Wodtke, Alec Michael

[["dc.bibliographiccitation.firstpage","12255"],["dc.bibliographiccitation.issue","50"],["dc.bibliographiccitation.journal","The Journal of Physical Chemistry A"],["dc.bibliographiccitation.lastpage","12262"],["dc.bibliographiccitation.volume","119"],["dc.contributor.author","Harding, Dan J."],["dc.contributor.author","Neugebohren, J."],["dc.contributor.author","Auerbach, Daniel J."],["dc.contributor.author","Kitsopoulos, T. N."],["dc.contributor.author","Wodtke, Alec Michael"],["dc.date.accessioned","2018-11-07T09:47:27Z"],["dc.date.available","2018-11-07T09:47:27Z"],["dc.date.issued","2015"],["dc.description.abstract","We present a new implementation of ion imaging for the study of surface scattering processes. The technique uses a combination of spatial ion imaging with laser slicing and delayed pulsed extraction. The scattering velocities of interest are parallel to the imaging plane, allowing speed and angular distributions to be extracted from a single image. The first results of direct scattering of N-2 from a clean, single-crystal Au(111) surface are reported, and the speed resolution is shown to be competitive with current state-of-the-art time-of-flight methods for velocity measurements while providing simultaneous measurements of in-plane angular distributions."],["dc.identifier.doi","10.1021/acs.jpca.5b06272"],["dc.identifier.isi","000366881000034"],["dc.identifier.pmid","26418228"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/35115"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.relation.issn","1089-5639"],["dc.title","Using Ion Imaging to Measure Velocity Distributions in Surface Scattering Experiments"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","1467"],["dc.bibliographiccitation.issue","9-11"],["dc.bibliographiccitation.journal","ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS"],["dc.bibliographiccitation.lastpage","1490"],["dc.bibliographiccitation.volume","227"],["dc.contributor.author","Janke, Svenja M."],["dc.contributor.author","Pavanello, Michele"],["dc.contributor.author","Kroes, Geert-Jan"],["dc.contributor.author","Auerbach, Daniel J."],["dc.contributor.author","Wodtke, Alec Michael"],["dc.contributor.author","Kandratsenka, Alexander"],["dc.date.accessioned","2018-11-07T09:17:57Z"],["dc.date.available","2018-11-07T09:17:57Z"],["dc.date.issued","2013"],["dc.description.abstract","We report an analytic potential energy surface (PES) based on several hundred DFT energies for H interacting with a Au(111) surface. Effective medium theory is used to fit the DFT data, which were obtained for the Au atoms held at their equilibrium positions. This procedure also provides an adequate treatment of the PES for displacements of Au atoms that occur during scattering of H atoms. The fitted PES is compared to DFT energies obtained from ab initio molecular dynamics trajectories. We present molecular dynamics simulations of energy and angle resolved scattering probabilities at five incidence angles at an incidence energy, E-i = 5 eV, and at a surface temperature, T-S = 10 K. Simple single bounce trajectories are important at all incidence conditions explored here. Double bounce events also make up a significant fraction of the scattering. A qualitative analysis of the double-bounce events reveals that most occur as collisions of an H-atom with two neighboring surface gold atoms. The energy losses observed are consistent with a simple binary collision model, transferring typically less than 150meV to the solid per bounce."],["dc.description.sponsorship","ANR-DFG-CHEMISTRY"],["dc.identifier.doi","10.1524/zpch.2013.0411"],["dc.identifier.isi","000327861100017"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/10834"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/28295"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Walter De Gruyter Gmbh"],["dc.relation.issn","0942-9352"],["dc.rights","Goescholar"],["dc.rights.uri","https://goescholar.uni-goettingen.de/licenses"],["dc.title","Toward Detection of Electron-Hole Pair Excitation in H-atom Collisions with Au(111): Adiabatic Molecular Dynamics with a Semi-Empirical Full-Dimensional Potential Energy Surface"],["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.firstpage","4887"],["dc.bibliographiccitation.issue","19"],["dc.bibliographiccitation.journal","The Journal of Physical Chemistry Letters"],["dc.bibliographiccitation.lastpage","4892"],["dc.bibliographiccitation.volume","8"],["dc.contributor.author","Wagner, Roman J. V."],["dc.contributor.author","Henning, Niklas"],["dc.contributor.author","Krüger, Bastian C."],["dc.contributor.author","Park, G. Barratt"],["dc.contributor.author","Altschäffel, Jan"],["dc.contributor.author","Kandratsenka, Alexander"],["dc.contributor.author","Wodtke, Alec M."],["dc.contributor.author","Schäfer, Tim"],["dc.date.accessioned","2020-12-10T15:22:46Z"],["dc.date.available","2020-12-10T15:22:46Z"],["dc.date.issued","2017"],["dc.identifier.doi","10.1021/acs.jpclett.7b02207"],["dc.identifier.issn","1948-7185"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/73533"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-354"],["dc.title","Vibrational Relaxation of Highly Vibrationally Excited CO Scattered from Au(111): Evidence for CO – Formation"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dspace.entity.type","Publication"]]

[["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","14306"],["dc.bibliographiccitation.issue","50"],["dc.bibliographiccitation.journal","The Journal of Physical Chemistry A"],["dc.bibliographiccitation.lastpage","14314"],["dc.bibliographiccitation.volume","115"],["dc.contributor.author","LaRue, Jerry L."],["dc.contributor.author","Schaefer, Tim"],["dc.contributor.author","Matsiev, Daniel"],["dc.contributor.author","Velarde, Luis"],["dc.contributor.author","Nahler, N. Hendrik"],["dc.contributor.author","Auerbach, Daniel J."],["dc.contributor.author","Wodtke, Alec Michael"],["dc.date.accessioned","2018-11-07T08:48:46Z"],["dc.date.available","2018-11-07T08:48:46Z"],["dc.date.issued","2011"],["dc.description.abstract","We report kinetic energy distributions of exoelectrons produced by collisions of highly vibrationally excited NO molecules with a low work function Cs dosed Au(111) surface. These measurements show that energy dissipation pathways involving nonadiabatic conversion of vibrational energy to electronic energy can result in electronic excitation of more than 3 eV, consistent with the available vibrational energy. We measured the dependence of the electron energy distributions on the translational and vibrational energy of the incident NO and find a clear positive correlation between final electron kinetic energy and initial vibrational excitation and a weak but observable inverse dependence of electron kinetic energy on initial translational energy. These observations are consistent with a vibrational autodetachment mechanism, where an electron is transferred to NO near its outer vibrational turning point and ejected near its inner vibrational turning point. Within the context of this model, we estimate the NO-to-surface distance for electron transfer."],["dc.identifier.doi","10.1021/jp205868g"],["dc.identifier.isi","000297947300010"],["dc.identifier.pmid","22112161"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/21305"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","1089-5639"],["dc.title","Electron Kinetic Energies from Vibrationally Promoted Surface Exoemission: Evidence for a Vibrational Autodetachment Mechanism"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.artnumber","5373"],["dc.bibliographiccitation.journal","Nature Communications"],["dc.bibliographiccitation.volume","5"],["dc.contributor.author","Kaufmann, Sven"],["dc.contributor.author","Schwarzer, Dirk"],["dc.contributor.author","Reichardt, Christian"],["dc.contributor.author","Wodtke, Alec Michael"],["dc.contributor.author","Buenermann, Oliver"],["dc.date.accessioned","2018-11-07T09:32:50Z"],["dc.date.available","2018-11-07T09:32:50Z"],["dc.date.issued","2014"],["dc.description.abstract","Ultra-short light pulses enable many time-resolved studies in chemistry, especially when used in pump-probe experiments. However, most chemical events are not initiated by light, but rather by collisions. Time-resolved collisional experiments require ultra-short pulses of atoms and molecules-sadly, methods for producing such pulses are so far unknown. Here we introduce bunch-compression photolysis, an approach to forming ultra-short and highly intense pulses of neutral atoms. We demonstrate H-atom pulses of 1.2 +/- 0.3 ns duration, far shorter than any previously reported. Owing to its extraordinarily simple physical principles, we can accurately model the method-the model shows H-atom pulses as short as 110-ps are achievable. Importantly, due to the bunch-compression, large (mm(3)) photolysis volumes are possible, a key advantage for pulse intensity. This technique overcomes the most challenging barrier to a new class of experiments on time-resolved collisions involving atoms and molecules."],["dc.identifier.doi","10.1038/ncomms6373"],["dc.identifier.isi","000345740200004"],["dc.identifier.pmid","25371239"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/31835"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Nature Publishing Group"],["dc.relation.issn","2041-1723"],["dc.title","Generation of ultra-short hydrogen atom pulses by bunch-compression photolysis"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","680"],["dc.bibliographiccitation.issue","4"],["dc.bibliographiccitation.journal","Proceedings of the National Academy of Sciences"],["dc.bibliographiccitation.lastpage","684"],["dc.bibliographiccitation.volume","115"],["dc.contributor.author","Kandratsenka, Alexander"],["dc.contributor.author","Jiang, Hongyan"],["dc.contributor.author","Dorenkamp, Yvonne"],["dc.contributor.author","Janke, Svenja M."],["dc.contributor.author","Kammler, Marvin"],["dc.contributor.author","Wodtke, Alec Michael"],["dc.contributor.author","Bünermann, Oliver"],["dc.date.accessioned","2020-12-10T18:12:47Z"],["dc.date.available","2020-12-10T18:12:47Z"],["dc.date.issued","2018"],["dc.identifier.doi","10.1073/pnas.1710587115"],["dc.identifier.eissn","1091-6490"],["dc.identifier.issn","0027-8424"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/74499"],["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","Unified description of H-atom–induced chemicurrents and inelastic scattering"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","3735"],["dc.bibliographiccitation.issue","21"],["dc.bibliographiccitation.journal","The Journal of Physical Chemistry Letters"],["dc.bibliographiccitation.lastpage","3740"],["dc.bibliographiccitation.volume","4"],["dc.contributor.author","Pavanello, Michele"],["dc.contributor.author","Auerbach, Daniel J."],["dc.contributor.author","Wodtke, Alec Michael"],["dc.contributor.author","Blanco-Rey, Maria"],["dc.contributor.author","Alducin, Maite"],["dc.contributor.author","Kroes, Geert-Jan"],["dc.date.accessioned","2018-11-07T09:17:40Z"],["dc.date.available","2018-11-07T09:17:40Z"],["dc.date.issued","2013"],["dc.description.abstract","Nonadiabatic energy transfer from the translational motion (T) of a molecule impinging on metal surface to the metal's electrons may determine whether the molecule can lose enough energy to adsorb or react. Although it is thus relevant to heterogeneous catalysis, little is known about the strength of the coupling of T to electron hole pair (ehp) excitation. We present adiabatic ab initio molecular dynamics (AIMD) predictions of the scattering of S eV H-atoms from Cu and Au surfaces. Calculations of angularly resolved scattering reveal experimentally realizable conditions where only about 2% of the incidence energy is lost to the metal's phonons. Under these conditions, measurements of the translational energy loss should be able to determine the magnitude of any additional energy loss due to ehp excitation, information that is very valuable to the development of accurate theoretical descriptions of T -> ehp coupling."],["dc.identifier.doi","10.1021/jz401955r"],["dc.identifier.isi","000326845200004"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/28220"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","1948-7185"],["dc.title","Adiabatic Energy Loss in Hyperthermal H Atom Collisions with Cu and Au: A Basis for Testing the Importance of Nonadiabatic Energy Loss"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.artnumber","013939"],["dc.bibliographiccitation.issue","1"],["dc.bibliographiccitation.journal","The Journal of Chemical Physics"],["dc.bibliographiccitation.volume","147"],["dc.contributor.author","Harding, Dan J."],["dc.contributor.author","Neugebohren, Jannis"],["dc.contributor.author","Hahn, Hinrich W."],["dc.contributor.author","Auerbach, Daniel J."],["dc.contributor.author","Kitsopoulos, T. N."],["dc.contributor.author","Wodtke, Alec Michael"],["dc.date.accessioned","2018-11-07T10:22:00Z"],["dc.date.available","2018-11-07T10:22:00Z"],["dc.date.issued","2017"],["dc.description.abstract","We describe a new instrument that uses ion imaging to study molecular beam-surface scattering and surface desorption kinetics, allowing independent determination of both residence times on the surface and scattering velocities of desorbing molecules. This instrument thus provides the capability to derive true kinetic traces, i.e., product flux versus residence time, and allows dramatically accelerated data acquisition compared to previous molecular beam kinetics methods. The experiment exploits non-resonant multiphoton ionization in the near-IR using a powerful 150-fs laser pulse, making detection more general than previous experiments using resonance enhanced multiphoton ionization. We demonstrate the capabilities of the new instrument by examining the desorption kinetics of CO on Pd(111) and Pt(111) and obtain both pre-exponential factors and activation energies of desorption. We also show that the new approach is compatible with velocity map imaging. Published by AIP Publishing."],["dc.identifier.doi","10.1063/1.4983307"],["dc.identifier.isi","000402196200040"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/42198"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","PUB_WoS_Import"],["dc.relation.issn","1089-7690"],["dc.relation.issn","0021-9606"],["dc.title","Ion and velocity map imaging for surface dynamics and kinetics"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","723"],["dc.bibliographiccitation.issue","12"],["dc.bibliographiccitation.journal","Nature Reviews. Chemistry"],["dc.bibliographiccitation.lastpage","732"],["dc.bibliographiccitation.volume","3"],["dc.contributor.author","Park, G. Barratt"],["dc.contributor.author","Kitsopoulos, Theofanis N."],["dc.contributor.author","Borodin, Dmitriy"],["dc.contributor.author","Golibrzuch, Kai"],["dc.contributor.author","Neugebohren, Jannis"],["dc.contributor.author","Auerbach, Daniel J."],["dc.contributor.author","Campbell, Charles T."],["dc.contributor.author","Wodtke, Alec M."],["dc.date.accessioned","2020-01-10T13:29:59Z"],["dc.date.available","2020-01-10T13:29:59Z"],["dc.date.issued","2019"],["dc.description.abstract","The kinetics of elementary reactions is fundamental to our understanding of catalysis. Just as microkinetic models of atmospheric chemistry provided the predictive power that led to the Montreal Protocol reversing loss of stratospheric ozone, pursuing a microkinetic approach to heterogeneous catalysis has tremendous potential for societal impact. However, the development of this approach for catalysis faces great challenges. Methods for measuring rate constants are quite limited, and the present predictive theoretical methods remain largely unvalidated. Here, we present a short Perspective on recent experimental advances in the measurement of rates of elementary reactions at surfaces that rely on a stroboscopic pump–probe concept for neutral matter. We present the principles behind successful measurement methods and discuss a recent implementation of those principles. The topic is discussed within the context of a specific but highly typical surface reaction, CO oxidation on Pt, which, despite more than 40 years of study, was only clarified after experiments with velocity-resolved kinetics became possible. This deceptively simple reaction illustrates fundamental lessons concerning the coverage dependence of activation energies, the nature of reaction mechanisms involving multiple reaction sites, the validity of transition-state theory to describe reaction rates at surfaces and the dramatic changes in reaction mechanism that are possible when studying reactions at low temperatures."],["dc.identifier.doi","10.1038/s41570-019-0138-7"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/62847"],["dc.language.iso","en"],["dc.notes.status","final"],["dc.relation.issn","2397-3358"],["dc.title","The kinetics of elementary thermal reactions in heterogeneous catalysis"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dspace.entity.type","Publication"]]