Theoretical Description of Hydrogen Atom Scattering off Noble Metals

Janke, Svenja Maria

dc.contributor.advisor	Wodtke, Alec Prof. Dr.
dc.contributor.author	Janke, Svenja Maria
dc.date.accessioned	2016-07-01T09:01:12Z
dc.date.available	2016-07-01T09:01:12Z
dc.date.issued	2016-07-01
dc.identifier.uri	http://hdl.handle.net/11858/00-1735-0000-0028-87A3-4
dc.identifier.uri	http://dx.doi.org/10.53846/goediss-5714
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	Theoretical Description of Hydrogen Atom Scattering off Noble Metals	de
dc.type	doctoralThesis	de
dc.contributor.referee	Wodtke, Alec Prof. Dr.
dc.date.examination	2016-05-13
dc.description.abstracteng	I have constructed a full-dimensional potential energy surface (PES) for a H atom interacting with a Au(111) surface by fitting the analytic form of the Effective Medium Theory to density functional theory (DFT) energies. The fit used energies of the H-Au system with the Au atoms at their relaxed lattice positions as well as configurations with the Au atoms displaced from these positions. The procedure provides an accurate treatment for displacements of Au atoms and compares well to DFT energies for scattering of H atoms obtained from ab initio molecular dynamics (AIMD). In adiabatic molecular dynamics simulation, the PES is capable of reproducing the energy loss behavior of AIMD. The effective medium theory also provides the background electron density which makes it possible to treat the excitation of energetically low lying electron hole pairs self-consistently in the frame of local density friction approximation. I have tested various incidence conditions for H scattering from Au(111) and find that in all cases, the energy loss by electron hole pair excitation is by far the most efficient pathway and dominates the scattering behavior and influences the adsorption mechanism significantly. Comparison to experiment confirms that energy loss to electron hole pairs is the dominant energy dissipation pathway. Molecular dynamics simulations including nonadiabatic effects for multiple incidence conditions are in very good agreement with experiment. Furthermore, the theory offers an explanation for the apparent lack of an isotope effect observed experimentally. I consider the effect of changes in the electron density and the inclusion of surface reconstruction and find the results are not much altered. For molecular dynamics simulations and fitting, I used a self-written program package to which I contributed substantially.	de
dc.contributor.coReferee	Kroes, Geert-Jan Prof. Dr.
dc.contributor.thirdReferee	Schroeder, Jörg Prof. Dr.
dc.contributor.thirdReferee	Mata, Ricardo A. Prof. Dr.
dc.contributor.thirdReferee	Schwarzer, Dirk Prof. Dr.
dc.contributor.thirdReferee	Schäfer, Tim Dr.
dc.subject.eng	Gold	de
dc.subject.eng	potential energy surface	de
dc.subject.eng	H on Au(111)	de
dc.subject.eng	molecular dynamics	de
dc.subject.eng	Effective Medium Theory	de
dc.subject.eng	comparison to experiment	de
dc.subject.eng	electronic friction	de
dc.subject.eng	scattering	de
dc.subject.eng	Au(111) surface reconstruction	de
dc.subject.eng	density functional theory	de
dc.subject.eng	nonadiabatic	de
dc.subject.eng	Hydrogen	de
dc.identifier.urn	urn:nbn:de:gbv:7-11858/00-1735-0000-0028-87A3-4-8
dc.affiliation.institute	Fakultät für Chemie	de
dc.subject.gokfull	Chemie (PPN62138352X)	de
dc.identifier.ppn	862513189

Dateien

Name:Janke_Dissertation2016.pdf

Größe:28.73Mb

Format:PDF

Öffnen

Name:: Janke_Dissertation2016.pdf
Größe:: 28.73Mb
Format:: PDF

Öffnen

Das Dokument erscheint in:

Fakultät für Chemie (inkl. GAUSS) [702]

Zur Kurzanzeige