Towards a chemically accurate description of reactive molecule-surface scattering

DIPC Seminars

Geert-Jan Kroes (Leiden Institute of Chemistry, The Netherlands)
Donostia International Physics Center (DIPC). Paseo Manuel de Lardizabal, 4, Donostia
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Towards a chemically accurate description of reactive molecule-surface scattering **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)