacial dipole moment created by n-CPE PDPPNBr can substantially reduce the work function of ITO and induce a better energy alignment in the device, facilitating electron extraction and decreasing exctions recombination at active layer/cathode interface. As a result, the power conversion efficiency (PCE) of the inverted devices based poly(3-hexylthiophene) (P3HT):(6,6)-phenyl-C 61 butyric acid methyl ester (PC 61 BM) active layer with PDPPNBr as ETL achieves a value of 4.03%, with 25% improvement than that of the control device with ZnO ETL. Moreover, the universal PDPPNBr ETL also delivers a notable PCE of 8.02% in the devices based on polythieno[3,4-b]-thiophene-co-benzodithiophene (PTB7):(6,6)-phenyl-C 71 -butyric acid methyl ester (PC 71 BM). To our best knowledge, this is the first time that n-type conjugated polyelectrolyte-based cathode interlayer is reported. Quite different from the traditional p-type conjugated and nonconjugated polyelectrolytes ETLs, n-CPE PDPPNBr as ETL could function efficiently with a thickness approximate 30 nm because of the high conductivity and electron mobility. Furthermore, the PDPPNBr interlayer also can ensure the device with the improved long-term stability. The successful application of this alcohol solution processed n-type conjugated polyelectrolyte indicates that the electron-deficient planar structure with high electron mobility could be very promising in developing high performance and environmentally friendly polymer solar cells.

A novel triple dipole effect has been observed for Cl-assisted self-assembled small-molecules on ITO substrate, and a highest polymer solar cell performance of 9.2% is obtained.

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Two novel liquid-crystal-conjugated polyelectrolytes (LCCPEs) poly[9,9-bis[6-(4-cyanobiphenyloxy)-hexyl]-fluorene-alt-9,9-bis(6-(N,N-diethylamino)-hexyl)-fluorene] (PF6Ncbp) and poly[9,9-bis[6-(4-cyanobiphenyloxy)-hexyl]-fluorene-alt-9,9-bis(6-(N-methylimidazole)-hexyl]-fluorene] (PF6lmicbp) are obtained by covalent linkage of the cyanobiphenyl mesogen polar groups onto conjugated polyelectrolytes. After deposition a layer of LCCPEs on ZnO interlayer, the spontaneous orientation of liquid-crystal groups can induce a rearrangement of dipole moments at the interface, subsequently leading to the better energy-level alignment. Moreover, LCCPEs favors intimate interfacial contact between ZnO and the photon harvesting layer and induce active layer to form the nanofibers morphology for the enhancement of charge extraction, transportation and collection. The water/alcohol solubility of the LCCPEs also enables them to be environment-accepted solvent processability. On the basis of these advantages, the poly(3-hexylthiophene) (P3HT):[6,6]-phenyl-C60-butyric acid methyl ester (PC60BM)-based inverted polymer solar cells (PSCs) combined with ZnO/PF6Ncbp and ZnO/PF6lmicbp bilayers boost the power conversion efficiency (PCE) to 3.9% and 4.2%, respectively. Incorporation of the ZnO/PF6lmicbp into the devices based on a blend of a narrow band gap polymer thieno[3,4-b]thiophene/benzodithiophene (PTB7) with [6,6]-phenyl C70-butyric acid methyl ester (PC71BM) affords a notable efficiency of 7.6%.

Although ternary organic solar cells (OSCs) have unique advantages in improving device performance, the morphology assembly in the ternary‐phase would be more uncertain or complex than that in the binary‐phase. Here, we propose a new concept of oligomer‐assisted photoactive layers for high‐performance OSCs. The formed alloy‐like phase of the oligomer : host polymer blend enabled the oligomer‐assisted OSCs to fuse the advantages of both binary and ternary devices, exhibiting substantially enhanced performance and stability compared to the control devices. With the addition of oligomers, outstanding efficiencies of 17.33 % for a PM6 : Y6 device, 18.32 % for a PM6 : BTP‐eC9 device, and 17.13 % for a PM6/Y6 pseudo‐bilayer device were achieved, all of which are one of the highest values in their corresponding fields. The improved performance originated from the downshift energy levels, enhanced light absorption, optimized blend morphology, favorable charge dynamics, and reduced non‐radiative energy loss.

Semitransparent organic solar cells (ST‐OSCs) based on all narrow bandgap (all‐NBG) semiconductors are attractive for building integration. Unfortunately, advanced NBG Y‐series acceptors cannot well match with the NBG donors, resulting from their mismatched energy levels and poor compatibility. Herein, a facile terpolymer design strategy is adopted to improve the matching of Y6 with efficient NBG polymer donor PCE10. F or Cl atom functionalized benzodithiophene (BDT) are introduced into the PCE10 matrix to afford two series of terpolymers, namely PCE10‐BDT2F and PCE10‐BDT2Cl. Compared with PCE10, all terpolymers show deeper energy levels, higher extinction coefficients, enhanced face‐on orientation, and better compatibility with Y6. Consequently, significant breakthroughs are achieved for both opaque and semitransparent devices. Particularly, a record power conversion efficiency (PCE) of 13.80% is achieved by PCE10‐BDT2F:Y6‐based device, nearly 40% higher than PCE10:Y6‐based device. ST‐OSCs also achieve impressive PCEs of 12.00% and 10.85% with average visible transmittance (AVT) of 30.98% and 41.08%, respectively, and both PCEs are the highest values with AVT over 30% and 40%. An outstanding light utilization efficiency (LUE) of 4.46% further demonstrates the successful balance of PCE and AVT. These results demonstrate that the design of NBG terpolymers is a facile and highly encouraging strategy for promoting breakthroughs in ST‐OSCs.

Overlapping near-infrared absorption not only does not reduce short-circuit current density (JSC), but also can ensure a high average visible transmittance (AVT) and get a high open-circuit voltage (VOC) and power conversion efficiency (PCE) at the same time.

The polar groups in the conjugated polyelectrolytes (CPEs) can create the favorable dipoles at the electrode/active layer interface, which is critical for the CPEs to minimize the interfacial energy barrier in polymer solar cells (PSCs). Herein, a series of CPEs based on poly [(9,9-bis(3'-(N,N-dimethylamino)propyl)-2,7-fluorene)-co-2,7-(9,9-dioctylfluorene)] derivates (PFNs) (PFN30, PFN50, PFN70, and PFN100) with different mole ratio of polar groups (-N(C2H5)2) were designed and synthesized to investigate the effect of the numbers of polar groups on the interfacial dipoles. Controllably interfacial dipoles could be readily achieved by only tuning the numbers of -N(C2H5)2 in PFNs, as revealed by the work function of the PFNs modified ITO gradually reduced as the loadings of the -N(C2H5)2 increased. In addition, increasing the numbers of -N(C2H5)2 in PFNs were also favorable for developing the smooth and homogeneous morphology of the active layer. As a result, the content of the polar amine in the PFNs exerted great influence on the performance of polymer solar cells. Increasing the numbers of the pendent -N(C2H5)2 could effectively improve the power conversion efficiency (PCE) of the devices. Among these PFNs, PFN100 with the highest content of -N(C2H5)2 polar groups delivered the device with the best PCE of 3.27%. It indicates tailoring the content of the polar groups in the CPEs interlayer is a facial and promising approach for interfacial engineering to developing high performance PSCs.