  The interaction of the strong electron-acceptor tetracyanoethylene (TCNE)
with the Cu(100) surface has been studied with scanning tunneling microscopy
experiments and first-principles density functional theory calculations. We
compare two different adsorption models with the experimental results and show
that the molecular self-assembly is caused by a strong structural modification
of the Cu(100) surface rather than the formation of a coordination network by
diffusing Cu adatoms. Surface atoms become highly buckled and the chemisorption
of TCNE is accompanied by a partial charge-transfer.
