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.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.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","8750"],["dc.bibliographiccitation.issue","36"],["dc.bibliographiccitation.journal","The Journal of Physical Chemistry A"],["dc.bibliographiccitation.lastpage","8760"],["dc.bibliographiccitation.volume","117"],["dc.contributor.author","Golibrzuch, Kai"],["dc.contributor.author","Shirhatti, Pranav R."],["dc.contributor.author","Altschaeffel, Jan"],["dc.contributor.author","Rahinov, Igor"],["dc.contributor.author","Auerbach, Daniel J."],["dc.contributor.author","Wodtke, Alec Michael"],["dc.contributor.author","Bartels, Christof"],["dc.date.accessioned","2018-11-07T09:19:55Z"],["dc.date.available","2018-11-07T09:19:55Z"],["dc.date.issued","2013"],["dc.description.abstract","Translational motion is believed to be a spectator degree of freedom in electronically nonadiabatic vibrational energy transfer between molecules and metal surfaces, but the experimental evidence available to support this view is limited. In this work, we have experimentally determined the translational inelasticity in collisions of NO molecules with a single-crystal Au(111) surface-a system with strong electronic nonadiabaticity. State-to-state molecular beam surface scattering was combined with an IR-UV double resonance scheme to obtain high-resolution time-of-flight data. The measurements include vibrationally elastic collisions (v = 3 -> 3, 2 -> 2) as well as collisions where one or two quanta of molecular vibration are excited (2 -> 3, 2 -> 4) or de-excited (2 -> 1, 3 -> 2, 3 -> 1). In addition, we have carried out comprehensive measurements of the effects of rotational excitation on the translational energy of the scattered molecules. We find that under all conditions of this work, the NO molecules lose a large fraction (similar to 0.45) of their incidence translational energy to the surface. Those molecules that undergo vibrational excitation (relaxation) during the collision recoil slightly slower (faster) than vibrationally elastically scattered molecules. The amount of translational energy change depends on the surface temperature. The translation-to-rotation coupling, which is well-known for v = 0 -> 0 collisions, is found to be significantly weaker for vibrationally inelastic than elastic channels. Our results clearly show that the spectator view of the translational motion in electronically nonadiabatic vibrational energy transfer between NO and Au(111) is only approximately correct."],["dc.description.sponsorship","Alexander von Humboldt foundation"],["dc.identifier.doi","10.1021/jp403382b"],["dc.identifier.isi","000330145400028"],["dc.identifier.pmid","23808714"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/28755"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","1089-5639"],["dc.title","State-to-State Time-of-Flight Measurements of NO Scattering from Au(111): Direct Observation of Translation-to-Vibration Coupling in Electronically Nonadiabatic Energy Transfer"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","1346"],["dc.bibliographiccitation.issue","7"],["dc.bibliographiccitation.journal","The Journal of Physical Chemistry Letters"],["dc.bibliographiccitation.lastpage","1350"],["dc.bibliographiccitation.volume","7"],["dc.contributor.author","Shirhatti, Pranav R."],["dc.contributor.author","Geweke, Jan"],["dc.contributor.author","Steinsiek, Christoph"],["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","2018-11-07T10:15:36Z"],["dc.date.available","2018-11-07T10:15:36Z"],["dc.date.issued","2016"],["dc.description.abstract","We report zero-coverage reaction probabilities (S-0) for HCl dissociative adsorption on Au(111) obtained by the seeded molecular beam hot-nozzle method. For measurements at normal incidence with mean translational energies ranging from 0.94 to 2.56 eV (nozzle temperatures 296 to 1060 K), S-0 increased from 6 x 10(-6) to 2 x 10(-2). S-0 also increased with increasing nozzle temperature for fixed incidence energy associated with the motion normal to the surface. Accounting for the influence of the vibrational state population and translational energy distributions in the incident beam, we are able to compare the experimental results to recent theoretical predictions. These calculations, performed employing 6-D quantum dynamics on an electronically adiabatic potential energy surface obtained using density functional theory at the level of the generalized gradient approximation and the static surface approximation, severely overestimate the reaction probabilities when compared with our experimental results. We discuss some possible reasons for this large disagreement."],["dc.identifier.doi","10.1021/acs.jpclett.6b00289"],["dc.identifier.isi","000373867600041"],["dc.identifier.pmid","26990513"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/40841"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","1948-7185"],["dc.title","Activated Dissociation of HCl on Au(111)"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.journal","ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY"],["dc.bibliographiccitation.volume","241"],["dc.contributor.author","Wodtke, Alec Michael"],["dc.contributor.author","Cooper, Russell"],["dc.contributor.author","Bartels, Christof"],["dc.contributor.author","Schaefer, Tim"],["dc.contributor.author","Larue, Jerry"],["dc.contributor.author","Li, Zhisheng"],["dc.contributor.author","Auerbach, Daniel J."],["dc.date.accessioned","2018-11-07T08:58:01Z"],["dc.date.available","2018-11-07T08:58:01Z"],["dc.date.issued","2011"],["dc.identifier.isi","000291982803915"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/23542"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.publisher.place","Washington"],["dc.relation.conference","241st National Meeting and Exposition of the American-Chemical-Society (ACS)"],["dc.relation.eventlocation","Anaheim, CA"],["dc.relation.issn","0065-7727"],["dc.title","Energy transfer at metal surfaces beyond the Born-Oppenheimer approximation"],["dc.type","conference_abstract"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","592"],["dc.bibliographiccitation.issue","6"],["dc.bibliographiccitation.journal","Nature Chemistry"],["dc.bibliographiccitation.lastpage","598"],["dc.bibliographiccitation.volume","10"],["dc.contributor.author","Shirhatti, Pranav R."],["dc.contributor.author","Rahinov, Igor"],["dc.contributor.author","Golibrzuch, Kai"],["dc.contributor.author","Werdecker, Jörn"],["dc.contributor.author","Geweke, Jan"],["dc.contributor.author","Altschäffel, Jan"],["dc.contributor.author","Kumar, Sumit"],["dc.contributor.author","Auerbach, Daniel J."],["dc.contributor.author","Bartels, Christof"],["dc.contributor.author","Wodtke, Alec M."],["dc.date.accessioned","2020-12-10T18:09:54Z"],["dc.date.available","2020-12-10T18:09:54Z"],["dc.date.issued","2018"],["dc.identifier.doi","10.1038/s41557-018-0003-1"],["dc.identifier.eissn","1755-4349"],["dc.identifier.issn","1755-4330"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/73797"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-354"],["dc.title","Observation of the adsorption and desorption of vibrationally excited molecules on a metal surface"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","3268"],["dc.bibliographiccitation.issue","6"],["dc.bibliographiccitation.journal","The Journal of Physical Chemistry C"],["dc.bibliographiccitation.lastpage","3272"],["dc.bibliographiccitation.volume","119"],["dc.contributor.author","Krueger, Bastian Christopher"],["dc.contributor.author","Bartels, Nils"],["dc.contributor.author","Bartels, Christof"],["dc.contributor.author","Kandratsenka, Alexander"],["dc.contributor.author","Tully, John C."],["dc.contributor.author","Wodtke, Alec Michael"],["dc.contributor.author","Schaefer, Tim"],["dc.date.accessioned","2018-11-07T10:00:57Z"],["dc.date.available","2018-11-07T10:00:57Z"],["dc.date.issued","2015"],["dc.description.abstract","During a collision of highly vibrationally excited NO with a Au(111) surface, the molecule can lose a large fraction of its vibrational energy into electronic excitation of the metal. This process violates the Born-Oppenheimer approximation and represents a major challenge to theories of molecule-surface interaction. Two ab initio approaches to this problem, one using independent electron surface hopping (IESH) and the other electronic friction, previously reported good agreement with the limited available data on multiquantum vibrational relaxation; however, at that time only experiments for NO(v(i) = 15) at an incidence translational energy of E-i = 0.05 eV were available. In this work, we report a comparison of recently reported experiments characterizing the multiquantum vibrational relaxation of NO on Au(111) for a wider range of incidence translational and vibrational energies to IESH and molecular dynamics with electronic friction (MDEF) calculations for these conditions. Both theories fail to explain the large amount of vibrational energy transferred from NO to the solid."],["dc.description.sponsorship","Alexander von Humboldt Foundation; U.S. DOE-BES [DE-FG02-05ER15677]"],["dc.identifier.doi","10.1021/acs.jpcc.5b00388"],["dc.identifier.isi","000349578400040"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/37915"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","1932-7447"],["dc.title","NO Vibrational Energy Transfer on a Metal Surface: Still a Challenge to First-Principles Theory"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]