The quantum dynamics of H2 on Cu(111) at a surface temperature of 925 K: Comparing state-of-the-art theory to state-of-the-art experiments

** Authors:

B. Smits
M. F. Somers

** Contact e-mail:

b.smits@lic.leidenuniv.nl
m.somers@chem.leidenuniv.nl

** Abstract:

We present results on our recently expanded static corrugation model (SCM) approach to including the relevant surface temperature effects, applied to the dissociative chemisorption reaction of H$_{2}$ on a Cu(111).
The reaction and rovibrationally elastic scattering probabilities we obtain at a quantum dynamical (QD) level, as an average of many statically distorted surface configurations, show great agreement with those of a dynamic surface model, which reinforces the validity of the sudden approximation inherent to the SCM.
We further investigate several simple methods of binning the final rovibrational state of quasi-classical dynamics simulations, to find those best suited to reproduce QD results for our system.
Finally, we show that the SCM obtained results reproduce experimental dissociation curves very well, when the uncertainty in experimental saturation values are taken into account.
Some indication of a slow channel, so far only observed in experiment, can also be found at low incidence energies, although more rigorous QD simulations are required to reduce the noise inherent to our propagation methods.

** Folder FIG12:

Data files for the QD-BOSS and QD-SCM results, as well as the QCD-BOSS, -SCM, and -DCM results binned using both the discussed standard and weighted binning methods.
Files include the reaction probabilities, as well as final state scattering results and some other data, for each incidence energy.

IMPORTANT: For the QCD results, direct and indirect reaction are included separately.

** Folder FIG34:

Data files for the QD-BOSS and QD-SCM results, as well as the QCD-BOSS, -SCM, and -DCM results binned using the discussed standard, weighted and floor binning methods.
Files include the reaction probabilities, as well as final state scattering results and some other data, for each incidence energy.
For elastic scattering, find the column matching the initial rovibrational state.

IMPORTANT: For the QCD results, direct and indirect reaction are included separately.

** Folder FIG567:

Again the same data files for the QD-BOSS and QD-SCM results, as well as the QCD-BOSS, -SCM, and -DCM results binned using the discussed standard binning methods.
Included in Experiment_Parameters.dat is the way we constructed the experimental curves, using the parameters as published by the respective groups.