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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.

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

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This Special Issue is one of the first for the new MDPI flagship journal Chemistry (ISSN 2624-8549) which has a broad remit for publishing original research in all areas of chemistry. The theme of this issue is Supramolecular Chemistry in the 3rd Millennium and I am sure that this topic will attract many exciting contributions. We chose this topic because it encompasses the unity of contemporary pluridisciplinary science, in which organic, inorganic, physical and theoretical chemists work together with molecular biologists and physicists to develop a systems-level understanding of molecular interactions. The description of supramolecular chemistry as ‘chemistry beyond the molecule’ (Jean-Marie Lehn, Nobel Lecture and Gautam R. Desiraju, Nature, 2001, 412, 397) addresses the wide variety of weak, non-covalent interactions that are the basis for the assembly of supramolecular architectures, molecular receptors and molecular recognition, programed molecular systems, dynamic combinatorial libraries, coordination networks and functional supramolecular materials. We welcome submissions from all disciplines involved in this exciting and evolving area of science.

Technology: general issues --- anion binding --- chloride receptor --- switchable system --- hydroquinone --- redox switch --- metal-organic frameworks --- vapour sorption --- solvatochromism --- desorption kinetics --- ion-channels --- crown-ethers --- bilayer membranes --- self-assembly --- supramolecular chemistry --- host–guest chemistry --- coordination cage --- catalysis --- crystal structure --- copper chloride complexes --- H-bonding pattern --- tetrazole ligands --- X-ray diffraction --- Hirshfeld surfaces --- uranium(VI) --- carboxylates --- capsules --- structure --- luminescence --- multicomponent cocrystal --- cocrystallization mechanism --- cocrystal synthesis --- crystal engineering --- porous material --- molecular recognition --- halogen bond --- co-crystal --- molecular tecton --- binary solid --- network structure --- σ-hole --- molecular electrostatic potential --- calixarenes --- coordination clusters --- manganese --- molecular magnetism --- host–guest interaction --- cucurbit[7]uril --- 4-pyrrolidinopyridinium --- copper complexes --- chlorido ligand displacement --- catalysis regulation --- Schiff base ligands --- urea hydrolysis --- coordination chemistry --- hydrogen bonds --- metalla-assemblies --- coordination-driven self-assembly --- orthogonality --- ligands --- metal ions --- complementarity --- hydrogen bonding --- cyclotricatechylene --- metal–organic cage --- helicate --- metallosupramolecular --- chirality --- copper(II) complexes --- pyrazolato ligands --- supramolecular assembly --- X-ray crystallography --- magnetic susceptibility --- EPR spectroscopy --- isotropic exchange --- antisymmetric exchange --- dipolar interaction --- DFT calculations --- hydrogen bond --- pyrazine --- chloropyrazine --- chloropyrazin-2-amine --- copper halide --- supramolecular structure --- conformational polymorphism --- intermolecular contacts --- N,N′,N″,N‴-Tetraisopropylpyrophosphoramide --- pyrophosphoramide --- synthons --- supramolecular motifs --- n/a --- host-guest chemistry --- host-guest interaction --- metal-organic cage --- N,N',N",N‴-Tetraisopropylpyrophosphoramide