The influence caused by the position of the chlorine atom on end groups of two non-fullerene acceptors (ITIC-2Cl-delta and ITIC-2Cl-gamma) was intensely investigated. The single-crystal structures show that ITIC-2Cl-gamma has a better molecular planarity and closer pi-pi interaction distance. More importantly, a 3D rectangle-like interpenetrating network is formed in ITIC-2Cl-gamma and is beneficial to rapid charge transfer along multiple directions, whereas only a linear stacked structure could be observed in ITIC-2Cl-delta. The two acceptor-based solar cells show power conversion efficiencies (PCEs) over 11%, higher than that of the ITIC-2Cl-m-based device (10.85%). An excellent PCE of 13.03% is obtained by the ITIC-2Cl-gamma-based device. In addition, the ITIC-2Cl-gamma-based device also shows the best device stability. This study indicates that chlorine positioning has a great impact on the acceptors; more importantly, the 3D network structure may be a promising strategy for non-fullerene acceptors to improve the PCE and stability of organic solar cells.
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