Electronic and molecular structures of C60-based polyanionic high-spin molecular clusters: Direct spin identification and electron spin transient nutation spectroscopy for high-spin chemistry

C60-based polyanionic high-spin clusters (S = 1-3) in their ground state have been prepared by chemical reductions of pristine C60 fullerene in 2-methyltetrahydrofuran, being identified by CW-ESR and pulse-ESR-based two-dimensional electron spin transient nutation spectroscopy in the glass. The molecular structures of the clusters have been determined by a well-established semi-empirical D-tensor approach.