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  Adsorbate modification of electronic nonadiabaticity: H atom scattering from p(2 × 2) O on Pt(111)

Lecroart, L., Hertl, N., Dorenkamp, Y., Jiang, H., Kitsopoulos, T. N., Kandratsenka, A., et al. (2021). Adsorbate modification of electronic nonadiabaticity: H atom scattering from p(2 × 2) O on Pt(111). The Journal of Chemical Physics, 155(3): 034702. doi:10.1063/5.0058789.

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Lecroart, L.1, Author           
Hertl, N.1, Author           
Dorenkamp, Y., Author
Jiang, H.1, Author           
Kitsopoulos, T. N., Author
Kandratsenka, A.1, Author           
Bünermann, O., Author
Wodtke, A. M.2, Author           
Affiliations:
1Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society, ou_578600              
2Department of Dynamics at Surfaces, MPI for biophysical chemistry, Max Planck Society, ou_578600              

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 Abstract: We report inelastic differential scattering experiments for energetic H and D atoms colliding at a Pt(111) surface with and without adsorbed O atoms. Dramatically, more energy loss is seen for scattering from the Pt(111) surface compared to p(2 × 2) O on Pt(111), indicating that O adsorption reduces the probability of electron–hole pair (EHP) excitation. We produced a new full-dimensional potential energy surface for H interaction with O/Pt that reproduces density functional theory energies accurately. We then attempted to model the EHP excitation in H/D scattering with molecular dynamics simulations employing the electronic density information from the Pt(111) to calculate electronic friction at the level of the local density friction approximation (LDFA). This approach, which assumes that O atoms simply block the Pt atom from the approaching H atom, fails to reproduce experiment due to the fact that the effective collision cross section of the O atom is only 10% of the area of the surface unit cell. An empirical adiabatic sphere model that reduces electronic nonadiabaticity within an O–Pt bonding length scale of 2.8 Å reproduces experiment well, suggesting that the electronic structure changes induced by chemisorption of O atoms nearly remove the H atom’s ability to excite EHPs in the Pt. Alternatives to LDFA friction are needed to account for this adsorbate effect.

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Language(s): eng - English
 Dates: 2021-07-19
 Publication Status: Published online
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 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1063/5.0058789
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Title: The Journal of Chemical Physics
Source Genre: Journal
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Pages: - Volume / Issue: 155 (3) Sequence Number: 034702 Start / End Page: - Identifier: -