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Abstract:
Electrons tunneling from a scanning tunneling microscope tip to individual CO molecules on Cu(111) can cause their hopping from the surface to the tip if the bias exceeds a threshold of 2.4 V. Polarization- and time-resolved two-photon photoemission identifies the underlying elementary process as intermediate population of a CO 2π* -derived level, which exhibits an ultrashort lifetime of 0.8–5 fs. From an isotope effect of 2.7 - 0.5 + 0.3 it can be calculated that ≈ 0.05 % of the tunneling current transiently occupies this level while a desorption of the excited molecule occurs only in 5 × 10 - 9 of the cases.