English

Self-Interaction Correction in Water-Ion Clusters

Chemical Physics 2021-03-17 v1

Abstract

We study the importance of self-interaction errors in density functional approximations for various water-ion clusters. We have employed the Fermi-L\"owdin orbital self-interaction correction (FLOSIC) method in conjunction with LSDA, PBE, and SCAN to describe binding energies of hydrogen-bonded water-ion clusters, \textit{i.e.}, water-hydronium, water-hydroxide, water-halide, as well as non-hydrogen-bonded water-alkali clusters. In the hydrogen-bonded water-ion clusters, the building blocks are linked by hydrogen atoms, although the links are much stronger and longer-ranged than the normal hydrogen bonds between water molecules, because the monopole on the ion interacts with both permanent and induced dipoles on the water molecules. We find that self-interaction errors overbind the hydrogen-bonded water-ion clusters and that FLOSIC reduces the error and brings the binding energies into closer agreement with higher-level calculations. The non-hydrogen-bonded water-alkali clusters are not significantly affected by self-interaction errors. Self-interaction corrected PBE predicts the lowest mean unsigned error in binding energies (\leq 50 meV/\ce{H2O}) for hydrogen-bonded water-ion clusters. Self-interaction errors are also largely dependent on the cluster size, and FLOSIC does not accurately capture the subtle variation in all clusters, indicating the need for further refinement.

Keywords

Cite

@article{arxiv.2012.13469,
  title  = {Self-Interaction Correction in Water-Ion Clusters},
  author = {Kamal Wagle and Biswajit Santra and Puskar Bhattarai and Chandra Shahi and Mark R. Pederson and Koblar A. Jackson and John P. Perdew},
  journal= {arXiv preprint arXiv:2012.13469},
  year   = {2021}
}

Comments

13 pages, 9 figures

R2 v1 2026-06-23T21:24:16.706Z