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Multiferroic charge-transfer crystals have drawn significant interest due to their simultaneous dipolar and spin ordering. Numerous theoretical and experimental studies have shown that the molecular stacking between donor and acceptor complexes plays an important role in tuning charge-transfer enabled multifunctionality. Herein, we show that the charge-transfer interactions can be controlled by the segregated stack, consisting of polythiophene donor- and fullerene acceptor-based all-conjugated block copolymers. Room temperature magnetic field effects, ferroelectricity, and anisotropic magnetism are observed in charge-transfer crystals, which can be further controlled by photoexcitation and charge doping. Furthermore, the charge-transfer segregated stack crystals demonstrate external stimuli controlled polarization and magnetization, which opens up their multifunctional applications for all-organic multiferroics.
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