Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 9, Issue 12, Pages 3271-3277Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.8b01470
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Funding
- National Key R&D Program of China [2017YFA0303500]
- National Natural Science Foundation of China [21722306, 91645202, 21573203]
- U.S. National Science Foundation [CHE-1462109]
- Anhui Initiative in Quantum Information Technologies
- Austrian Science Fund [FWF SFB-041 ViCoM]
- National Science Foundation [1265700]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1265700] Funding Source: National Science Foundation
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1462109] Funding Source: National Science Foundation
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Dissociative chemisorption of O-2 on the Al(111) surface represents an extensively studied prototype for understanding the interaction between O-2 and metal surfaces. It is well known that the experimentally observed activation barrier for O-2 dissociation is not captured by conventional density functional theory. The interpretation of this barrier as a result of spin transitions along the reaction path has been challenged by recent embedded correlated wave function (ECW) calculations that naturally yield an adiabatic barrier. However, the ECW calculations have been limited to a static analysis of the reaction pathways and have not yet been tested by dynamics simulations. We present a global six-dimensional potential energy surface (PES) for this system parametrized with ECW data points. This new PES provides a reasonable description of the site-specific and orientation-dependent activation barriers. Quasi-classical trajectory calculations on this PES semiquantitatively reproduce both the observed translational energy dependence of the sticking probability and steric effects with aligned O-2 molecules.
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