Non-adiabatic effects during the dissociative adsorption of O2 at Ag(111)? A first-principles divide and conquer study

Details Non-adiabatic effects during the dissociative adsorption of O2 at Ag(111)? A first-principles divide and conquer study Non-adiabatic effects during the dissociative adsorption of O2 at Ag(111)? A first-principles divide and conquer study

2012-01-26

arxiv.org/abs/1201.5514v1

New J. Phys. 14, 013050 (2012)

Physics

Condensed Matter

Materials Science

18 pages including 6 figures

Scientific paper

10.1088/1367-2630/14/1/013050

We study the gas-surface dynamics of O2 at Ag(111) with the particular objective to unravel whether electronic non-adiabatic effects are contributing to the experimentally established inertness of the surface with respect to oxygen uptake. We employ a first-principles divide and conquer approach based on an extensive density-functional theory mapping of the adiabatic potential energy surface (PES) along the six O2 molecular degrees of freedom. Neural networks are subsequently used to interpolate this grid data to a continuous representation. The low computational cost with which forces are available from this PES representation allows then for a sufficiently large number of molecular dynamics trajectories to quantitatively determine the very low initial dissociative sticking coefficient at this surface. Already these adiabatic calculations yield dissociation probabilities close to the scattered experimental data. Our analysis shows that this low reactivity is governed by large energy barriers in excess of 1.1 eV very close to the surface. Unfortunately, these adiabatic PES characteristics render the dissociative sticking a rather insensitive quantity with respect to a potential spin or charge non-adiabaticity in the O2-Ag(111) interaction. We correspondingly attribute the remaining deviations between the computed and measured dissociation probabilities primarily to unresolved experimental issues with respect to surface imperfections.

Affiliated with

Also associated with

No associations

Rating

Non-adiabatic effects during the dissociative adsorption of O2 at Ag(111)? A first-principles divide and conquer study does not yet have a rating. At this time, there are no reviews or comments for this scientific paper.

If you have personal experience with Non-adiabatic effects during the dissociative adsorption of O2 at Ag(111)? A first-principles divide and conquer study, we encourage you to share that experience with our LandOfFree.com community. Your opinion is very important and Non-adiabatic effects during the dissociative adsorption of O2 at Ag(111)? A first-principles divide and conquer study will most certainly appreciate the feedback.

Rate now

Comments { 0 }

Profile ID: LFWR-SCP-O-445628