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

Autor: Lischka H; Department of Chemistry and Biochemistry, Texas Tech University, Lubbock, Texas 79409, USA., Shepard R; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, USA., Müller T; Institute for Advanced Simulation, Jülich Supercomputing Centre, Forschungszentrum Jülich, Jülich 52428, Germany., Szalay PG; ELTE Eötvös Loránd University, Institute of Chemistry, Budapest, Hungary., Pitzer RM; Department of Chemistry and Biochemistry, The Ohio State University, Columbus, Ohio 43210, USA., Aquino AJA; School of Pharmaceutical Sciences and Technology, Tianjin University, Tianjin 300072, People's Republic of China., Araújo do Nascimento MM; Universidade Federal da Paraíba, 58059-900 João Pessoa, PB, Brazil., Barbatti M; Aix Marseille University, CNRS, ICR, Marseille, France., Belcher LT; Laser and Optics Research Center, Department of Physics, US Air Force Academy, Colorado 80840, USA., Blaudeau JP; PRKK, LLC, 1424 NW Coconut LN, Stuart, Florida 34994, USA., Borges I Jr; Departamento de Química, Instituto Militar de Engenharia, Rio de Janeiro, RJ 22290-270, Brazil., Brozell SR; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, USA., Carter EA; Office of the Chancellor and Department of Chemical and Biomolecular Engineering, University of California, Los Angeles, Box 951405, Los Angeles, California 90095-1405, USA., Das A; Indian Institute of Engineering Science and Technology, Shibpur, Howrah, India., Gidofalvi G; Department of Chemistry and Biochemistry, Gonzaga University, Spokane, Washington 99258, USA., González L; Institute of Theoretical Chemistry, Faculty of Chemistry, University of Vienna, Währinger Straße 17, 1090 Vienna, Austria., Hase WL; Department of Chemistry and Biochemistry, Texas Tech University, Lubbock, Texas 79409, USA., Kedziora G; Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433, USA., Kertesz M; Department of Chemistry, Georgetown University, 37th and O Streets, NW, Washington, DC 20057-1227, USA., Kossoski F; Aix Marseille University, CNRS, ICR, Marseille, France., Machado FBC; Departamento de Química, Instituto Tecnológico de Aeronáutica, São José dos Campos 12228-900, São Paulo, Brazil., Matsika S; Department of Chemistry, Temple University, 1901 N. 13th St., Philadelphia, Pennsylvania 19122, USA., do Monte SA; Universidade Federal da Paraíba, 58059-900 João Pessoa, PB, Brazil., Nachtigallová D; Institute of Organic Chemistry and Biochemistry v.v.i., The Czech Academy of Sciences, Flemingovo nám. 2, 160610 Prague 6, Czech Republic., Nieman R; Department of Chemistry and Biochemistry, Texas Tech University, Lubbock, Texas 79409, USA., Oppel M; Institute of Theoretical Chemistry, Faculty of Chemistry, University of Vienna, Währinger Straße 17, 1090 Vienna, Austria., Parish CA; Department of Chemistry, Gottwald Center for the Sciences, University of Richmond, Richmond, Virginia 23173, USA., Plasser F; Department of Chemistry, Loughborough University, Loughborough LE11 3TU, United Kingdom., Spada RFK; Departamento de Física, Instituto Tecnológico de Aeronáutica, São José dos Campos 12228-900, São Paulo, Brazil., Stahlberg EA; Biomedical Informatics and Data Science, Frederick National Laboratory for Cancer Research, Frederick, Maryland 21702, USA., Ventura E; Universidade Federal da Paraíba, 58059-900 João Pessoa, PB, Brazil., Yarkony DR; Department of Chemistry, Johns Hopkins University, 3400 N. Charles Street, Baltimore, Maryland 21218, USA., Zhang Z; Stanford Research Computing Center, Stanford University, 255 Panama Street, Stanford, California 94305, USA.
Jazyk: angličtina
Zdroj: The Journal of chemical physics [J Chem Phys] 2020 Apr 07; Vol. 152 (13), pp. 134110.
DOI: 10.1063/1.5144267
Abstrakt: 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.
Databáze: MEDLINE