Cooperative spin-state switching and anisotropic charge transport in two-dimensional Fe( ii ) Hofmann-type nitroprusside frameworks

NO] dominates the valence to conduction electronic transitions through metal to ligand charge transfer processes, whereas the external ligands modulate charge redistribution and transport pathways. Conductivity calculations further reveal pronounced anisotropic charge transport and enhanced electronic delocalization in NP-Py, which exhibits stronger low-energy optical features, larger spin-dependent hybridization, and a more pronounced band gap reduction than NP-4MIso. These results provide new insight into the cooperative SCO behavior of Fe(II) nitroprusside-based polymers and highlight their potential as electronically active materials with tunable magnetic and transport responses.