The design of two-dimensional molecular self-assemblies [1] offers a powerful way to fine tune the properties of surfaces. Tailoring functional monolayers is therefore highly attractive for a range of potential nanotechnological applications, for example, in molecular electronics and photonics, bio-interface engineering, catalysis, or sensoring.[2] In this context, the design of responsive switchable monolayers,[3] that is, monolayers able to undergo ...