** Reference to paper: https://pubs.acs.org/doi/10.1021/acs.jpcc.0c03756 ** DOI: 10.1021/acs.jpcc.0c03756 ** Title: Closing the Gap Between Experiment and Theory: Reactive Scattering of HCl from Au(111) ** Authors: Gerrits, Nick; Geweke, Jan; Smeets, Egidius; Voss, Johannes; Wodtke, Alec; Kroes, Geert-Jan ** Contact e-mail: n.gerrits@lic.leidenuniv.nl g.j.kroes@chem.leidenuniv.nl ** Abstract: Accurate simulation of molecules reacting on metal surfaces, which can help in improving heterogeneous catalysts, remains out of reach for several reactions. For example, a large disagreement between theory and experiment for HCl reacting on Au(111) still remains, despite many efforts. In this work, the dissociative chemisorption of HCl on Au(111) is investigated with a recently developed MGGA density functional (MS-RPBEl) and a high-dimensional neural network potential. Additionally, previous experimental sticking probabilities are re-examined. A considerably improved agreement between experiment and theory is obtained, although theory still overestimates experimental sticking probabilities by a factor 2 to 7 at the highest incidence energy. Computed and measured vibrational transition probabilities are also in improved agreement. Several dynamical effects such as angular steering and energy transfer from the molecule to the surface are found to play an important role. ** Description per file: The program used for DFT is VASP v5.4.4 with a special modification (made by Egidius Smeets) in order to use the MS-RPBEl functional and with VTST (http://theory.cm.utexas.edu/vtsttools/index.html). Molecular dynamics (MD) are performed with LAMMPS (version 16Mar18). All figures are made with matplotlib 3.0, except figure 1 which was made with mathematica by Jan Geweke and figure 3 which was made with Blender 1.79 and annoted with GIMP. MD data is not included as this would be too much to store. However, it should be easy to regenerate the data with the files included in this folder. ** Folder Barrier: POSCAR - The DFT minimum barrier geometry obtained for HCl + Au(111) at Ts=170 K. POSCAR_convergedinterlayer - Is the same as POSCAR, but employing a converged interlayer spacing (see SI for details) ** Folder Equilibrated_slabs: surface_snapshots.tar.gz - Contains all the equilibrated slabs and their snapshots used in the MD for the initial conditions. ** Folder LAMMPS: check-HCl-NN.py - Analyzes the trajectory (states.xyz) and outputs all the relevant information create_poscar.py - Creates the folders and POSCARs for the MD create_poscar_scratch_.py - Similar to create_poscar.py but does this on the fly per trajectory (better for massive jobs as it reduces traffic) dynamics-sub.py - Submits jobs on a cluster energytransfer.py - Analyzes the energy transfer after a trajectory is finished Genlammps_AIMD.py - Converts a POSCAR to an XYZ file that is suitable for LAMMPS Job_mob_ - The job file for the cluster sim.lmp - Input file of LAMMPS submit-dynamics.py - Submits jobs for several different initial conditions on a cluster Traj_Analysis.py - Analyzes of the reaction probability ** Folder RuNNer: All the input files required for RuNNer or LAMMPS to perform the calculations with the HD-NNP. ** Folder SurfaceEquilibration: Contains all the files required for running surface equilibration and obtaining the snapshots in the Equilibrated_slabs folder. All the figures: ** Folder Figure01: cvd_ex_plot.png ** Folder Figure02: reactionprobability.pdf plotsticking.py - Generates the plot sticking_data.py - Contains the sticking probabilities ** Folder Figure03: coordinatesystem.pdf ** Folder Figure04: elbow_multi.pdf draw_elbow_multipanel.py - Generates the plot phi_scan* - The original version of finding the MEP, and the modifications that were required to find the MEP on some of the elbows *_relaxed - The data of the elbow plots and their individual elbow plots ** Folder Figure05: top_elbow_theta_multi.pdf draw_elbow_multi.py - Generates the plot energy.dat - Contains the data phi_scan* - The original version of finding the MEP, and the modifications that were required to find the MEP on some of the elbows ** Folder Figure06: coupling.pdf plotcoupling.py - Generates the plot ** Folder Figure07: reactionprobability_surfacemotion.pdf plotsticking_surfacemotion.py - Generates the plot, requires sticking_data.py (Figure02) ** Folder Figure08: reactionprobability_vibrational.pdf plotsticking_vibrational.py - Generates the plot, requires sticking_data.py (Figure02) ** Folder Figure09: Tvjprobability.pdf plotTvj.py - Generates the plot Note that for the MD concerning the transition probabilities dt=0.2 fs is employed instead of dt=0.4 fs. The time step does not influence the reaction probability but it does have a small effect on the transition probability. It is possible that this is partially due to how the analysis works in the check script since the energy conservation error is reasonable (see article). ** Folder Figure10: energytransfer.pdf plotenergytransfer.py - Generates the plot ** Folder Figure11: translationJ.pdf plottranslationJ.py - Generates the plot ** Folder Figure12: ET_site.pdf Analysis_ET_site.py - Generates the plot, requires the analysis of the check script ** Folder Figure13: xysteering.pdf Analysis_xysteering.py - Generates the plot, requires the analysis of the check script ** Folder Figure14: site_density.pdf Analysis_site_density.py - Generates the plot, requires the analysis of the check script ** Folder Figure15: Zts.pdf plotzts.py - Generates the plot ** Folder Figure16: angles.pdf Analysis_angle.py - Generates the plot, requires the analysis of the check script ** Folder Figure17: reactionsite_p.pdf plotreactionsite_p.py - Generates the plot ** Folder FigureS1: convergence.pdf plotconvergence.py - Generates the plot ** Folder FigureS2: errorfraction.pdf errorfraction_plot.py - Generates the plot. Requires one to generate data files that contain the errors w.r.t. DFT calculations. ** Folder FigureS3 plotreactioncoordinate.py - Generates the plot reactioncoordinate.pdf ** Folder FigureS4 plotreactionsite_p_v2.py - Generates the plot reactionsite_p_v2.pdf ** Folder FigureS5 Analysis_vj_scattering_angle.py - Obtains the transition probability of MD plotTvj_scatteringangle.py - Generates the plot Tvjprobability_angle.pdf ** Folder FigureS6 Analysis_vj.py - Obtains the transition probability of MD plotTvj_beamparameters.py - Generates the plot Tvjprobability_beamparameters.pdf ** Folder FigureS7 draw_elbow_lines.py - Generates the plot energy.dat - Contains the energies to generate the plot TS_elbow_lines.pdf ** Folder FigureS8 barrier_theta_phi_*.dat - Barrier energies barrier_theta_phi.pdf draw_theta_phi_barrier.py - Generates the plot Other files: