Universiteit Leiden

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Theoretical Chemistry

Quantum dynamics of dissociative chemisorption of hydrogen and other diatomic molecules on metal surfaces

It is possible to treat the dynamics of the dissociation of hydrogen on metal surfaces quantum mechanically, while taking into account the motion in all six molecular degrees of freedom without making approximations. Because the approximations of neglecting surface phonons and electron-hole pair excitation are reasonable for many experiments on reactive scattering of H2 from metal surfaces, this makes these systems ideal for testing the accuracy of electronic structure methods for molecule-surface reactions.

We have recently introduced a new implementation of specific reaction parameter DFT (SRP-DFT), and shown that this allows a chemically accurate description of many reactive scattering experiments on the benchmark H2 + Cu(111) reaction. Also, it turns out that the SRP density functional for H2 + Cu(111) is transferable to H2 interacting with another low index face of copper, i.e., the (100) face.

In new research, we are investigating whether SRP-DFT can also be made to work for H2 interacting with other metal surfaces, and for other diatomic molecules (e.g., N2) reacting with metal surfaces. We are also investigating the effect of phonons and intend to investigate the effect of electron-hole pair excitation on reactions of molecules at metal surfaces.

For an overview of the exciting questions that need to be addressed for these reactions, see the papers "Frontiers in Surface Scattering Simulations, G.J. Kroes, Science 321, 794-797 (2008)", and "Towards chemically accurate simulation of molecule-surface reactions, G.J. Kroes, Phys. Chem. Chem. Phys.14, 14966-14981 (2012)".

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