Accelerating the coupled-cluster singles and doubles method using the chain-of-sphere approximation

• Published in: Molecular Physics
• Main Authors: Dutta, A., Neese, F., Izsák, R.
• Format: Article in Journal/Newspaper
• Language: English
• Published: 2018
• Subjects: Orca
• Online Access: http://hdl.handle.net/21.11116/0000-0007-6E41-5

In this paper, we present a chain-of-sphere implementation of the external exchange term, the computational bottleneck of coupled-cluster calculations at the singles and doubles level. This implementation is compared to standard molecular orbital, atomic orbital and resolution of identity implementations of the same term within the ORCA package and turns out to be the most efficient one for larger molecules, with a better accuracy than the resolution-of-identity approximation. Furthermore, it becomes possible to perform a canonical CC calculation on a tetramer of nucleobases in 17 days, 20 hours.