On the Covalent Fields of Molecule–Surface Interactions

Contents

Reference structures.* The PtPdAuAgCu high-entropy alloy (HEA) nanoparticle (55 atoms, equimolar fcc composition) and the partially reduced high-entropy oxide (HEO) surface slab, as used without further relaxation as field-generating references R\mathcal{R} R.

Surface manifolds. Quadrilateral meshes fitted to both reference structures at probe-surface distances spanning 1.5–3.5 Å, including vertex coordinates, face connectivity, and surface normal vectors.

*Covalent field evaluations.* Interaction energies for atomic and molecular probes (∗* ∗C, ∗* ∗O, ∗* ∗CO, ∗* ∗H, ∗* ∗OH, ∗* ∗N, ∗* ∗NH, ∗* ∗NH₂, ∗* ∗CH, ∗* ∗CH₂, ∗* ∗CH₃, ∗* ∗NNH, glycerol) evaluated at each manifold vertex using MACE-MH1-r2scan. Includes scalar, anisotropic (36 orientations per vertex), and spectral field data where applicable.

*NEB calculations.* Eleven-image climbing-image NEB chains for the ∗* ∗C + ∗* ∗O → ∗* ∗CO reaction on the HEA nanoparticle, including all images, energies, and forces.

*PMD analysis.* PMD probe geometries, anisotropic field evaluations (10° increments), intrinsic barrier fields, and the full set of ~120,000 candidate reaction pathways with initial-state, PMD, and final-state energies.

Local minima. Relaxed adsorption geometries for all intermediates used as reference points in the computational tractability benchmarks.

Computational details

All interaction energies were evaluated with MACE-MH1-r2scan interfaced through the Atomic Simulation Environment (ASE). No additional DFT calculations were performed; the reference structures are taken from Arce-Ramos et al. (HEA) and Han et al. (HEO) as cited in the manuscript.

File format

Structures are provided in extxyz format and comma-separated tables (.csv) with column headers matching the notation of the manuscript. 

Software

The CFT framework used to generate all field evaluations is available at https://github.com/schwallergroup/CFT. A notebook pointing towards the data contained in the zenodo repository gives context to the indixidual files.