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We discuss recent insights into the dynamical nature of electron- and photon-stimulated surface processes for chemisorbed molecules. Much of what we have learned stems from the correlation of quantum-resolved data on the products with the nature of the excited state(s), the excitation lifetimes, and the multidimensional potential energy surfaces. The latter are particularly important when two or more...
Photoexcited processes of NO and CO at photon energies ranging from 2.3 to 6.4 eV are investigated on Pt(111), Ni(111) and Pt(111)-Ge surface alloys by reflection-absorption infrared spectroscopy and resonance-enhanced multiphoton ionization. The branching between three competitive processes of desorption, recapture and dissociation upon laser irradiation is dramatically changed on the three surfaces...
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