2025/05/09 by Edoardo Spadetto, Spadetto, Edoardo, Pier Philipsen +5 · 1 citation
Engineering · Materials Science · Physics and Astronomy · #Advanced Chemical Physics Studies #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Machine Learning in Materials Science #Materials Science (cond-mat.mtrl-sci) #Surface Chemistry and Catalysis
paper · pdf · doi:10.48550/arxiv.2505.06021
openalex publication_date 2025/05/09 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
The random phase approximation (RPA) has emerged as a prominent first-principles method in material science, particularly to study the adsorption and chemisorption of small molecules on surfaces. However, its widespread application is hampered by its relatively high computational cost. Here, we present a well-parallelised implementation of the RPA with localised atomic orbitals and pair-atomic density fitting, which is especially suitable for studying two-dimensional systems. Through a dual k-grid scheme, we achieve fast and reliable convergence of RPA correlation energies to the thermodynamic limit. We demonstrate the efficacy of our implementation through an application to the adsorption of CO on MgO(001) using PBE input orbitals (RPA@PBE) Our calculated adsorption energy is in good agreement with previously published RPA@PBE studies, but, as expected, overestimates the experimentally available adsorption energies as well as recent CCSD(T) results.