Simutaneously high open circuit voltage and high short circuit current density is a big challenge for achieving high efficiency polymer solar cells due to the excitonic nature of organic semdonductors. Herein, we developed a trialkylsilyl substituted 2D-conjugated polymer with the highest occupied molecular orbital level down-shifted by Si–C bond interaction. The polymer solar cells obtained by pairing this polymer with a non-fullerene acceptor demonstrated a high power conversion efficiency of 11.41% with both high open circuit voltage of 0.94 V and high short circuit current density of 17.32 mA cm−2 benefitted from the complementary absorption of the donor and acceptor, and the high hole transfer efficiency from acceptor to donor although the highest occupied molecular orbital level difference between the donor and acceptor is only 0.11 eV. The results indicate that the alkylsilyl substitution is an effective way in designing high performance conjugated polymer photovoltaic materials.

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.

High-efficiency all-polymer solar cells with less thickness-dependent behavior are demonstrated by using a low bandgap n-type conjugated polymer N2200 as acceptor and an absorption-complementary difluorobenzotriazole-based medium-bandgap polymer J51 as donor.

Low bandgap n-type organic semiconductor (n-OS) ITIC has attracted great attention for the application as an acceptor with medium bandgap p-type conjugated polymer as donor in nonfullerene polymer solar cells (PSCs) because of its attractive photovoltaic performance. Here we report a modification on the molecular structure of ITIC by side-chain isomerization with meta-alkyl-phenyl substitution, m-ITIC, to further improve its photovoltaic performance. In a comparison with its isomeric counterpart ITIC with para-alkyl-phenyl substitution, m-ITIC shows a higher film absorption coefficient, a larger crystalline coherence, and higher electron mobility. These inherent advantages of m-ITIC resulted in a higher power conversion efficiency (PCE) of 11.77% for the nonfullerene PSCs with m-ITIC as acceptor and a medium bandgap polymer J61 as donor, which is significantly improved over that (10.57%) of the corresponding devices with ITIC as acceptor. To the best of our knowledge, the PCE of 11.77% is one of the highest values reported in the literature to date for nonfullerene PSCs. More importantly, the m-ITIC-based device shows less thickness-dependent photovoltaic behavior than ITIC-based devices in the active-layer thickness range of 80-360 nm, which is beneficial for large area device fabrication. These results indicate that m-ITIC is a promising low bandgap n-OS for the application as an acceptor in PSCs, and the side-chain isomerization could be an easy and convenient way to further improve the photovoltaic performance of the donor and acceptor materials for high efficiency PSCs.

Non-fullerene polymer solar cells (PSCs) with solution-processable n-type organic semiconductor (n-OS) as acceptor have seen rapid progress recently owing to the synthesis of new low bandgap n-OS, such as ITIC. To further increase power conversion efficiency (PCE) of the devices, it is of a great challenge to develop suitable polymer donor material that matches well with the low bandgap n-OS acceptors thus providing complementary absorption and nanoscaled blend morphology, as well as suppressed recombination and minimized energy loss. To address this challenge, we synthesized three medium bandgap 2D-conjugated bithienyl-benzodithiophene-alt-fluorobenzotriazole copolymers J52, J60, and J61 for the application as donor in the PSCs with low bandgap n-OS ITIC as acceptor. The three polymers were designed with branched alkyl (J52), branched alkylthio (J60), and linear alkylthio (J61) substituent on the thiophene conjugated side chain of the benzodithiophene (BDT) units for studying effect of the substituents on the photovoltaic performance of the polymers. The alkylthio side chain, red-shifted absorption down-shifted the highest occupied molecular orbital (HOMO) level and improved crystallinity of the 2D conjugated polymers. With linear alkylthio side chain, the tailored polymer J61 exhibits an enhanced JSC of 17.43 mA/cm(2), a high VOC of 0.89 V, and a PCE of 9.53% in the best non-fullerene PSCs with the polymer as donor and ITIC as acceptor. To the best of our knowledge, the PCE of 9.53% is one of the highest values reported in literature to date for the non-fullerene PSCs. The results indicate that J61 is a promising medium bandgap polymer donor in non-fullerene PSCs.

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.

All-polymer solar cells (all-PSCs) offer unique morphology stability for the application as flexible devices, but the lack of high-performance polymer acceptors limits their power conversion efficiency (PCE) to a value lower than those of the PSCs based on fullerene derivative or organic small molecule acceptors. We herein demonstrate a strategy to synthesize a high-performance polymer acceptor PZ1 by embedding an acceptor-donor-acceptor building block into the polymer main chain. PZ1 possesses broad absorption with a low band gap of 1.55 eV and high absorption coefficient (1.3×10 cm ). The all-PSCs with the wide-band-gap polymer PBDB-T as donor and PZ1 as acceptor showed a record-high PCE of 9.19 % for the all-PSCs. The success of our polymerization strategy can provide a new way to develop efficient polymer acceptors for all-PSCs.

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.