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  • American Association for the Advancement of Science (AAAS)  (7)
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  • 1
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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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  • 2
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    Enhanced reactivity of highly vibrationally excited molecules on metal surfaces (1999)
    American Association for the Advancement of Science (AAAS)
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    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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  • 3
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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)
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    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〉
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    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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    The "Ozone Deficit" Problem: O2(X, v ge 26) + O(3P) from 226-nm Ozone Photodissociation (1994)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 1994-09-23
    Description: Highly vibrationally excited O(2)(X(3)sigmag(-), v 〉/= 26) has been observed from the photodissociation of ozone (O(3)), and the quantum yield for this reaction has been determined for excitation at 226 nanometers. This observation may help to address the "ozone deficit" problem, or why the previously predicted stratospheric O(3) concentration is less than that observed. Recent kinetic studies have suggested that O(2)(X(3)sigmag(-), v 〉/= 26) can react rapidly with O(2) to form O(3) + O and have led to speculation that, if produced in the photodissociation of O(3), this species might be involved in resolving the discrepancy. The sequence O(3) + hv --〉 O(2)(X(3)sigmag(-), v 〉/= 26) + O; O(2)(X(3)sigmag(-), v 〉/= 26) + O(2) --〉 O(3) + O (where hv is a photon) would be an autocatalytic mechanism for production of odd oxygen. A two-dimensional atmospheric model has been used to evaluate the importance of this new mechanism. The new mechanism can completely account for the tropical O(3) deficit at an altitude of 43 kilometers, but it does not completely account for the deficit at higher altitudes. The mechanism also provides for isotopic fractionation and may contribute to an explanation for the anomalously high concentration of heavy O(3) in the stratosphere.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Miller, R L -- Suits, A G -- Houston, P L -- Toumi, R -- Mack, J A -- Wodtke, A M -- New York, N.Y. -- Science. 1994 Sep 23;265(5180):1831-8.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/17797220" target="_blank"〉PubMed〈/a〉
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  • 5
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    Chemistry. Chemistry in a computer: advancing the in silico dream (2006)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 2006-04-08
    Description: 〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Wodtke, Alec M -- New York, N.Y. -- Science. 2006 Apr 7;312(5770):64-5.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemistry and Biochemistry, University of California, Santa Barbara, CA 93106, USA. wodtke@chem.ucsb.edu〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/16601182" target="_blank"〉PubMed〈/a〉
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  • 6
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    Imaging techniques. Ultrafast low-energy electron diffraction in transmission resolves polymer/graphene superstructure dynamics (2014)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 2014-07-12
    Description: Two-dimensional systems such as surfaces and molecular monolayers exhibit a multitude of intriguing phases and complex transitions. Ultrafast structural probing of such systems offers direct time-domain information on internal interactions and couplings to a substrate or bulk support. We have developed ultrafast low-energy electron diffraction and investigate in transmission the structural relaxation in a polymer/graphene bilayer system excited out of equilibrium. The laser-pump/electron-probe scheme resolves the ultrafast melting of a polymer superstructure consisting of folded-chain crystals registered to a free-standing graphene substrate. We extract the time scales of energy transfer across the bilayer interface, the loss of superstructure order, and the appearance of an amorphous phase with short-range correlations. The high surface sensitivity makes this experimental approach suitable for numerous problems in ultrafast surface science.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Gulde, Max -- Schweda, Simon -- Storeck, Gero -- Maiti, Manisankar -- Yu, Hak Ki -- Wodtke, Alec M -- Schafer, Sascha -- Ropers, Claus -- New York, N.Y. -- Science. 2014 Jul 11;345(6193):200-4. doi: 10.1126/science.1250658.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉4th Physical Institute, University of Gottingen, 37077 Gottingen, Germany. ; Max Planck Institute for Biophysical Chemistry, 37077 Gottingen, Germany. ; Max Planck Institute for Biophysical Chemistry, 37077 Gottingen, Germany. Institute for Physical Chemistry, University of Gottingen, 37077 Gottingen, Germany. ; 4th Physical Institute, University of Gottingen, 37077 Gottingen, Germany. cropers@gwdg.de.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/25013072" target="_blank"〉PubMed〈/a〉
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  • 7
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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
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    Topics: Biology , Chemistry and Pharmacology , Computer Science , Medicine , Natural Sciences in General , Physics
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