Intramolecular Chloro-Sulfur Interaction and Asymmetric Side-Chain Isomerization to Balance Crystallinity and
Wei Gao1,2, Mengyun Jiang3, Ziang Wu4
1Department of Materials Science and Engineering, City University of Hong Kong, Kowloon, 999077, Hong Kong, Hong Kong.
Abstract:
Intramolecular Cl-S non-covalent interaction is introduced to modify molecular backbone of a benzodithiophene terthiophene rhodamine (BTR) benchmark structure, helping planarize and rigidify the molecular framework for improving charge transport. Theoretical simulations and temperature-variable NMR experiments clearly validate the existence of Cl-S non-covalent interaction in two designed chlorinated donors and explain its important role in enhancing planarity and rigidity of the molecules for enhancing their crystallinity. The asymmetric isomerization of side-chains further optimizes the molecular orientation and surface energy to strike a balance between its crystallinity and miscibility. This carefully manipulated molecular design helps result in increased carrier mobility and suppressed charge recombination to obtain simultaneously enhanced short-circuit current (Jsc ) and fill factor (FF) and a very high efficiency of 15.73 % in binary all-small-molecule organic solar cells.
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