JCP19-AR-ESS2020-05373_accepted.pdf (6.99 MB)

The generality of the GUGA MRCI approach in COLUMBUS for treating complex quantum chemistry

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journal contribution
posted on 21.04.2020, 13:20 by Hans Lischka, Ron Shepard, Thomas Müller, Péter G Szalay, Russell M Pitzer, Adelia JA Aquino, Mayzza M Araújo do Nascimento, Mario Barbatti, Lachlan T Belcher, Jean-Philippe Blaudeau, Itamar Borges, Scott R Brozell, Emily A Carter, Anita Das, Gergely Gidofalvi, Leticia González, William L Hase, Gary Kedziora, Miklos Kertesz, Fábris Kossoski, Francisco BC Machado, Spiridoula Matsika, Silmar A do Monte, Dana Nachtigallová, Reed Nieman, Markus Oppel, Carol A Parish, Felix Plasser, Rene FK Spada, Eric A Stahlberg, Elizete Ventura, David R Yarkony, Zhiyong Zhang
The core part of the program system COLUMBUS allows highly efficient calculations using variational multireference (MR) methods in the framework of configuration interaction with single and double excitations (MR-CISD) and averaged quadratic coupled-cluster calculations (MR-AQCC), based on uncontracted sets of configurations and the graphical unitary group approach (GUGA). The availability of analytic MR-CISD and MR-AQCC energy gradients and analytic nonadiabatic couplings for MR-CISD enables exciting applications including, e.g., investigations of π-conjugated biradicaloid compounds, calculations of multitudes of excited states, development of diabatization procedures, and furnishing the electronic structure information for on-the-fly surface nonadiabatic dynamics. With fully variational uncontracted spin-orbit MRCI, COLUMBUS provides a unique possibility of performing high-level calculations on compounds containing heavy atoms up to lanthanides and actinides. Crucial for carrying out all of these calculations effectively is the availability of an efficient parallel code for the CI step. Configuration spaces of several billion in size now can be treated quite routinely on standard parallel computer clusters. Emerging developments in COLUMBUS, including the all configuration mean energy multiconfiguration self-consistent field method and the graphically contracted function method, promise to allow practically unlimited configuration space dimensions. Spin density based on the GUGA approach, analytic spin-orbit energy gradients, possibilities for local electron correlation MR calculations, development of general interfaces for nonadiabatic dynamics, and MRCI linear vibronic coupling models conclude this overview.

History

School

  • Science

Department

  • Chemistry

Published in

Journal of Chemical Physics

Volume

152

Issue

13

Citation

Lischka, H. ... et al. 2020. The generality of the GUGA MRCI approach in COLUMBUS for treating complex quantum chemistry. Journal of Chemical Physics, 152(13): 134110.

Publisher

AIP Publishing

Version

AM (Accepted Manuscript)

Rights holder

© The authors

Publisher statement

This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This article appeared in Lischka, H. ... et al. 2020. The generality of the GUGA MRCI approach in COLUMBUS for treating complex quantum chemistry. Journal of Chemical Physics, 152(13): 134110 and may be found at https://doi.org/10.1063/1.5144267

Acceptance date

01/03/2020

Publication date

2020-04-06

Copyright date

2020

Notes

Paper published as part of the special topic on Electronic Structure Software. Note: This article is part of the JCP Special Topic on Electronic Structure Software

ISSN

0021-9606

eISSN

1089-7690

Language

en

Depositor

Dr Felix Plasser Deposit date: 14 April 2020

Article number

134110

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