Spin‐Crossover Molecules on Surfaces: From Isolated Molecules to Ultrathin Films

Abstract Molecular spintronics seeks to use single or few molecules as functional building blocks for spintronic applications, directly relying on molecular properties or properties of interfaces between molecules and inorganic electrodes. Spin‐crossover molecules (SCMs) are one of the most promising classes of candidates for molecular spintronics due to their bistability deriving from the existence of two spin states that can be reversibly switched by temperature, light, electric fields, etc. Building devices based on single or few molecules would entail connecting the molecule(s) with solid surfaces and understanding the fundamental behavior of the resulting assemblies. Herein, the investigations of SCMs on solid surfaces, ranging from isolated single molecules (submonolayers) to ultrathin films (mainly in the sub‐10 nm range) are summarized. The achievements, challenges and prospects in this field are highlighted.