The application of polymer solar cells requires the realization of high efficiency, high stability, and low cost devices. Here we demonstrate a low-cost polymer donor poly[(thiophene)-alt-(6,7-difluoro-2-(2-hexyldecyloxy)quinoxaline)] (PTQ10), which is synthesized with high overall yield of 87.4% via only two-step reactions from cheap raw materials. More importantly, an impressive efficiency of 12.70% is obtained for the devices with PTQ10 as donor, and the efficiency of the inverted structured PTQ10-based device also reaches 12.13% (certificated to be 12.0%). Furthermore, the as-cast devices also demonstrate a high efficiency of 10.41% and the devices exhibit insensitivity of active layer thickness from 100 nm to 300 nm, which is conductive to the large area fabrication of the devices. In considering the advantages of low cost and high efficiency with thickness insensitivity, we believe that PTQ10 will be a promising polymer donor for commercial application of polymer solar cells.

In organic solar cells (OSCs), cathode interfacial materials are generally designed with highly polar groups to increase the capability of lowering the work function of cathode. However, the strong polar group could result in a high surface energy and poor physical contact at the active layer surface, posing a challenge for interlayer engineering to address the trade-off between device stability and efficiency. Herein, we report a hydrogen-bonding interfacial material, aliphatic amine-functionalized perylene-diimide (PDINN), which simultaneously down-shifts the work function of the air stable cathodes (silver and copper), and maintains good interfacial contact with the active layer. The OSCs based on PDINN engineered silvercathode demonstrate a high power conversion efficiency of 17.23% (certified value 16.77% by NREL) and high stability. Our results indicate that PDINN is an effective cathode interfacial material and interlayer engineering via suitable intermolecular interactions is a feasible approach to improve device performance of OSCs.

Herein, we investigated a series of fullerene-free organic solar cells (OSCs) based on six different donor:acceptor (D:A) blends with varied highest occupied molecular orbital (HOMO) offsets from −0.05 to 0.21 eV. First, to verify the energetic compatibility of a specific D:A pair, especially for HOMO offsets, we established a simple method to estimate the hole transfer tendencies between D and A by using bilayer hole-only devices. It reveals that the asymmetrical diode effect of the bilayer hole-only devices can correlate with the FF and J sc of the relevant OSCs. Second, to find out whether HOMO offset is the main restriction of hole transfer, we measured transient absorption spectra and examined the hole transfer behavior in the blends, revealing that the occurrence of hole transfer is independent of the HOMO offsets and ultrafast in the time scale of ≤4.6 ps for those blends with ≥0 eV HOMO offsets. In contrast, a negative HOMO offset can significantly slow down the hole transfer with a half-time of ∼400 ps. Furthermore, we compare the device parameters under varied light intensities and discover that the bimolecular recombination should be one of the main restrictions for high device performance. Surprisingly, small HOMO offsets of 0 and 0.06 eV can also enable high PCEs of 10.42% and 11.75% for blend 2 (PTQ10:HC-PCIC) and blend 3 (PBDB-TF:HC-PCIC), respectively. Overall, our work demonstrates not only the validity of high-performance OSCs operating at the near zero HOMO offsets but also the charge dynamic insights of these blends, which will help gain understanding on the further improvement of OSCs.

Achieving efficient charge transfer at small frontier molecular orbital offsets between donor and acceptor is crucial for high performance polymer solar cells (PSCs). Here we synthesize a new wide band gap polymer donor, PTQ11, and a new low band gap acceptor, TPT10, and report a high power conversion efficiency (PCE) PSC (PCE = 16.32%) based on PTQ11–TPT10 with zero HOMO (the highest occupied molecular orbital) offset (ΔE HOMO(D–A)). TPT10 is a derivative of Y6 with monobromine instead of bifluorine substitution, and possesses upshifted lowest unoccupied molecular orbital energy level (E LUMO) of −3.99 eV and E HOMO of −5.52 eV than Y6. PTQ11 is a derivative of low cost polymer donor PTQ10 with methyl substituent on its quinoxaline unit and shows upshifted E HOMO of −5.52 eV, stronger molecular crystallization, and better hole transport capability in comparison with PTQ10. The PSC based on PTQ11–TPT10 shows highly efficient exciton dissociation and hole transfer, so that it demonstrates a high PCE of 16.32% with a higher V oc of 0.88 V, a large J sc of 24.79 mA cm–2, and a high FF of 74.8%, despite the zero ΔE HOMO(D–A) value between donor PTQ11 and acceptor TPT10. The PCE of 16.32% is one of the highest efficiencies in the PSCs. The results prove the feasibility of efficient hole transfer and high efficiency for the PSCs with zero ΔE HOMO(D–A), which is highly valuable for understanding the charge transfer process and achieving high PCE of PSCs.

The precise control of stoichiometric balance and ionic defects on the surface of solution-processed perovskite is critical to the performance and stability of perovskite solar cells (pero-SCs). Here, we introduce a low-cost and stable conjugated donor polymer (PTQ10) as interfacial layer in the planar n–i–p structured pero-SCs. The polymer was applied to the perovskite intermediate phase before the thermal annealing. This treatment significantly reduced the loss of surface organic cation during thermal annealing. Importantly, the kinetics of phase conversion of perovskite was influenced, and perovskite crystal showed a more preferential orientation. Moreover, the polymer proved to be an effective hole extraction layer due to the proper energy alignment with perovskite. Finally, a champion power conversion efficiency of the planar pero-SCs was achieved at 21.2% with a high fill factor of 81.6%. The devices also showed great ambient and thermal stability. This work presents a facile way of perovskite surface control to achieve high-performance pero-SCs.

A universal layer-by-layer solution-processing approach is proven to be effective for the fabrication of high-performance non-fullerene organic solar cells.

The application of polymer solar cells (PSCs) with n-type organic semiconductor as acceptor requires further improving powder conversion efficiency, increasing stability and decreasing cost of the related materials and devices. Here we report a simplified synthetic route for 4,4,9,9-tetrahexyl-4,9-dihydro-s-indaceno [1,2-b:5,6-b’] dithiophene by using the catalyst of amberlyst15. Based on this synthetic route and methoxy substitution, two low cost acceptors with less synthetic steps, simple post-treatment and high yield were synthesized. In addition, the methoxy substitution improves both yield and efficiency. The high efficiency of 13.46% was obtained for the devices with MO-IDIC-2F (3,9-bis(2-methylene-5 or 6-fluoro-(3-(1,1-dicyanomethylene)-indanone)-4,4,9,9-tetrahexyl-5,10-dimethoxyl-4,9-dihydro-s-indaceno[1,2-b:5,6-b’] dithiophene) as acceptor. Based on the cost analysis, the PSCs based on MO-IDIC-2F possess the great advantages of low cost and high photovoltaic performance in comparison with those PSCs reported in literatures. Therefore, MO-IDIC-2F will be a promising low cost acceptor for commercial application of PSCs.

In the last two years, polymer solar cells (PSCs) developed quickly with n-type organic semiconductor (n-OSs) as acceptor. In contrast, the research progress of nonfullerene organic solar cells (OSCs) with organic small molecule as donor and the n-OS as acceptor lags behind. Here, we synthesized a D-A structured medium bandgap organic small molecule H11 with bithienyl-benzodithiophene (BDTT) as central donor unit and fluorobenzotriazole as acceptor unit, and achieved a power conversion efficiency (PCE) of 9.73% for the all organic small molecules OSCs with H11 as donor and a low bandgap n-OS IDIC as acceptor. A control molecule H12 without thiophene conjugated side chains on the BDT unit was also synthesized for investigating the effect of the thiophene conjugated side chains on the photovoltaic performance of the p-type organic semiconductors (p-OSs). Compared with H12, the 2D-conjugated H11 with thiophene conjugated side chains shows intense absorption, low-lying HOMO energy level, higher hole mobility and ordered bimodal crystallite packing in the blend films. Moreover, a larger interaction parameter (χ) was observed in the H11 blends calculated from Hansen solubility parameters and differential scanning calorimetry measurements. These special features combined with the complementary absorption of H11 donor and IDIC acceptor resulted in the best PCE of 9.73% for nonfullerene all small molecule OSCs up to date. Our results indicate that fluorobenzotriazole based 2D conjugated p-OSs are promising medium bandgap donors in the nonfullerene OSCs.