Zhiguo Zhang

A novel non-fullerene electron acceptor (ITIC) that overcomes some of the shortcomings of fullerene acceptors, for example, weak absorption in the visible spectral region and limited energy-level variability, is designed and synthesized. Fullerene-free polymer solar cells (PSCs) based on the ITIC acceptor are demonstrated to exhibit power conversion efficiencies of up to 6.8%, a record for fullerene-free PSCs. As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.

Abstract 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.

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.

With the power conversion efficiency of polymer solar cells (PSCs) approaching the milestone value of 10%, their instability associated with a low work function metal cathode, particularly in the presence of oxygen and moisture, becomes a critical issue for real applications. To alleviate the air-sensitive problem, two easy-accessible solution-processed, environmentally friendly organic small-molecule cathode interlayers, with perylene diimides (PDI) as the core and amino (PDIN) or amino N-oxide (PDINO) as the terminal substituent, are explored. Benefitting from the extended planar structure of the PDI units, the two interlayer materials show high conductivities of ∼10−5 S cm−1, which make them capable of functioning efficiently in a wide thickness range of 6 to 25 nm. This is the first time that thickness-insensitive small-molecule-based cathode interlayers are reported. It is also found that the work function tuning effect of the two PDI-based interlayers allows high work function metals (such as Au and Ag) to act as the cathode. With the conventional device structure with PTB7 as a donor and PC70BM as an acceptor, the PDINO-based devices exhibit an efficiency of 8.24% with Al as the top electrode and 8.16% with Ag as the top electrode, much higher than that of the corresponding Ca/Al-based device (6.98%). The high efficiency of 8.35% is also achieved in the device with PTB7-Th as the donor. The success of the two PDI-interlayers indicates that π-delocalized planar structures with high electron affinities could be particularly useful in developing high-performance organic interlayer 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.