Abstract
A 6-oxophenalenoxyl system is found to be the first example of the molecular system with redox-based spin diversity nature. To generalize this nature, we focus on the 3-oxophenalenoxyl system as a topological isomer of 6-oxophenalenoxyl system. The radical dianion derivative 3 which is the redox state in the 3-oxophenalenoxyl system was successfully generated by the reduction of the corresponding hydroxyphenalenone 5 with potassium mirror. Our ESR/ENDOR/TRIPLE measurements and DFT calculation of 3 demonstrated that the 3-oxophenalenoxyl system has also redox-based spin diversity nature. In addition, for the elucidation of the interplay between spin and charge fluctuation in 3, we discuss a VB approach derived from MO calculations.
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