Towards a chemically accurate description of reactive molecule-surface scattering
DIPC Seminars
- Speaker
-
Geert-Jan Kroes (Leiden Institute of Chemistry, The Netherlands)
- When
-
2015/03/10
13:00 - Place
- Donostia International Physics Center (DIPC). Paseo Manuel de Lardizabal, 4, Donostia
- Add to calendar
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**Towards a chemically accurate description of reactive molecule-surface
scattering.**
_ _
_Geert-Jan Kroes_ _,_ Leiden Institute of Chemistry, Gorlaeus Laboratories,
Leiden University, P.O. Box 9502, 2300 RA Leiden, The Netherlands
Achieving chemical accuracy in the theoretical description of reactive
scattering at metal surfaces requires a chemically accurate description of the
molecule-metal surface interaction and the dynamics of the involved
molecule(s), and may additionally require an accurate description of surface
phonons and electron-hole pair excitation. We have recently shown that a
chemically accurate description of the molecule-surface interaction is
possible with a novel implementation of specific reaction parameter density
functional theory (SRP-DFT) for the H2 \+ Cu(111) system. Progress with the
quest for chemical accuracy for reaction of molecules on metal surfaces will
be reported for four systems. First, for H2 \+ Cu(111) a reanalysis of the
associative desorption experiments performed on D2 \+ Cu(111) [1] yields
effective barrier heights that agree to within chemical accuracy with dynamics
results obtained with the SRP-DFT PES [2]. Second, an improved description of
reactive scattering in the early barrier system H2 \+ Ru(0001) is obtained
with SRP density functionals incorporating a description of the van der Waals
interaction [3]. Third, we report results of AIMD calculations on the reaction
of CHD3 on Pt(111) and Ni(111). The PBE functional underestimates the barrier
height for CHD3 \+ Pt(111) by 0.1 eV [4]. Progress made with obtaining a more
accurate functional for this system will be reported in the talk. Finally,
AIMD results will be presented on the dissociative chemisorption of N2 on
W(110), looking at the effect of surface motion on the reaction probability.
**References.**
[1] H. A. Michelsen, C. T. Rettner, D. J. Auerbach, and R. N. Zare,
J.Chem.Phys. **98** , 8294 (1993).
[2] F. Nattino, A. Genova, M. Guijt, A. S. Muzas, C. Díaz, D. J.
Auerbach, and G. J. Kroes, J.Chem.Phys. **141** , 124705 (2014).
[3] M. Wijzenbroek and G. J. Kroes, J.Chem.Phys. **140** , 084702
(2014).
[4] F. Nattino, H. Ueta, H. Chadwick, M. E. van Reijzen, R. D.
Beck, B. Jackson, M. C. van Hemert, and G. J. Kroes, J.Phys.Chem.Lett. **5** ,
1294 (2014).
(host Maite Alducin)