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  • 1
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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)
    Details
    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
    Published by American Institute of Physics (AIP)
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  • 2
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    Surface science. Hitting the surface--softly (2001)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 2001-12-26
    Description: 〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Auerbach, D J -- New York, N.Y. -- Science. 2001 Dec 21;294(5551):2488-9.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Almaden Research Center, IBM, Almaden, CA 95120, USA. dja@almaden.ibm.com〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/11752560" 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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  • 3
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    Vibrational promotion of electron transfer (2000)
    American Association for the Advancement of Science (AAAS)
    Details
    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
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  • 4
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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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  • 5
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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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  • 6
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    Chemically accurate simulation of a prototypical surface reaction: H2 dissociation on Cu(111) (2009)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 2009-11-07
    Description: Methods for accurately computing the interaction of molecules with metal surfaces are critical to understanding and thereby improving heterogeneous catalysis. We introduce an implementation of the specific reaction parameter (SRP) approach to density functional theory (DFT) that carries the method forward from a semiquantitative to a quantitative description of the molecule-surface interaction. Dynamics calculations on reactive scattering of hydrogen from the copper (111) surface using an SRP-DFT potential energy surface reproduce data on the dissociative adsorption probability as a function of incidence energy and reactant state and data on rotationally inelastic scattering with chemical accuracy (within approximately 4.2 kilojoules per mole).〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Diaz, C -- Pijper, E -- Olsen, R A -- Busnengo, H F -- Auerbach, D J -- Kroes, G J -- New York, N.Y. -- Science. 2009 Nov 6;326(5954):832-4. doi: 10.1126/science.1178722.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Leiden Institute of Chemistry, Gorlaeus Laboratories, Leiden University, Post Office Box 9502, 2300 RA Leiden, Netherlands.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/19892978" 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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  • 7
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    Distinguishing the direct and indirect products of a gas-surface reaction (1994)
    American Association for the Advancement of Science (AAAS)
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    Publication Date: 1994-01-21
    Description: It has long been postulated that gas-surface chemical reactions can occur by means of two distinct mechanisms: direct reaction on a single gas-surface encounter or reaction between two adsorbed species. It is shown here that these mechanisms have distinct dynamical signatures, as illustrated by the reaction of hydrogen with chlorine on gold(111). The direct reaction product leaves the surface with a high kinetic energy in a narrow angular distribution that displays a "memory" of the direction and energy of the incident hydrogen atom. The indirect reaction product has a near-thermal energy distribution and an angular distribution that is close to that of a cosine function.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Rettner, C T -- Auerbach, D J -- New York, N.Y. -- Science. 1994 Jan 21;263(5145):365-7.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/17769801" 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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  • 8
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    Electron-hole pair excitation determines the mechanism of hydrogen atom adsorption (2015)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 2015-11-28
    Description: How much translational energy atoms and molecules lose in collisions at surfaces determines whether they adsorb or scatter. The fact that hydrogen (H) atoms stick to metal surfaces poses a basic question. Momentum and energy conservation demands that the light H atom cannot efficiently transfer its energy to the heavier atoms of the solid in a binary collision. How then do H atoms efficiently stick to metal surfaces? We show through experiments that H-atom collisions at an insulating surface (an adsorbed xenon layer on a gold single-crystal surface) are indeed nearly elastic, following the predictions of energy and momentum conservation. In contrast, H-atom collisions with the bare gold surface exhibit a large loss of translational energy that can be reproduced by an atomic-level simulation describing electron-hole pair excitation.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Bunermann, Oliver -- Jiang, Hongyan -- Dorenkamp, Yvonne -- Kandratsenka, Alexander -- Janke, Svenja M -- Auerbach, Daniel J -- Wodtke, Alec M -- New York, N.Y. -- Science. 2015 Dec 11;350(6266):1346-9. doi: 10.1126/science.aad4972. Epub 2015 Nov 26.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Institute for Physical Chemistry, Georg-August University of Gottingen, Tammannstrasse 6, 37077 Gottingen, Germany. Department of Dynamics at Surfaces, Max Planck Institute for Biophysical Chemistry, Am Fassberg 11, 37077 Gottingen, Germany. International Center for Advanced Studies of Energy Conversion, Georg-August University of Gottingen, Tammannstrasse 6, 37077 Gottingen, Germany. oliver.buenermann@chemie.uni-goettingen.de. ; Institute for Physical Chemistry, Georg-August University of Gottingen, Tammannstrasse 6, 37077 Gottingen, Germany. ; Institute for Physical Chemistry, Georg-August University of Gottingen, Tammannstrasse 6, 37077 Gottingen, Germany. Department of Dynamics at Surfaces, Max Planck Institute for Biophysical Chemistry, Am Fassberg 11, 37077 Gottingen, Germany. ; Institute for Physical Chemistry, Georg-August University of Gottingen, Tammannstrasse 6, 37077 Gottingen, Germany. Department of Dynamics at Surfaces, Max Planck Institute for Biophysical Chemistry, Am Fassberg 11, 37077 Gottingen, Germany. International Center for Advanced Studies of Energy Conversion, Georg-August University of Gottingen, Tammannstrasse 6, 37077 Gottingen, Germany.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/26612832" 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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  • 9
    Electronic Resource
    Electronic Resource
    Dynamics of recombinative desorption: Angular distributions of H2, HD, and D2 desorbing from Cu(111) (1991)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 94 (1991), S. 7499-7501 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We have determined the angular distributions of H2, HD, and D2 desorbing from Cu(111) for surface temperatures in the range 370–800 K. These are found to be strongly peaked and symmetric about the surface normal in every case. Results for all three isotopes are found to be indistinguishable, being close to a cos 12θf distribution at 600 K, slightly narrower at 370 K, and slightly broader at 800 K. Results are discussed in terms of other previous desorption measurements and related to adsorption data via detailed balance.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.460181
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  • 10
    Electronic Resource
    Electronic Resource
    A critical examination of data on the dissociative adsorption and associative desorption of hydrogen at copper surfaces (1991)
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 94 (1991), S. 7502-7520 
    Details
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We examine experimental data on the activated dissociative adsorption and associative recombination of hydrogen at copper surfaces with respect to the role played by molecular vibrational states. We use models describing the variation of the adsorption probability with the vibrational state, kinetic energy, and angle of the incident molecules, establishing the parameters of the models by a nonlinear least squares fit to adsorption data. Using the principle of detailed balance, we apply these models to the corresponding data on associative desorption thus comparing adsorption data with desorption angular, velocity, and internal state distributions. The most consistent picture resulting from this analysis is that the adsorption has significant contributions from both H2(v=0) and H2(v=1) and that these components have markedly different translational thresholds. Within the framework of this picture we are able to resolve the apparent contradiction between the strong angular dependence of the kinetic energy required for adsorption and the lack of angular dependence of the mean kinetic energy of desorption. We also partially resolve the apparent discrepancy in interpretation of the role of H2(v=1) in recent adsorption experiments.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1063/1.460182
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