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Charge transport and polarity in organic D–A mixed‐stack crystals are examined in terms of super‐exchange electronic couplings. When the super‐exchange coupling is dominated by the interaction between donor HOMO and acceptor LUMO, ambipolar transport is achieved. Otherwise, involvement of other bridge orbitals can lead to unbalanced, even to unipolar transport in a special case that the HOMO–LUMO...
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