A finite-element Delta-Sternheimer approach for accurate all-electron RPA correlation energies of arbitrary molecules
Authors
Hao Peng
Haochen Liu
Chuhao Li
Hehu Xie
Xinguo Ren
Abstract
The incompleteness of single-particle basis sets has long cast a shadow over correlated electronic-structure methods, making it highly challenging to obtain numerically converged results. In this work, we compute the RPA correlation energies of general molecules using the finite element method, while ingeniously combining atomic orbital basis sets to accelerate the convergence of total energies. We report atomization energies for 50 molecules within the RPA framework, achieving accuracies on the order of meV per atom. The computational strategy that integrates real-space discretization techniques with atomic orbitals is expected to inspire the entire correlated electronic-structure community.
