Following the microscopic pathway to adsorption through chemisorption and physisorption wells.


Journal

Science (New York, N.Y.)
ISSN: 1095-9203
Titre abrégé: Science
Pays: United States
ID NLM: 0404511

Informations de publication

Date de publication:
18 09 2020
Historique:
received: 24 05 2020
accepted: 14 07 2020
entrez: 18 9 2020
pubmed: 19 9 2020
medline: 19 9 2020
Statut: ppublish

Résumé

Adsorption involves molecules colliding at the surface of a solid and losing their incidence energy by traversing a dynamical pathway to equilibrium. The interactions responsible for energy loss generally include both chemical bond formation (chemisorption) and nonbonding interactions (physisorption). In this work, we present experiments that revealed a quantitative energy landscape and the microscopic pathways underlying a molecule's equilibration with a surface in a prototypical system: CO adsorption on Au(111). Although the minimum energy state was physisorbed, initial capture of the gas-phase molecule, dosed with an energetic molecular beam, was into a metastable chemisorption state. Subsequent thermal decay of the chemisorbed state led molecules to the physisorption minimum. We found, through detailed balance, that thermal adsorption into both binding states was important at all temperatures.

Identifiants

pubmed: 32943520
pii: 369/6510/1461
doi: 10.1126/science.abc9581
doi:

Types de publication

Journal Article Research Support, Non-U.S. Gov't

Langues

eng

Sous-ensembles de citation

IM

Pagination

1461-1465

Subventions

Organisme : Deutsche Forschungsgemeinschaft
Pays : International

Informations de copyright

Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.

Auteurs

Dmitriy Borodin (D)

Institute for Physical Chemistry, Georg-August University of Göttingen, Tammannstraße 6, 37077 Göttingen, Germany.
Department of Dynamics at Surfaces, Max Planck Institute for Biophysical Chemistry, Am Faßberg 11, 37077 Göttingen, Germany.

Igor Rahinov (I)

Department of Natural Sciences, The Open University of Israel, 4353701 Raanana, Israel.

Pranav R Shirhatti (PR)

Tata Institute of Fundamental Research, 500046 Hyderabad, India.

Meng Huang (M)

Department of Chemistry and Chemical Biology, University of New Mexico, Albuquerque, NM 87131, USA.

Alexander Kandratsenka (A)

Department of Dynamics at Surfaces, Max Planck Institute for Biophysical Chemistry, Am Faßberg 11, 37077 Göttingen, Germany.

Daniel J Auerbach (DJ)

Department of Dynamics at Surfaces, Max Planck Institute for Biophysical Chemistry, Am Faßberg 11, 37077 Göttingen, Germany.

Tianli Zhong (T)

Institute for Physical Chemistry, Georg-August University of Göttingen, Tammannstraße 6, 37077 Göttingen, Germany.
Department of Dynamics at Surfaces, Max Planck Institute for Biophysical Chemistry, Am Faßberg 11, 37077 Göttingen, Germany.

Hua Guo (H)

Department of Chemistry and Chemical Biology, University of New Mexico, Albuquerque, NM 87131, USA.

Dirk Schwarzer (D)

Department of Dynamics at Surfaces, Max Planck Institute for Biophysical Chemistry, Am Faßberg 11, 37077 Göttingen, Germany.

Theofanis N Kitsopoulos (TN)

Institute for Physical Chemistry, Georg-August University of Göttingen, Tammannstraße 6, 37077 Göttingen, Germany.
Department of Dynamics at Surfaces, Max Planck Institute for Biophysical Chemistry, Am Faßberg 11, 37077 Göttingen, Germany.
Department of Chemistry, University of Crete, 71003 Heraklion, Greece.
Institute of Electronic Structure and Laser, FORTH, 71110 Heraklion, Greece.

Alec M Wodtke (AM)

Institute for Physical Chemistry, Georg-August University of Göttingen, Tammannstraße 6, 37077 Göttingen, Germany. alec.wodtke@mpibpc.mpg.de.
Department of Dynamics at Surfaces, Max Planck Institute for Biophysical Chemistry, Am Faßberg 11, 37077 Göttingen, Germany.
International Center for Advanced Studies of Energy Conversion, Georg-August University of Göttingen, Tammannstraße 6, 37077 Göttingen, Germany.

Classifications MeSH