The Dynamics of Highly Vibrationally Excited CO Scattered from Metal Surfaces

Wagner, Roman Jonathan Viktor

dc.contributor.advisor	Wodtke, Alec Prof. Dr.
dc.contributor.author	Wagner, Roman Jonathan Viktor
dc.date.accessioned	2019-04-26T08:40:28Z
dc.date.available	2019-04-26T08:40:28Z
dc.date.issued	2019-04-26
dc.identifier.uri	http://hdl.handle.net/11858/00-1735-0000-002E-E619-C
dc.identifier.uri	http://dx.doi.org/10.53846/goediss-7411
dc.identifier.uri	http://dx.doi.org/10.53846/goediss-7411
dc.language.iso	eng	de
dc.publisher	Niedersächsische Staats- und Universitätsbibliothek Göttingen	de
dc.rights.uri	http://creativecommons.org/licenses/by-nc-nd/4.0/
dc.subject.ddc	540	de
dc.title	The Dynamics of Highly Vibrationally Excited CO Scattered from Metal Surfaces	de
dc.type	doctoralThesis	de
dc.contributor.referee	Wodtke, Alec M. Prof. Dr.
dc.date.examination	2019-04-09
dc.description.abstracteng	Supersonic molecular beams of highly vibrationally excited CO are scattered from atomically clean Au(111) and Ag(111) surfaces. Specifically, incident CO is prepared in the (v = 17, J = 0) state of the electronic ground state. Scattered molecules are detected quantum state-selectively by means of resonance-enhanced multi-photon ionization. Final vibrational state distributions and rotational state distributions are presented as well as time-of-flight distributions and angular distributions. Rotationally hot scattering products, narrow angular distributions, and final translational energies consistent with the Baule limit indicate a direct scattering mechanism. The vibrational relaxation probability of CO(v = 17) at Ag(111) is higher than that at Au(111). For both metals, the vibrational relaxation probability increases with incidence translational energy. The incidence translational energy dependence is more pronounced for Au(111) than for Ag(111). The comparison to previously studied molecule-surface systems—including two molecules (CO and NO), two surfaces (gold and silver), and various incidence vibrational excitations (ranging from v = 2 to v = 17)—reveals a unifying trend, according to which the vibrational relaxation probability depends on both the work function of the surface and the electron binding energy of the molecule. This strongly suggests that an electron transfer process is essential to the electronically non-adiabatic coupling between molecular vibration and electronic degrees of freedom of the surface. Thus, for a single-bounce collision event with a metal surface, the vibrational relaxation probability of a diatomic molecule can be predicted simply by evaluating energetic quantities characterizing the isolated molecule and surface. This allows easy identification of molecule-surface systems in which non-adiabatic surface dynamics are likely to be governed by electron transfer.	de
dc.contributor.coReferee	Schwarzer, Dirk Prof. Dr.
dc.contributor.thirdReferee	Behler, Jörg Prof. Dr.
dc.contributor.thirdReferee	Geil, Burkhard Prof. Dr.
dc.contributor.thirdReferee	Kitsopoulos, Theofanis N. Prof. Dr.
dc.contributor.thirdReferee	Troe, Jürgen Prof. Dr.
dc.subject.eng	Dynamics at Surfaces	de
dc.subject.eng	Molecular Beam Surface Scattering	de
dc.subject.eng	Energy Transfer	de
dc.subject.eng	Highly Vibrationally Excited CO	de
dc.subject.eng	Vibrational Relaxation	de
dc.subject.eng	Electron Transfer	de
dc.subject.eng	REMPI Spectroscopy	de
dc.subject.eng	Stark Deceleration	de
dc.identifier.urn	urn:nbn:de:gbv:7-11858/00-1735-0000-002E-E619-C-4
dc.affiliation.institute	Fakultät für Chemie	de
dc.subject.gokfull	Chemie (PPN62138352X)	de
dc.identifier.ppn	1666650609

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