“…Metal–polypyridyl complexes are potentially useful for a variety of photophysical, electrochemical, and spectro-electrochemical applications. − Particular beneficial aspects of these systems are their structural tunability and flexible choice of metal ions, which also affect the positions of the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) states as well as the respective energy gap. , Accordingly, the solubility, stability, redox potential and kinetics, and optical characteristics of metal–polypyridyl complexes can be controlled and manipulated in a desired way. For these reasons, functional polypyridyl complexes have found great utility in the design of metallo-supramolecular architectures as well as active elements in photodynamic therapy, , catalysts, , sensing modules, , components of nonvolatile memory devices, , photochromic or electrochromic elements in solid-state devices, , and media for charge and spin transport. , Most of these applications rely on covalent or noncovalent assembly of polypyridyl complexes on suitably functionalized solid substrates, which provide aligned and densely packed nanometric architectures, with a much better control over molecular orientation, integrity, and functionality compared to the liquid media case. , Such molecular assemblies can also serve as a basis for creating application-oriented novel multifunctional materials and also act as a versatile tool box for discerning structure–property relationship, which is an essential requirement for modeling a variety of interfacial phenomena.…”