Local embedding of coupled cluster theory into the random phase approximation using plane waves

Author(s)
Tobias Schäfer, Florian Libisch, Georg Kresse, Andreas Grüneis
Abstract

We present an embedding approach to treat local electron correlation effects in periodic environments. In a single consistent framework, our plane wave based scheme embeds a local high-level correlation calculation [here, Coupled Cluster (CC) theory], employing localized orbitals, into a low-level correlation calculation [here, the direct Random Phase Approximation (RPA)]. This choice allows for an accurate and efficient treatment of long-range dispersion effects. Accelerated convergence with respect to the local fragment size can be observed if the low-level and high-level long-range dispersions are quantitatively similar, as is the case for CC in RPA. To demonstrate the capabilities of the introduced embedding approach, we calculate adsorption energies of molecules on a surface and in a chabazite crystal cage, as well as the formation energy of a lattice impurity in a solid at the level of highly accurate many-electron perturbation theories. The absorption energy of a methane molecule in a zeolite chabazite is converged with an error well below 20 meV at the CC level. As our largest periodic benchmark system, we apply our scheme to the adsorption of a water molecule on titania in a supercell containing more than 1000 electrons.

Organisation(s)
Computational Materials Physics
External organisation(s)
Technische Universität Wien
Journal
Journal of Chemical Physics
Volume
154
No. of pages
6
ISSN
0021-9606
DOI
https://doi.org/10.1063/5.0036363
Publication date
01-2021
Peer reviewed
Yes
Austrian Fields of Science 2012
103006 Chemical physics, 103018 Materials physics
Portal url
https://ucris.univie.ac.at/portal/en/publications/local-embedding-of-coupled-cluster-theory-into-the-random-phase-approximation-using-plane-waves(2f92cfa9-e7f0-427e-9a29-c8a6092d5162).html