Quantum Coherent Beating in Polar Disubphthalocyanine-Fullerene Cocrystals for Ultrafast Photothermal Conversion
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Cocrystallization is an effective pathway to enhance the performance of optoelectronic devices. A dumbbell-shaped disubphthalocyanine (DiSubPc) linked by oligoynes, namely 2DiSubPc and 4DiSubPc, has been successfully prepared. The supramolecular interactions of DiSubPcs with fullerenes are comprehensively investigated. Different from 2DiSubPc-C60 cocrystals, 2DiSubPc-C70 ones exhibit an unexpectedly polar noncentrosymmetric packing, despite being composed of two centrosymmetric components. In 2DiSubPc-C70, 17.6 GHz quantum coherent beating and ultrafast energy transfer to delocalized states over the whole structure is observed, which is a rare feature in supramolecular two-component organic systems. Based on this nonradiative mechanism, the dense polar packing opens an additional route for ultrafast photothermal conversion, which can rapidly reach 228℃ within 5 s upon 0.5 W cm−2 laser irradiation, and achieve the highest equilibrium temperature of 242℃ among all reported organic solids (not dispersed in solutions). This study provides a new paradigm for the development of quantum-enhanced energy conversion materials.
