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A four-stepped cascade of Fe(ii) high spin (HS) to low spin (LS) states is demonstrated in a family of 2-D Hofmann materials, [Fe 3  II (saltrz) 6 (M II (CN) 4 ) 3 ]·8(H 2 O) (M II = Pd ( 1 Pd  ), Pt ( 1 Pt  ); saltrz = ( E )-2-(((4 H -1,2,4-triazol-4-yl)imino)methyl)phenol). Alongside the fully HS and LS Fe(ii) states, fractional spin state stabilization occurs at HS/LS values of 5/6, 2/3, and 1/6. This unconventional spin state periodicity is driven by the presence of multiple spin crossover (SCO) active Fe(ii) sites which are in subtly distinct environments driven by a network of antagonistic host-host and host-guest interactions. Alternating long- and short-range magnetostructural ordering is achieved over the five distinct spin state ratios HS 1.0 LS 0.0 , HS 0.833 LS 0.167 , HS 0.667 LS 0.333 , HS 0.167 LS 0.833 , and HS 0.0 LS 1.0 owing to the flexibility of this 2-D interdigitated lattice topology interconnected by intermolecular interactions. A distinct wave-like spin state patterning is structurally evidenced for each intermediate phase.

Four-step iron(ii) spin state cascade driven by antagonistic solid state interactions