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A quantitative structural investigation is reported, aimed at resolving theissue of whether substrate adatoms are incorporated into the monolayers formedby strong molecular electron acceptors deposited onto metallic electrodes. Acombination of normal-incidence X-ray standing waves, low energy electrondiffraction, scanning tunnelling microscopy and X-ray photoelectronspectroscopy measurements demonstrate that the systems TCNQ and F4TCNQ onAg(100) lie at the boundary between these two possibilities and thus representideal model systems with which to study this effect. A room-temperaturecommensurate phase of adsorbed TCNQ is found not to involve Ag adatoms, but toadopt an inverted bowl configuration, long predicted but not previouslyidentified experimentally. By contrast, a similar phase of adsorbed F4TCNQ doeslead to Ag adatom incorporation in the overlayer, the cyano endgroups of themolecule being twisted relative to the planar quinoid ring. Density functionaltheory (DFT) calculations show that this behaviour is consistent with theadsorption energetics. Annealing of the commensurate TCNQ overlayer phase leadsto an incommensurate phase that does appear to incorporate Ag adatoms. Ourresults indicate that the inclusion (or exclusion) of metal atoms into theorganic monolayers is the result of both thermodynamic and kinetic factors.

Thermodynamic Driving Forces for Substrate Atom Extraction by Adsorption of Strong Electron Acceptor Molecules