Chemically induced rearrangements of amphifunctional molecules have been demonstrated using strong nonuniform electric fields (10 8-10 10 V/m) induced in the vicinity of nanoscale asperities. Electrostatic interactions utilizing these rearrangements of alkylthiolates assembled on Au(111) result in the nanopatterning of raised nanostructure (1.5-9 nm high, 15-100 nm wide) arrays on a second time scale by manipulating an atomic force microscope (AFM) tip above the monolayer. It is suspected that, as a result of the oxidative cleavage initiated by a weak bias of the tip, the S end of the alkylthiolate chain carrying a sulfenium cation is attracted to the (lifting) tip, forming bi-and higher-layer structures in the vicinity of the tip apex. Stabilization of the multiplelayered structures is accomplished via mutual attraction and entanglement of hydrocarbon chains. The rearrangements suggest a novel and general approach for nanoscale architecture in self-assembled systems. Water condensation is shown to have a major influence on electric charge transport and nanostructure formation in polymer-, and semiconductor-thin-film surfaces in the proximity of a biased Atomic Force Microscope (AFM) tip. The water forms a meniscus bridge between the AFM tip and the surface to form a three-component system comprised of the AFM tip, water meniscus, and the surface. The associated electric field in the meniscus is spatially non-uniform and has a magnitude of the order of 10 8-10 10