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The crystal chemistry of spin crossover (SCO) behavior in coordination compounds can potentially be in association with smart materials—promising materials for applications as components of memory devices, displays, sensors and mechanical devices and, especially, actuators, such as artificial muscles. This Special Issue is devoted to various aspects of SCO and related research, comprising 18 interesting original papers on valuable and important SCO topics. Significant and fundamental scientific attention has been focused on the SCO phenomena in a wide research range of fields of fundamental chemical and physical and related sciences, containing the interdisciplinary regions of chemical and physical sciences related to the SCO phenomena. Coordination materials with bistable systems between the LS and the HS states are usually triggered by external stimuli, such as temperature, light, pressure, guest molecule inclusion, soft X-ray, and nuclear decay. Since the first Hofmann-like spin crossover (SCO) behavior in {Fe(py)2[Ni(CN)4]}n (py = pyridine) was demonstrated, this crystal chemistry motif has been frequently used to design Fe(II) SCO materials to enable determination of the correlations between structural features and magnetic properties.

spin crossover --- spin transition --- cobalt(II) ion --- paramagnetic ligand --- aminoxyl --- switch --- mosaicity --- spin crossover --- X-ray diffraction --- fatigability --- single crystal --- phase transition --- structural disorder --- spin-crossover --- dinuclear triple helicate --- Fe(II) --- solvent effects --- metal dithiolene complexes --- [Au(dmit)2]?, [Au(dddt)2]? --- ion-pair crystals --- [Fe(III)(3-OMesal2-trien)]+ --- coordination complexes --- crystal structure --- magnetic properties --- magnetic susceptibility --- magnetization --- spin-crossover transition --- Fe(II) complex --- dipyridyl-N-alkylamine ligands --- high spin (HS) --- low spin (LS) --- spin cross-over (SCO) --- magnetic transition --- cobalt oxide --- spin polaron --- impurity effect --- spin-state crossover --- coordination polymer --- supramolecular isomerism --- spin crossover --- crystal engineering --- spin crossover --- X-ray absorption spectroscopy --- soft X-ray induced excited spin state trapping --- high spin --- spin-crossover --- LIESST effect --- hydrogen bonding --- ?-? interactions --- charge-transfer phase transition --- iron mixed-valence complex --- hetero metal complex --- dithiooxalato ligand --- substitution of 3d transition metal ion --- ferromagnetism --- dielectric response --- 57Fe Mössbauer spectroscopy --- Fe(III) coordination complexes --- hexadentate ligand --- Schiff base --- spin crossover --- UV-Vis spectroscopy --- SQUID --- EPR spectroscopy --- spin-crossover --- optical microscopy --- reaction diffusion --- spin crossover --- Fe(III) complex --- qsal ligand --- thermal hysteresis --- structure phase transition --- counter-anion --- solvate --- lattice energy --- optical conductivity spectrum --- spiral structure --- 1,2-bis(4-pyridyl)ethane --- supramolecular coordination polymer --- chiral propeller structure --- atropisomerism --- spin crossover --- iron(II) complexes --- C–H···? interactions --- magnetic properties --- thermochromism --- spin crossover --- linear pentadentate ligand --- iron(II) --- mononuclear --- 1,2,3-triazole --- crystal structure --- magnetic properties --- DFT calculation --- intermolecular interactions --- amorphous --- spin crossover --- Cu(II) complexes --- nitroxides --- phase transitions --- magnetostructural correlations --- iron (II), spin crossover --- X-ray diffraction --- coordination polymers --- n/a