COLUMBUS─An Efficient and General Program Package for Ground and Excited State Computations Including Spin–Orbit Couplings and Dynamics

Plasser, Felix [Loughborough University (United Kingdom); et al.] (ORCID:000000030751148X); Lischka, Hans [Department of Chemistry and Biochemistry; Texas Tech University] (ORCID:0000000256563975); Shepard, Ron [Chemical Sciences and Engineering Division; Argonne National Laboratory] (ORCID:0000000202720824); Szalay, Péter G. [Laboratoy of Theoretical Chemistry, Institute of Chemistry; ELTE Eötvös Loránd University] (ORCID:0000000318853557); Pitzer, Russell M. [Department of Chemistry and Biochemistry; The Ohio State University]; Alves, Rodolpho L. R. [Departamento de Química, CCEN; Universidade Federal da Paraíba]; Aquino, Adelia J. A. [Department of Mechanical Engineering; Texas Tech University] (ORCID:0000000348916512); Autschbach, Jochen [Department of Chemistry; University at Buffalo, State University of New York] (ORCID:000000019392877X); Barbatti, Mario [Aix Marseille University, CNRS, ICR; Institut Universitaire de France] (ORCID:0000000193366607); Carvalho, Jhonatas R. [Department of Chemistry and Biochemistry; Texas Tech University]; Chagas, Julio C. V. [Department of Chemistry; Aeronautics Institute of Technology; Advanced Scientific Computing and Modeling Laboratory; Aeronautics Institute of Technology; Department of Chemistry; Northwestern University] (ORCID:0000000196470821); González, Leticia [Institute of Theoretical Chemistry, Faculty of Chemistry; University of Vienna; Vienna Research Platform on Accelerating Photoreaction Discovery; University of Vienna] (ORCID:000000015112794X); Hansen, Andreas [Mulliken Center for Theoretical Chemistry; University of Bonn] (ORCID:0000000316598206); Jayee, Bhumika [Department of Chemistry and Biochemistry; Texas Tech University; Physical Sciences and Computational Division; Pacific Northwest National Laboratory]; Kertesz, Miklos [Chemistry Department and Institute of Soft Matter; Georgetown University] (ORCID:0000000279303260); Machado, Francisco B. C. [Department of Chemistry; Aeronautics Institute of Technology; Advanced Scientific Computing and Modeling Laboratory; Aeronautics Institute of Technology] (ORCID:0000000220643463); Matsika, Spiridoula [Department of Chemistry, Temple University, 1901 N 13th St, Philadelphia, Pennsylvania 19122, United States] (ORCID:0000000327733979); do Monte, Silmar A. [Departamento de Química, CCEN; Universidade Federal da Paraíba]; Mukherjee, Saikat [Faculty of Chemistry; Nicolaus Copernicus University in Torun] (ORCID:0000000200254735); Nachtigallová, Dana [Institute of Organic Chemistry and Biochemistry; Academy of Sciences of the Czech Republic; IT4Innovations; VŠBTechnical University of Ostrava] (ORCID:0000000295888625); Nieman, Reed [Department of Chemistry and Biochemistry; Texas Tech University] (ORCID:0000000330115223); Oliveira, Vytor P. [Department of Chemistry; Aeronautics Institute of Technology] (ORCID:0000000266147625); Oppel, Markus [Institute of Theoretical Chemistry, Faculty of Chemistry; University of Vienna] (ORCID:0000000163632310); Parish, Carol A. [Department of Chemistry, Gottwald Center for the Sciences; University of Richmond] (ORCID:0000000328783070); Pittner, Jiri [J. Heyrovsky Institute of Physical Chemistry, Academy of Sciences of the Czech Republic, v.v.i., Dolejškova 3, 18223 Praha 8, Czech Republic] (ORCID:0000000303978410); F. dos Santos, Luan G. [Department of Chemistry and Biochemistry; Texas Tech University] (ORCID:000000025979148X); Scrinzi, Armin [Department of Physics, Ludwig Maximilian University, Theresienstrasse 37, 80333 Munich, Germany]; Sit, Mahesh K. [J. Heyrovsky Institute of Physical Chemistry, Academy of Sciences of the Czech Republic, v.v.i., Dolejškova 3, 18223 Praha 8, Czech Republic]; Spada, Rene F. K. [Departamento de Física; Instituto Tecnológico de Aeronáutica]; Thodika, Mushir [National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, Colorado 80401, United States]; Valente, Daniel C. A. [Departamento de Física; Instituto Tecnológico de Aeronáutica]; Vázquez-Mayagoitia, Álvaro [Computational Science Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States] (ORCID:0000000214156300); Ventura, Elizete [Departamento de Química, CCEN; Universidade Federal da Paraíba]; Westermayr, Julia [Wilhelm-Ostwald-Institute for Physical and Theoretical Chemistry; Leipzig University; ScaDS.AI (Center for Scalable Data Analytics and Artificial Intelligence) Dresden/Leipzig] (ORCID:0000000265310742); Zaichenko, Aleksandr [Department of Chemistry; University at Buffalo, State University of New York]; Zhang, Zhiyong [Stanford Research Computing; Stanford University]

doi:10.1021/acs.jpca.5c02047

DOE OSTI · 2572513

COLUMBUS─An Efficient and General Program Package for Ground and Excited State Computations Including Spin–Orbit Couplings and Dynamics

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Abstract

The COLUMBUS program system provides the tools for performing high-level multireference (MR) computations, including the multireference configuration interaction (MRCI) method and its multireference averaged quadratic coupled cluster (MR-AQCC) extension, allowing computations on a wide range of fascinating atomic and molecular systems, including the treatment of open-shells and complicated excited state phenomena. The inclusion of spin−orbit coupling (SOC) directly within the MRCI step enables the description of systems containing heavy elements, such as lanthanides and actinides, whose properties are strongly influenced by SOC. Analytic energy gradients and nonadiabatic couplings at the correlated MRCI level provide the foundation for a variety of dynamics studies, giving insight into ultrafast photochemistry. New and ongoing method developments in COLUMBUS include the computation of spin densities, improved descriptions of ionic states, enhancements to the AQCC method, and the porting of COLUMBUS to graphical processing units (GPUs). New external interfaces enable an enhanced description of electronic resonances and molecules in strong laser fields. This work highlights these new developments while providing a detailed account of the diverse applications of COLUMBUS in recent years.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Chemical calculations Coupling reactions Energy Excited states Quantum Chemistry Quantum mechanics energy excited states multireference computations quantum chemistry spin-orbit coupling unpaired electrons

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Plasser, Felix [Loughborough University (United Kingdom); et al.] (ORCID:000000030751148X), Lischka, Hans [Department of Chemistry and Biochemistry; Texas Tech University] (ORCID:0000000256563975), Shepard, Ron [Chemical Sciences and Engineering Division; Argonne National Laboratory] (ORCID:0000000202720824), Szalay, Péter G. [Laboratoy of Theoretical Chemistry, Institute of Chemistry; ELTE Eötvös Loránd University] (ORCID:0000000318853557), Pitzer, Russell M. [Department of Chemistry and Biochemistry; The Ohio State University], Alves, Rodolpho L. R. [Departamento de Química, CCEN; Universidade Federal da Paraíba], Aquino, Adelia J. A. [Department of Mechanical Engineering; Texas Tech University] (ORCID:0000000348916512), Autschbach, Jochen [Department of Chemistry; University at Buffalo, State University of New York] (ORCID:000000019392877X), Barbatti, Mario [Aix Marseille University, CNRS, ICR; Institut Universitaire de France] (ORCID:0000000193366607), Carvalho, Jhonatas R. [Department of Chemistry and Biochemistry; Texas Tech University], Chagas, Julio C. V. [Department of Chemistry; Aeronautics Institute of Technology; Advanced Scientific Computing and Modeling Laboratory; Aeronautics Institute of Technology; Department of Chemistry; Northwestern University] (ORCID:0000000196470821), González, Leticia [Institute of Theoretical Chemistry, Faculty of Chemistry; University of Vienna; Vienna Research Platform on Accelerating Photoreaction Discovery; University of Vienna] (ORCID:000000015112794X), Hansen, Andreas [Mulliken Center for Theoretical Chemistry; University of Bonn] (ORCID:0000000316598206), Jayee, Bhumika [Department of Chemistry and Biochemistry; Texas Tech University; Physical Sciences and Computational Division; Pacific Northwest National Laboratory], Kertesz, Miklos [Chemistry Department and Institute of Soft Matter; Georgetown University] (ORCID:0000000279303260), Machado, Francisco B. C. [Department of Chemistry; Aeronautics Institute of Technology; Advanced Scientific Computing and Modeling Laboratory; Aeronautics Institute of Technology] (ORCID:0000000220643463), Matsika, Spiridoula [Department of Chemistry, Temple University, 1901 N 13th St, Philadelphia, Pennsylvania 19122, United States] (ORCID:0000000327733979), do Monte, Silmar A. [Departamento de Química, CCEN; Universidade Federal da Paraíba], Mukherjee, Saikat [Faculty of Chemistry; Nicolaus Copernicus University in Torun] (ORCID:0000000200254735), Nachtigallová, Dana [Institute of Organic Chemistry and Biochemistry; Academy of Sciences of the Czech Republic; IT4Innovations; VŠBTechnical University of Ostrava] (ORCID:0000000295888625), Nieman, Reed [Department of Chemistry and Biochemistry; Texas Tech University] (ORCID:0000000330115223), Oliveira, Vytor P. [Department of Chemistry; Aeronautics Institute of Technology] (ORCID:0000000266147625), Oppel, Markus [Institute of Theoretical Chemistry, Faculty of Chemistry; University of Vienna] (ORCID:0000000163632310), Parish, Carol A. [Department of Chemistry, Gottwald Center for the Sciences; University of Richmond] (ORCID:0000000328783070), Pittner, Jiri [J. Heyrovsky Institute of Physical Chemistry, Academy of Sciences of the Czech Republic, v.v.i., Dolejškova 3, 18223 Praha 8, Czech Republic] (ORCID:0000000303978410), F. dos Santos, Luan G. [Department of Chemistry and Biochemistry; Texas Tech University] (ORCID:000000025979148X), Scrinzi, Armin [Department of Physics, Ludwig Maximilian University, Theresienstrasse 37, 80333 Munich, Germany], Sit, Mahesh K. [J. Heyrovsky Institute of Physical Chemistry, Academy of Sciences of the Czech Republic, v.v.i., Dolejškova 3, 18223 Praha 8, Czech Republic], Spada, Rene F. K. [Departamento de Física; Instituto Tecnológico de Aeronáutica], Thodika, Mushir [National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, Colorado 80401, United States], Valente, Daniel C. A. [Departamento de Física; Instituto Tecnológico de Aeronáutica], Vázquez-Mayagoitia, Álvaro [Computational Science Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States] (ORCID:0000000214156300), Ventura, Elizete [Departamento de Química, CCEN; Universidade Federal da Paraíba], Westermayr, Julia [Wilhelm-Ostwald-Institute for Physical and Theoretical Chemistry; Leipzig University; ScaDS.AI (Center for Scalable Data Analytics and Artificial Intelligence) Dresden/Leipzig] (ORCID:0000000265310742), Zaichenko, Aleksandr [Department of Chemistry; University at Buffalo, State University of New York], Zhang, Zhiyong [Stanford Research Computing; Stanford University]. 2025-07-08. COLUMBUS─An Efficient and General Program Package for Ground and Excited State Computations Including Spin–Orbit Couplings and Dynamics. https://doi.org/10.1021/acs.jpca.5c02047

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