Remarkable Impact of KBr Pelletization on Spin Switching: Probing Hofmann-Type 3D Spin-crossover Frameworks by Solid-State Optical Spectroscopy

Abstract

KBr pelletization profoundly influences the thermal and photoinduced spin-crossover behavior in dehydrated [Fe1-xMx(pz)Pd(CN)4] in bulk, nanoparticles and polymer composite forms by inducing tensile strain, defects, dopant-rattling, and electrostatic perturbations that alter ∆E0HL and cooperativity. It enables hidden thermal switching, dopant dynamics, and quantum-tunneling-driven LIESST relaxation, revealing mechanical processing as a versatile tool to tune spin-state energetics and cooperativity.