Cleverly designed molecular building blocks provide chemists with the tools
of a powerful molecular-scale construction set. They enable them to engine
er materials that have a predictable order and useful solid-state propertie
s. Hence, it is in the realm of supramolecular chemistry to follow a strate
gy for synthesizing materials that combine a selected set of properties, fo
r instance from the areas of magnetism, photophysics and electronics. As a
possible approach, host-guest solids that are based on extended anionic, ho
mo- and bi-metallic oxalato-bridged transition-metal compounds with two- an
d three-dimensional connectivities are investigated. In particular, we repo
rt in detail about their structural properties and their multifunctional ch
aracteristics in the area of molecular magnetism and photophysics.