High-Dimensional PES-Derived Free Energy Landscapes (2D PMF) of CO on Pt(111): A Coverage-Temperature Bivariate Dataset

Overview This repository contains a comprehensive bivariate dataset of two-dimensional Potential of Mean Force (2D PMF) landscapes for carbon monoxide (CO) adsorption on the relaxed Pt(111) surface. The data spans 15 discrete coverages (ranging from low coverage to a saturation coverage of 0.750 ML) and 7 temperatures (from 300 K to 600 K at 50 K intervals), totaling 105 unique physical conditions. The free energy landscapes were derived from extensive finite-temperature molecular dynamics (MD) simulations. These simulations were driven by a high-precision, high-dimensional neural network potential energy surface (HD NN-PES) constructed via a many-body expansion strategy (explicitly including surface, single-molecule, and intermolecular interactions). This dataset serves as the fundamental evidence resolving the long-standing "CO/Pt(111) puzzle", dynamically illustrating phenomena such as the "Kinetic Gateway" at intermediate coverages (~0.611 ML) and "Thermodynamic Locking" at saturation limits (0.750 ML). Repository Structure 2DPMF_RawData.zip: Contains the 105 raw data files (.dat) extracted from MD trajectories. 2DPMF_figures.zip: Contains the rendered high-resolution 2D PMF contour maps (.pdf) for all evaluated coverages and temperatures. matlab_scripts.zip: Contains the MATLAB scripts used to process the raw data and plot the contour figures. Data Format and Naming Convention The raw data files within 2DPMF_RawData.zip are named following the format: PMF_HD_[Temperature]K_[Coverage].dat (e.g., PMF_HD_300K_0.361.dat). Each .dat file is structured as a matrix containing 90,000 rows and 4 columns. The columns are defined as follows: Column 1: Cartesian X coordinate of the CO molecule mapped onto a 2×2 Pt(111) surface supercell (Unit: Å). Column 2: Cartesian Y coordinate of the CO molecule mapped onto a 2×2 Pt(111) surface supercell (Unit: Å). Column 3: Relative Free Energy (ΔG) representing the potential of mean force (Unit: kcal/mol). Column 4: Occupancy number (statistical frequency) directly sampled from the MD trajectories. Usage Notes Researchers can easily reproduce the contour plots or conduct further thermodynamic and kinetic analyses using the provided MATLAB scripts. When plotting the PMF, Column 1 (X) and Column 2 (Y) serve as the spatial grid, while Column 3 (Free Energy) serves as the Z-axis for contour mapping. The occupancy numbers (Column 4) provide raw statistical weights for customized re-weighting or alternative free-energy calculations.