Following the microscopic pathway to adsorption through chemisorption and physisorption wells

Dmitriy Borodin, Igor Rahinov, Pranav R. Shirhatti, Meng Huang, Alexander Kandratsenka, Daniel J. Auerbach, Tianli Zhong, Hua Guo, Dirk Schwarzer, Theofanis N. Kitsopoulos, Alec M. Wodtke

Research output: Contribution to journalArticlepeer-review

38 Scopus citations

Abstract

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.

Original languageEnglish
Article numberABC9581
Pages (from-to)1461-1465
Number of pages5
JournalScience
Volume369
Issue number6509
DOIs
StatePublished - 1 Sep 2020
Externally publishedYes

ASJC Scopus subject areas

  • General

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