Wodtke, Alec Michael

[["dc.bibliographiccitation.firstpage","17738"],["dc.bibliographiccitation.issue","44"],["dc.bibliographiccitation.journal","PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA"],["dc.bibliographiccitation.lastpage","17743"],["dc.bibliographiccitation.volume","110"],["dc.contributor.author","Bartels, Nils"],["dc.contributor.author","Golibrzuch, Kai"],["dc.contributor.author","Bartels, Christof"],["dc.contributor.author","Chen, L. I."],["dc.contributor.author","Auerbach, Daniel J."],["dc.contributor.author","Wodtke, Alec Michael"],["dc.contributor.author","Schaefer, Tim"],["dc.date.accessioned","2018-11-07T09:18:27Z"],["dc.date.available","2018-11-07T09:18:27Z"],["dc.date.issued","2013"],["dc.description.abstract","Molecules typically must point in specific relative directions to participate efficiently in energy transfer and reactions. For example, Forster energy transfer favors specific relative directions of each molecule's transition dipole [Forster T (1948) Ann Phys 2(1-2):55-75] and electron transfer between gas- phase molecules often depends on the relative orientation of orbitals [Brooks PR, et al. (2007) J Am Chem Soc 129(50):15572-15580]. Surface chemical reactions can be many orders of magnitude faster than their gas-phase analogs, a fact that underscores the importance of surfaces for catalysis. One reason surface reactions can be so fast is the labile change of oxidation state that commonly takes place upon adsorption, a process involving electron transfer between a solid metal and an approaching molecule. By transferring electrons to or from the adsorbate, the process of bond weakening and/or cleavage is initiated, chemically activating the reactant [Yoon B, et al. (2005) Science 307(5708):403-407]. Here, we show that the vibrational relaxation of NO-an example of electronically nonadiabatic energy transfer that is driven by an electron transfer event [Gadzuk JW (1983) J Chem Phys 79(12):6341-6348]-is dramatically enhanced when the molecule approaches an Au(111) surface with the N atom oriented toward the surface. This represents a rare opportunity to investigate the steric influences on an electron transfer reaction happening at a surface."],["dc.description.sponsorship","Alexander von Humboldt Foundation"],["dc.identifier.doi","10.1073/pnas.1312200110"],["dc.identifier.isi","000326243100038"],["dc.identifier.pmid","24127598"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/28416"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Natl Acad Sciences"],["dc.relation.issn","0027-8424"],["dc.title","Observation of orientation-dependent electron transfer in molecule-surface collisions"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.artnumber","064705"],["dc.bibliographiccitation.issue","6"],["dc.bibliographiccitation.journal","The Journal of Chemical Physics"],["dc.bibliographiccitation.volume","137"],["dc.contributor.author","Cooper, Russell"],["dc.contributor.author","Li, Zhisheng"],["dc.contributor.author","Golibrzuch, Kai"],["dc.contributor.author","Bartels, Christof"],["dc.contributor.author","Rahinov, Igor"],["dc.contributor.author","Auerbach, Daniel J."],["dc.contributor.author","Wodtke, Alec Michael"],["dc.date.accessioned","2018-11-07T09:07:12Z"],["dc.date.available","2018-11-07T09:07:12Z"],["dc.date.issued","2012"],["dc.description.abstract","We describe a method to obtain absolute vibrational excitation probabilities of molecules scattering from a surface based on measurements of the rotational state, scattering angle, and temporal distributions of the scattered molecules and apply this method to the vibrational excitation of NO scattering from Au(111). We report the absolute excitation probabilities to the v = 1 and v = 2 vibrational states, rotational excitation distributions, and final scattering angle distributions for a wide range of incidence energies and surface temperatures. In addition to demonstrating the methodology for obtaining absolute scattering probabilities, these results provide an excellent benchmark for theoretical calculations of molecule-surface scattering. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4738596]"],["dc.description.sponsorship","Alexander von Humboldt Foundation"],["dc.identifier.doi","10.1063/1.4738596"],["dc.identifier.isi","000308048700052"],["dc.identifier.pmid","22897300"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/11562"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/25737"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Inst Physics"],["dc.relation.issn","1089-7690"],["dc.relation.issn","0021-9606"],["dc.rights","Goescholar"],["dc.rights.uri","https://goescholar.uni-goettingen.de/licenses"],["dc.title","On the determination of absolute vibrational excitation probabilities in molecule-surface scattering: Case study of NO on Au(111)"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dc.type.version","submitted_version"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","8153"],["dc.bibliographiccitation.issue","18"],["dc.bibliographiccitation.journal","Physical Chemistry Chemical Physics"],["dc.bibliographiccitation.lastpage","8162"],["dc.bibliographiccitation.volume","13"],["dc.contributor.author","Matsiev, Daniel"],["dc.contributor.author","Li, Zhisheng"],["dc.contributor.author","Cooper, Russell"],["dc.contributor.author","Rahinov, Igor"],["dc.contributor.author","Bartels, Christof"],["dc.contributor.author","Auerbach, Daniel J."],["dc.contributor.author","Wodtke, Alec Michael"],["dc.date.accessioned","2018-11-07T09:01:53Z"],["dc.date.available","2018-11-07T09:01:53Z"],["dc.date.issued","2011"],["dc.description.abstract","Here we extend a recently introduced state-to-state kinetic model describing single-and multi-quantum vibrational excitation of molecular beams of NO scattering from a Au(111) metal surface. We derive an analytical expression for the rate of electronically non-adiabatic vibrational energy transfer, which is then employed in the analysis of the temperature dependence of the kinetics of direct overtone and two-step sequential energy transfer mechanisms. We show that the Arrhenius surface temperature dependence for vibrational excitation probability reported in many previous studies emerges as a low temperature limit of a more general solution that describes the approach to thermal equilibrium in the limit of infinite interaction time and that the pre-exponential term of the Arrhenius expression can be used not only to distinguish between the direct overtone and sequential mechanisms, but also to deduce their relative contributions. We also apply the analytical expression for the vibrational energy transfer rates introduced in this work to the full kinetic model and obtain an excellent fit to experimental data, the results of which show how to extract numerical values of the molecule-surface coupling strength and its fundamental properties."],["dc.identifier.doi","10.1039/c0cp01418d"],["dc.identifier.isi","000289954300010"],["dc.identifier.pmid","21046047"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/8707"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/24540"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Royal Soc Chemistry"],["dc.relation.issn","1463-9076"],["dc.rights","Goescholar"],["dc.rights.uri","https://goescholar.uni-goettingen.de/licenses"],["dc.title","On the temperature dependence of electronically non-adiabatic vibrational energy transfer in molecule-surface collisions"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.artnumber","044701"],["dc.bibliographiccitation.issue","4"],["dc.bibliographiccitation.journal","The Journal of Chemical Physics"],["dc.bibliographiccitation.volume","140"],["dc.contributor.author","Golibrzuch, Kai"],["dc.contributor.author","Shirhatti, Pranav R."],["dc.contributor.author","Rahinov, Igor"],["dc.contributor.author","Kandratsenka, Alexander"],["dc.contributor.author","Auerbach, Daniel J."],["dc.contributor.author","Wodtke, Alec Michael"],["dc.contributor.author","Bartels, Christof"],["dc.date.accessioned","2018-11-07T09:45:00Z"],["dc.date.available","2018-11-07T09:45:00Z"],["dc.date.issued","2014"],["dc.description.abstract","We present a combined experimental and theoretical study of NO(v = 3 -> 3, 2, 1) scattering from a Au(111) surface at incidence translational energies ranging from 0.1 to 1.2 eV. Experimentally, molecular beam-surface scattering is combined with vibrational overtone pumping and quantum-state selective detection of the recoiling molecules. Theoretically, we employ a recently developed first-principles approach, which employs an Independent Electron Surface Hopping (IESH) algorithm to model the nonadiabatic dynamics on a Newns-Anderson Hamiltonian derived from density functional theory. This approach has been successful when compared to previously reported NO/Au scattering data. The experiments presented here show that vibrational relaxation probabilities increase with incidence energy of translation. The theoretical simulations incorrectly predict high relaxation probabilities at low incidence translational energy. We show that this behavior originates from trajectories exhibiting multiple bounces at the surface, associated with deeper penetration and favored (N-down) molecular orientation, resulting in a higher average number of electronic hops and thus stronger vibrational relaxation. The experimentally observed narrow angular distributions suggest that mainly single-bounce collisions are important. Restricting the simulations by selecting only single-bounce trajectories improves agreement with experiment. The multiple bounce artifacts discovered in this work are also present in simulations employing electronic friction and even for electronically adiabatic simulations, meaning they are not a direct result of the IESH algorithm. This work demonstrates how even subtle errors in the adiabatic interaction potential, especially those that influence the interaction time of the molecule with the surface, can lead to an incorrect description of electronically nonadiabatic vibrational energy transfer in molecule-surface collisions. (C) 2014 AIP Publishing LLC."],["dc.description.sponsorship","Alexander von Humboldt foundation"],["dc.identifier.doi","10.1063/1.4861660"],["dc.identifier.isi","000331211700071"],["dc.identifier.pmid","25669561"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/11564"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/34519"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Inst Physics"],["dc.relation.issn","1089-7690"],["dc.relation.issn","0021-9606"],["dc.rights","Goescholar"],["dc.rights.uri","https://goescholar.uni-goettingen.de/licenses"],["dc.title","The importance of accurate adiabatic interaction potentials for the correct description of electronically nonadiabatic vibrational energy transfer: A combined experimental and theoretical study of NO(v=3) collisions with a Au(111) surface"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dc.type.version","submitted_version"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","1929"],["dc.bibliographiccitation.issue","10-12"],["dc.bibliographiccitation.journal","ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS"],["dc.bibliographiccitation.lastpage","1949"],["dc.bibliographiccitation.volume","229"],["dc.contributor.author","Golibrzuch, Kai"],["dc.contributor.author","Baraban, Joshua H."],["dc.contributor.author","Shirhatti, Pranav R."],["dc.contributor.author","Werdecker, Joern"],["dc.contributor.author","Bartels, Christof"],["dc.contributor.author","Wodtke, Alec Michael"],["dc.date.accessioned","2018-11-07T10:02:47Z"],["dc.date.available","2018-11-07T10:02:47Z"],["dc.date.issued","2015"],["dc.description.abstract","We present quantum-state and velocity resolved experiments for molecular beam scattering of acetylene (C2H2) from a single-crystal Au(111) surface, observations that reveal translational, rotational and vibrational inelasticity. The experiments are made possible by a novel (1 + 2) REMPI scheme for acetylene. The scattered molecules' velocity distributions as well as their ro-vibrational quantum-state distributions depend on the translational energy of incidence, E-I providing unambiguous evidence that the scattered molecules were not trapped and equilibrated on the surface. We report the E-I-dependence of the collisional excitation of one and two quanta of the trans-bending vibrational mode, nu(4) = 0 -> 1, 2, which is consistent with a mechanism involving conversion of incidence translational energy to acetylene vibration. Rotationally resolved velocity measurements on scattered acetylene in its ground vibrational state are interpreted in terms of orientation-dependent rotational and vibrational excitation probabilities."],["dc.description.sponsorship","Alexander von Humboldt foundation"],["dc.identifier.doi","10.1515/zpch-2015-0606"],["dc.identifier.isi","000364609000025"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/38300"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Walter De Gruyter Gmbh"],["dc.relation.issn","0942-9352"],["dc.title","Observation of Translation-to-Vibration Excitation in Acetylene Scattering from Au(111): A REMPI Based Approach"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","14722"],["dc.bibliographiccitation.issue","26"],["dc.bibliographiccitation.journal","The Journal of Physical Chemistry C"],["dc.bibliographiccitation.lastpage","14727"],["dc.bibliographiccitation.volume","119"],["dc.contributor.author","Werdecker, Joern"],["dc.contributor.author","Shirhatti, Pranav R."],["dc.contributor.author","Golibrzuch, Kai"],["dc.contributor.author","Bartels, Christof"],["dc.contributor.author","Wodtke, Alec Michael"],["dc.contributor.author","Harding, Dan J."],["dc.date.accessioned","2018-11-07T09:54:46Z"],["dc.date.available","2018-11-07T09:54:46Z"],["dc.date.issued","2015"],["dc.description.abstract","Molecular beam surface scattering is used to compare vibrational excitation of N-2 molecules in collisions with clean Pt(111) and Au(111) surfaces under UHV conditions. Direct single-bounce collisions are dominant under all conditions of this work, as evidenced by narrow specular angular scattering distributions and translational incidence energy dependent rotational temperatures. N-2(v = 0 -> 1) vibrational excitation is observed for Pt(111), but not Au(111). The excitation probabilities, ranging from to similar to 10(-3), follow an Arrhenius surface temperature dependence and increase with translational incidence energy with zero threshold. The observations are the typical fingerprint of nonadiabatic vibrational excitation due to an electron mediated excitation mechanism, identified in previous work on NO and CO scattering from electron affinity of the N-2 molecule (EA = -2.3 eV) makes this observation surprising and we discuss possible mechanisms."],["dc.description.sponsorship","Alexander von Humboldt Foundation"],["dc.identifier.doi","10.1021/acs.jpcc.5b00202"],["dc.identifier.isi","000357623500029"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/36609"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","1932-7447"],["dc.title","Electronically Nonadiabatic Vibrational Excitation of N-2 Scattered from Pt(111)"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.artnumber","124704"],["dc.bibliographiccitation.issue","12"],["dc.bibliographiccitation.journal","The Journal of Chemical Physics"],["dc.bibliographiccitation.volume","141"],["dc.contributor.author","Shirhatti, Pranav R."],["dc.contributor.author","Werdecker, Joern"],["dc.contributor.author","Golibrzuch, Kai"],["dc.contributor.author","Wodtke, Alec Michael"],["dc.contributor.author","Bartels, Christof"],["dc.date.accessioned","2018-11-07T09:35:03Z"],["dc.date.available","2018-11-07T09:35:03Z"],["dc.date.issued","2014"],["dc.description.abstract","We investigated the translational incidence energy (E-i) and surface temperature (T-s) dependence of CO vibrational excitation upon scattering from a clean Au(111) surface. We report absolute v=0 -> 1 excitation probabilities for E-i between 0.16 and 0.84 eV and T-s between 473 and 973 K. This is now only the second collision system where such comprehensive measurements are available - the first is NO on Au(111). For CO on Au(111), vibrational excitation occurs via direct inelastic scattering through electron hole pair mediated energy transfer - it is enhanced by incidence translation and the electronically non-adiabatic coupling is about 5 times weaker than in NO scattering from Au(111). Vibrational excitation via the trapping desorption channel dominates at E-i = 0.16 eV and quickly disappears at higher E-i. (C) 2014 AIP Publishing LLC."],["dc.description.sponsorship","Alexander von Humboldt Foundation"],["dc.identifier.doi","10.1063/1.4894814"],["dc.identifier.isi","000342844100058"],["dc.identifier.pmid","25273458"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/11565"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/32306"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Inst Physics"],["dc.relation.issn","1089-7690"],["dc.relation.issn","0021-9606"],["dc.rights","Goescholar"],["dc.rights.uri","https://goescholar.uni-goettingen.de/licenses"],["dc.title","Electron hole pair mediated vibrational excitation in CO scattering from Au(111): Incidence energy and surface temperature dependence"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dc.type.version","submitted_version"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","10027"],["dc.bibliographiccitation.issue","18"],["dc.bibliographiccitation.journal","The Journal of Physical Chemistry C"],["dc.bibliographiccitation.lastpage","10033"],["dc.bibliographiccitation.volume","122"],["dc.contributor.author","Steinsiek, Christoph"],["dc.contributor.author","Shirhatti, Pranav R."],["dc.contributor.author","Geweke, Jan"],["dc.contributor.author","Bartels, Christof"],["dc.contributor.author","Wodtke, Alec Michael"],["dc.date.accessioned","2020-12-10T15:22:45Z"],["dc.date.available","2020-12-10T15:22:45Z"],["dc.date.issued","2018"],["dc.identifier.doi","10.1021/acs.jpcc.8b01950"],["dc.identifier.eissn","1932-7455"],["dc.identifier.issn","1932-7447"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/73522"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-354"],["dc.relation","SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen"],["dc.relation","SFB 1073 | Topical Area A | A04 Kontrolle von Energiedissipation an Oberflächen mittels einstellbaren Eigenschaften von Grenzflächen"],["dc.title","Work Function Dependence of Vibrational Relaxation Probabilities: NO( v = 2) Scattering from Ultrathin Metallic Films of Ag/Au(111)"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.artnumber","054709"],["dc.bibliographiccitation.issue","5"],["dc.bibliographiccitation.journal","The Journal of Chemical Physics"],["dc.bibliographiccitation.volume","145"],["dc.contributor.author","Geweke, Jan"],["dc.contributor.author","Shirhatti, Pranav R."],["dc.contributor.author","Rahinov, Igor"],["dc.contributor.author","Bartels, Christof"],["dc.contributor.author","Wodtke, Alec Michael"],["dc.date.accessioned","2018-11-07T10:10:17Z"],["dc.date.available","2018-11-07T10:10:17Z"],["dc.date.issued","2016"],["dc.description.abstract","In this work we seek to examine the nature of collisional energy transfer between HCl and Au(111) for nonreactive scattering events that sample geometries near the transition state for dissociative adsorption by varying both the vibrational and translational energy of the incident HCl molecules in the range near the dissociation barrier. Specifically, we report absolute vibrational excitation probabilities for HCl(v = 0 -> 1) and HCl(v = 1 -> 2) scattering from clean Au(111) as a function of surface temperature and incidence translational energy. The HCl(v = 2 -> 3) channel could not be observed-presumably due to the onset of dissociation. The excitation probabilities can be decomposed into adiabatic and nonadiabatic contributions. We find that both contributions strongly increase with incidence vibrational state by a factor of 24 and 9, respectively. This suggests that V-T as well as V-EHP coupling can be enhanced near the transition state for dissociative adsorption at a metal surface. We also show that previously reported HCl(v 0 -> 1) excitation probabilities [Q. Ran et al., Phys. Rev. Lett. 98, 237601 (2007)]-50 times smaller than those reported here-were influenced by erroneous assignment of spectroscopic lines used in the data analysis. Published by AIP Publishing."],["dc.identifier.doi","10.1063/1.4959968"],["dc.identifier.isi","000381680000043"],["dc.identifier.pmid","27497574"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/39820"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Inst Physics"],["dc.relation.issn","1089-7690"],["dc.relation.issn","0021-9606"],["dc.title","Vibrational energy transfer near a dissociative adsorption transition state: State-to-state study of HCl collisions at Au(111)"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","7091"],["dc.bibliographiccitation.issue","32"],["dc.bibliographiccitation.journal","The Journal of Physical Chemistry A"],["dc.bibliographiccitation.lastpage","7101"],["dc.bibliographiccitation.volume","117"],["dc.contributor.author","Golibrzuch, Kai"],["dc.contributor.author","Kandratsenka, Alexander"],["dc.contributor.author","Rahinov, Igor"],["dc.contributor.author","Cooper, Russell"],["dc.contributor.author","Auerbach, Daniel J."],["dc.contributor.author","Wodtke, Alec Michael"],["dc.contributor.author","Bartels, Christof"],["dc.date.accessioned","2018-11-07T09:21:14Z"],["dc.date.available","2018-11-07T09:21:14Z"],["dc.date.issued","2013"],["dc.description.abstract","We measured absolute probabilities for vibrational excitation of NO(v = 0) molecules in collisions with a Au(111) surface at an incidence energy of translation of 0.4 eV and surface temperatures between 300 and 1100 K. In addition to previously reported excitation to v = 1 and v = 2, we observed excitation to v = 3. The excitation probabilities exhibit an Arrhenius dependence on surface temperature, indicating that the dominant excitation mechanism is nonadiabatic coupling to electron hole pairs. The experimental data are analyzed in terms of a recently introduced kinetic model, which was extended to include four vibrational states. We describe a subpopulation decomposition of the kinetic model, which allows us to examine vibrational population transfer pathways. The analysis indicates that sequential pathways (v = 0 -> 1 -> 2 and v = 0 -> 1 -> 2 -> 3) alone cannot adequately describe production of v = 2 or 3. In addition, we performed first-principles molecular dynamics calculations that incorporate electronically nonadiabatic dynamics via an independent electron surface hopping (IESH) algorithm, which requires as input an ab initio potential energy hypersurface (PES) and nonadiabatic coupling matrix elements, both obtained from density functional theory (DFT). While the LESH-based simulations reproduce the v = 1 data well, they slightly underestimate the excitation probabilities for v = 2, and they significantly underestimate those for v = 3. Furthermore, this implementation of IESH appears to overestimate the importance of sequential energy transfer pathways. We make several suggestions concerning ways to improve this IESH-based model."],["dc.description.sponsorship","Alexander von Humboldt foundation"],["dc.identifier.doi","10.1021/jp400313b"],["dc.identifier.isi","000323300800020"],["dc.identifier.pmid","23947910"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/11561"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/29068"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","1089-5639"],["dc.rights","Goescholar"],["dc.rights.uri","https://goescholar.uni-goettingen.de/licenses"],["dc.title","Experimental and Theoretical Study of Multi-Quantum Vibrational Excitation: NO(v=0 -> 1,2,3) in Collisions with Au(111)"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dc.type.version","submitted_version"],["dspace.entity.type","Publication"]]