Abstract
The parent and p-nitrophenyl-substituted diradicals D-3a,b (triplets), tetraradicals T-3a,b (quintets), and hexaradicals H-3a,b (septets) were photochemically generated in matrix-isolated form (toluene, 77 K) by successive denitrogenation of the trisazoalkanes 3a,b and EPR spectrally characterized. In these high-spin polyradicals the spin-spin interaction within the localized spin-carrying 1,3-cyclopentanediyl diradical unit is much stronger than within the cross-conjugated ferromagnetic coupling unit. Accordingly, a change of the electronic properties in the cyclopentanediyl unit affects decisively the D value of the whole polyradical. Therefore, the spin-accepting p-nitro group reduces the D value of the tetra- and hexaradical in the same amount as that of the diradical. Thus, irrespective of the spin multiplicity, the substituent stabilizes electronically the triplet (D-3a,b), quintet (T-3a,b), and septet (H-3a,b) species with equal efficacy.
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