Abstract
Polyoxometalates (POMs) have attracted much attention in the development of data storage devices with new nanophysics. Numerous studies can be found on their integration into charge-based and resistive types of memory. However, the question of whether the POM behaves as a molecular capacitor or as a molecular memristor remains largely unexplored. In this Article, we clarify this fundamental question by placing the individual electronic properties of POMs in the context of their chemical and technical environment. By controlling the charge stabilization of reduced POMs through chemical functionalization, choice of countercations, surface properties, and intermolecular interactions, various physical switching mechanisms can be realized, demonstrating the remarkable uniqueness of these molecular oxides.