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  • 1
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    Vibrational energy transfer near a dissociative adsorption transition state: State-to-state study of HCl collisions at Au(111) (2016)
    American Institute of Physics (AIP)
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    Publication Date: 2016-08-05
    Description: 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.
    Print ISSN: 0021-9606
    Electronic ISSN: 1089-7690
    Topics: Chemistry and Pharmacology , Physics
    Published by American Institute of Physics (AIP)
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  • 2
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    CO Desorption from a Catalytic Surface: Elucidation of the Role of Steps by Velocity-Selected Residence Time Measurements (2015)
    American Chemical Society (ACS)
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    Publication Date: 2015-01-24
    Description: Journal of the American Chemical Society DOI: 10.1021/ja509530k
    Print ISSN: 0002-7863
    Electronic ISSN: 1520-5126
    Topics: Chemistry and Pharmacology
    Published by American Chemical Society (ACS)
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  • 3
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    A new Stark decelerator based surface scattering instrument for studying energy transfer at the gas-surface interface (2015)
    American Institute of Physics (AIP)
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    Publication Date: 2015-04-25
    Description: We report on the design and characterization of a new apparatus for performing quantum-state resolved surface scattering experiments. The apparatus combines optical state-specific molecule preparation with a compact hexapole and a Stark decelerator to prepare carrier gas-free pulses of quantum-state pure CO molecules with velocities controllable between 33 and 1000 m/s with extremely narrow velocity distributions. The ultrahigh vacuum surface scattering chamber includes homebuilt ion and electron detectors, a closed-cycle helium cooled single crystal sample mount capable of tuning surface temperature between 19 and 1337 K, a Kelvin probe for non-destructive work function measurements, a precision leak valve manifold for targeted adsorbate deposition, an inexpensive quadrupole mass spectrometer modified to perform high resolution temperature programmed desorption experiments and facilities to clean and characterize the surface.
    Print ISSN: 0034-6748
    Electronic ISSN: 1089-7623
    Topics: Electrical Engineering, Measurement and Control Technology , Physics
    Published by American Institute of Physics (AIP)
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  • 4
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    An accurate full-dimensional potential energy surface for H–Au(111): Importance of nonadiabatic electronic excitation in energy transfer and adsorption (2015)
    American Institute of Physics (AIP)
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    Publication Date: 2015-10-01
    Description: We have constructed a potential energy surface (PES) for H-atoms interacting with fcc Au(111) based on fitting the analytic form of the energy from Effective Medium Theory (EMT) to ab initio energy values calculated with density functional theory. The fit used input from configurations of the H–Au system with Au atoms at their lattice positions as well as configurations with the Au atoms displaced from their lattice positions. It reproduces the energy, in full dimension , not only for the configurations used as input but also for a large number of additional configurations derived from ab initio molecular dynamics (AIMD) trajectories at finite temperature. Adiabatic molecular dynamics simulations on this PES reproduce the energy loss behavior of AIMD. EMT also provides expressions for the embedding electron density, which enabled us to develop a self-consistent approach to simulate nonadiabatic electron-hole pair excitation and their effect on the motion of the incident H-atoms. For H atoms with an energy of 2.7 eV colliding with Au, electron-hole pair excitation is by far the most important energy loss pathway, giving an average energy loss ≈3 times that of the adiabatic case. This increased energy loss enhances the probability of the H-atom remaining on or in the Au slab by a factor of 2. The most likely outcome for H-atoms that are not scattered also depends prodigiously on the energy transfer mechanism; for the nonadiabatic case, more than 50% of the H-atoms which do not scatter are adsorbed on the surface, while for the adiabatic case more than 50% pass entirely through the 4 layer simulation slab.
    Print ISSN: 0021-9606
    Electronic ISSN: 1089-7690
    Topics: Chemistry and Pharmacology , Physics
    Published by American Institute of Physics (AIP)
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  • 5
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    Generation of ultra-short hydrogen atom pulses by bunch-compression photolysis (2014)
    Springer Nature
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    Publication Date: 2014-11-07
    Description: Article Short pulses of atoms or molecules can act as sensitive probes for numerous physical and chemical systems, but they are typically limited to the microsecond scale. By exploiting short pulse laser photolysis, Kaufmann et al . present a method that can produce pulses of hydrogen atoms on sub-nanosecond scales. Nature Communications doi: 10.1038/ncomms6373 Authors: Sven Kaufmann, Dirk Schwarzer, Christian Reichardt, Alec M. Wodtke, Oliver Bünermann
    Electronic ISSN: 2041-1723
    Topics: Biology , Chemistry and Pharmacology , Natural Sciences in General , Physics
    Published by Springer Nature
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  • 6
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    Electron hole pair mediated vibrational excitation in CO scattering from Au(111): Incidence energy and surface temperature dependence (2014)
    American Institute of Physics (AIP)
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    Publication Date: 2014-09-25
    Description: 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 .
    Print ISSN: 0021-9606
    Electronic ISSN: 1089-7690
    Topics: Chemistry and Pharmacology , Physics
    Published by American Institute of Physics (AIP)
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  • 7
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    Single-field slice-imaging with a movable repeller: Photodissociation of N2O from a hot nozzle (2014)
    American Institute of Physics (AIP)
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    Publication Date: 2014-08-05
    Description: We present a new photo-fragment imaging spectrometer, which employs a movable repeller in a single field imaging geometry. This innovation offers two principal advantages. First, the optimal fields for velocity mapping can easily be achieved even using a large molecular beam diameter (5 mm); the velocity resolution (better than 1%) is sufficient to easily resolve photo-electron recoil in (2 + 1) resonant enhanced multiphoton ionization of N 2 photoproducts from N 2 O or from molecular beam cooled N 2 . Second, rapid changes between spatial imaging, velocity mapping, and slice imaging are straightforward. We demonstrate this technique's utility in a re-investigation of the photodissociation of N 2 O. Using a hot nozzle, we observe slice images that strongly depend on nozzle temperature. Our data indicate that in our hot nozzle expansion, only pure bending vibrations – (0, v 2 , 0) – are populated, as vibrational excitation in pure stretching or bend-stretch combination modes are quenched via collisional near-resonant V-V energy transfer to the nearly degenerate bending states. We derive vibrationally state resolved absolute absorption cross-sections for (0, v 2 ≤ 7, 0). These results agree well with previous work at lower values of v 2 , both experimental and theoretical. The dissociation energy of N 2 O with respect to the O( 1 D) + N 2 Σ g + 1 asymptote was determined to be 3.65 ± 0.02 eV.
    Print ISSN: 0021-9606
    Electronic ISSN: 1089-7690
    Topics: Chemistry and Pharmacology , Physics
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  • 8
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    Vibrational promotion of electron transfer (2000)
    American Association for the Advancement of Science (AAAS)
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    Publication Date: 2000-10-06
    Description: By using laser methods to prepare specific quantum states of gas-phase nitric oxide molecules, we examined the role of vibrational motion in electron transfer to a molecule from a metal surface free from the complicating influence of solvation effects. The signature of the electron transfer process is a highly efficient multiquantum vibrational relaxation event, where the nitrogen oxide loses hundreds of kilojoules per mole of energy on a subpicosecond time scale. These results cannot be explained simply on the basis of Franck-Condon factors. The large-amplitude vibrational motion associated with molecules in high vibrational states strongly modulates the energetic driving force of the electron transfer reaction. These results show the importance of molecular vibration in promoting electron transfer reactions, a class of chemistry important to molecular electronics devices, solar energy conversion, and many biological processes.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Huang, Y -- Rettner, C T -- Auerbach, D J -- Wodtke, A M -- New York, N.Y. -- Science. 2000 Oct 6;290(5489):111-4.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemistry, University of California, Santa Barbara, CA 93106, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/11021790" target="_blank"〉PubMed〈/a〉
    Print ISSN: 0036-8075
    Electronic ISSN: 1095-9203
    Topics: Biology , Chemistry and Pharmacology , Computer Science , Medicine , Natural Sciences in General , Physics
    Published by American Association for the Advancement of Science (AAAS)
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  • 9
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    Enhanced reactivity of highly vibrationally excited molecules on metal surfaces (1999)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 1999-06-05
    Description: The chemical dynamics of highly vibrationally excited molecules have been studied by measuring the quantum state-resolved scattering probabilities of nitric oxide (NO) molecules on clean and oxygen-covered copper (111) surfaces, where the incident NO was prepared in single quantum states with vibrational energies of as much as 300 kilojoules per mole. The dependence of vibrationally elastic and inelastic scattering on oxygen coverage strongly suggests that highly excited NO (v = 13 and 15) reacts on clean copper (111) with a probability of 0.87 +/- 0.05, more than three orders of magnitude greater than the reaction probability of ground-state NO. Vibrational promotion of surface chemistry on metals (up to near-unit reaction probability) is possible despite the expected efficient relaxation of vibrational energy at metal surfaces.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Hou -- Huang -- Gulding -- Rettner -- Auerbach -- Wodtke -- New York, N.Y. -- Science. 1999 Jun 4;284(5420):1647-50.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉IBM Research Division, Almaden Research Center, San Jose, CA 95120, USA. Department of Chemistry, University of California, Santa Barbara, CA 93106, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/10356389" target="_blank"〉PubMed〈/a〉
    Print ISSN: 0036-8075
    Electronic ISSN: 1095-9203
    Topics: Biology , Chemistry and Pharmacology , Computer Science , Medicine , Natural Sciences in General , Physics
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  • 10
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    Inverse velocity dependence of vibrationally promoted electron emission from a metal surface (2008)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 2008-08-30
    Description: All previous experimental and theoretical studies of molecular interactions at metal surfaces show that electronically nonadiabatic influences increase with molecular velocity. We report the observation of a nonadiabatic electronic effect that follows the opposite trend: The probability of electron emission from a low-work function surface--Au(111) capped by half a monolayer of Cs--increases as the velocity of the incident NO molecule decreases during collisions with highly vibrationally excited NO(X(2)pi((1/2)), V = 18; V is the vibrational quantum number of NO), reaching 0.1 at the lowest velocity studied. We show that these results are consistent with a vibrational autodetachment mechanism, whereby electron emission is possible only beyond a certain critical distance from the surface. This outcome implies that important energy-dissipation pathways involving nonadiabatic electronic excitations and, furthermore, not captured by present theoretical methods may influence reaction rates at surfaces.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Nahler, N H -- White, J D -- Larue, J -- Auerbach, D J -- Wodtke, A M -- New York, N.Y. -- Science. 2008 Aug 29;321(5893):1191-4. doi: 10.1126/science.1160040.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemistry and Biochemistry, University of California Santa Barbara, Santa Barbara, CA 93106-9510, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/18755972" target="_blank"〉PubMed〈/a〉
    Print ISSN: 0036-8075
    Electronic ISSN: 1095-9203
    Topics: Biology , Chemistry and Pharmacology , Computer Science , Medicine , Natural Sciences in General , Physics
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