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The methanol solvomorph 1 • 2MeOH of the cobalt(II) complex [Co(L Sal,2À Ph ) 2 ] (1) with the sterically demanding Schiff-base ligand 2-(([1,1'-biphenyl]-2-ylimino)methyl)phenol (HL Sal,2À Ph ) shows the thus far largest dihedral twist distortion between the two chelate planes compared to an ideal pseudotetrahedral arrangement. The cobalt(II) ion in 1 • 2MeOH exhibits an easy-axis anisotropy leading to a spinreversal barrier of 55.3 cm À 1 , which corresponds to an increase of about 17 % induced by the larger dihedral twist compared to the solvent-free complex 1. The magnetic relaxation for 1 • 2MeOH is significantly slower compared to 1. An in-depth frequency-domain Fourier-transform (FD-FT) THz-EPR study not only allowed the direct measurement of the magnetic transition between the two lowest Kramers doublets for the cobalt(II) complexes, but also revealed the presence of spin-phonon coupling. Interestingly, a similar dihedral twist correlation is also observed for a second pair of cobalt(II)-based solvomorphs, which could be benchmarked by FD-FT THz-EPR.

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Two new mononuclear cobalt(II) complexes with the general formula [Co(L1,2)2] (1 and 2) were synthesized using bidentate Schiff base ligands with NO donor set, namely, 2-(benzothiazole-2-ylimino)methyl)-5-(diethylamino)phenol (HL1) and its methyl...