AustralieFrV1, Main, Exploration, bibRecord, 006869

On the temperature dependence of electronically non-adiabatic vibrational energy transfer in molecule-surface collisions

Identifieur interne : 006869 ( Main/Exploration ); précédent : 006868; suivant : 006870

On the temperature dependence of electronically non-adiabatic vibrational energy transfer in molecule-surface collisions

Auteurs : Daniel Matsiev [États-Unis] ; ZHISHENG LI [États-Unis] ; Russell Cooper [États-Unis, Allemagne] ; Igor Rahinov [États-Unis, Israël] ; Christof Bartels [États-Unis, Allemagne] ; Daniel J. Auerbach [États-Unis] ; Alec M. Wodtke [États-Unis, Allemagne]

Source :

PCCP. Physical chemistry chemical physics : (Print) [ 1463-9076 ] ; 2011.

RBID : Pascal:11-0291001

Descripteurs français

Pascal (Inist)
- Dépendance température, Energie vibrationnelle, Transfert énergie, Collision molécule surface, Modèle cinétique, Etat vibrationnel excité, Faisceau moléculaire, Cinétique, Séquentiel, Mécanisme, Basse température, Equilibre, Donnée expérimentale.

English descriptors

KwdEn :
- Energy transfer, Equilibrium, Experimental data, Kinetic model, Kinetics, Low temperature, Mechanism, Molecular beam, Molecule surface collision, Sequential, Temperature dependence, Vibrational energy, Vibrationally excited state.

Abstract

Here we extend a recently introduced state-to-state kinetic model describing single- and multi-quantum vibrational excitation of molecular beams of NO scattering from a Au(111) metal surface. We derive an analytical expression for the rate of electronically non-adiabatic vibrational energy transfer, which is then employed in the analysis of the temperature dependence of the kinetics of direct overtone and two-step sequential energy transfer mechanisms. We show that the Arrhenius surface temperature dependence for vibrational excitation probability reported in many previous studies emerges as a low temperature limit of a more general solution that describes the approach to thermal equilibrium in the limit of infinite interaction time and that the pre-exponential term of the Arrhenius expression can be used not only to distinguish between the direct overtone and sequential mechanisms, but also to deduce their relative contributions. We also apply the analytical expression for the vibrational energy transfer rates introduced in this work to the full kinetic model and obtain an excellent fit to experimental data, the results of which show how to extract numerical values of the molecule-surface coupling strength and its fundamental properties.

Affiliations:

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Le document en format XML

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<profileDesc><textClass><keywords scheme="KwdEn" xml:lang="en"><term>Energy transfer</term>
<term>Equilibrium</term>
<term>Experimental data</term>
<term>Kinetic model</term>
<term>Kinetics</term>
<term>Low temperature</term>
<term>Mechanism</term>
<term>Molecular beam</term>
<term>Molecule surface collision</term>
<term>Sequential</term>
<term>Temperature dependence</term>
<term>Vibrational energy</term>
<term>Vibrationally excited state</term>
</keywords>
<keywords scheme="Pascal" xml:lang="fr"><term>Dépendance température</term>
<term>Energie vibrationnelle</term>
<term>Transfert énergie</term>
<term>Collision molécule surface</term>
<term>Modèle cinétique</term>
<term>Etat vibrationnel excité</term>
<term>Faisceau moléculaire</term>
<term>Cinétique</term>
<term>Séquentiel</term>
<term>Mécanisme</term>
<term>Basse température</term>
<term>Equilibre</term>
<term>Donnée expérimentale</term>
</keywords>
</textClass>
</profileDesc>
</teiHeader>
<front><div type="abstract" xml:lang="en">Here we extend a recently introduced state-to-state kinetic model describing single- and multi-quantum vibrational excitation of molecular beams of NO scattering from a Au(111) metal surface. We derive an analytical expression for the rate of electronically non-adiabatic vibrational energy transfer, which is then employed in the analysis of the temperature dependence of the kinetics of direct overtone and two-step sequential energy transfer mechanisms. We show that the Arrhenius surface temperature dependence for vibrational excitation probability reported in many previous studies emerges as a low temperature limit of a more general solution that describes the approach to thermal equilibrium in the limit of infinite interaction time and that the pre-exponential term of the Arrhenius expression can be used not only to distinguish between the direct overtone and sequential mechanisms, but also to deduce their relative contributions. We also apply the analytical expression for the vibrational energy transfer rates introduced in this work to the full kinetic model and obtain an excellent fit to experimental data, the results of which show how to extract numerical values of the molecule-surface coupling strength and its fundamental properties.</div>
</front>
</TEI>
<affiliations><list><country><li>Allemagne</li>
<li>Israël</li>
<li>États-Unis</li>
</country>
<region><li>Basse-Saxe</li>
<li>Californie</li>
</region>
<settlement><li>Göttingen</li>
<li>Santa Barbara (Californie)</li>
</settlement>
<orgName><li>Université de Californie</li>
<li>Université de Californie à Santa Barbara</li>
</orgName>
</list>
<tree><country name="États-Unis"><region name="Californie"><name sortKey="Matsiev, Daniel" sort="Matsiev, Daniel" uniqKey="Matsiev D" first="Daniel" last="Matsiev">Daniel Matsiev</name>
</region>
<name sortKey="Auerbach, Daniel J" sort="Auerbach, Daniel J" uniqKey="Auerbach D" first="Daniel J." last="Auerbach">Daniel J. Auerbach</name>
<name sortKey="Auerbach, Daniel J" sort="Auerbach, Daniel J" uniqKey="Auerbach D" first="Daniel J." last="Auerbach">Daniel J. Auerbach</name>
<name sortKey="Bartels, Christof" sort="Bartels, Christof" uniqKey="Bartels C" first="Christof" last="Bartels">Christof Bartels</name>
<name sortKey="Cooper, Russell" sort="Cooper, Russell" uniqKey="Cooper R" first="Russell" last="Cooper">Russell Cooper</name>
<name sortKey="Rahinov, Igor" sort="Rahinov, Igor" uniqKey="Rahinov I" first="Igor" last="Rahinov">Igor Rahinov</name>
<name sortKey="Wodtke, Alec M" sort="Wodtke, Alec M" uniqKey="Wodtke A" first="Alec M." last="Wodtke">Alec M. Wodtke</name>
<name sortKey="Zhisheng Li" sort="Zhisheng Li" uniqKey="Zhisheng Li" last="Zhisheng Li">ZHISHENG LI</name>
</country>
<country name="Allemagne"><region name="Basse-Saxe"><name sortKey="Cooper, Russell" sort="Cooper, Russell" uniqKey="Cooper R" first="Russell" last="Cooper">Russell Cooper</name>
</region>
<name sortKey="Bartels, Christof" sort="Bartels, Christof" uniqKey="Bartels C" first="Christof" last="Bartels">Christof Bartels</name>
<name sortKey="Wodtke, Alec M" sort="Wodtke, Alec M" uniqKey="Wodtke A" first="Alec M." last="Wodtke">Alec M. Wodtke</name>
<name sortKey="Wodtke, Alec M" sort="Wodtke, Alec M" uniqKey="Wodtke A" first="Alec M." last="Wodtke">Alec M. Wodtke</name>
</country>
<country name="Israël"><noRegion><name sortKey="Rahinov, Igor" sort="Rahinov, Igor" uniqKey="Rahinov I" first="Igor" last="Rahinov">Igor Rahinov</name>
</noRegion>
</country>
</tree>
</affiliations>
</record>

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On the temperature dependence of electronically non-adiabatic vibrational energy transfer in molecule-surface collisions

On the temperature dependence of electronically non-adiabatic vibrational energy transfer in molecule-surface collisions

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