@article{b53680d1a4014480be8d773cadae50a2,
title = "The generality of the GUGA MRCI approach in COLUMBUS for treating complex quantum chemistry",
abstract = "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.",
author = "Hans Lischka and Ron Shepard and Thomas M{\"u}ller and Szalay, {P{\'e}ter G.} and Pitzer, {Russell M.} and Aquino, {Adelia J.A.} and {Ara{\'u}jo Do Nascimento}, {Mayzza M.} and Mario Barbatti and Belcher, {Lachlan T.} and Blaudeau, {Jean Philippe} and Itamar Borges and Brozell, {Scott R.} and Carter, {Emily A.} and Anita Das and Gergely Gidofalvi and Leticia Gonz{\'a}lez and Hase, {William L.} and Gary Kedziora and Miklos Kertesz and F{\'a}bris Kossoski and Machado, {Francisco B.C.} and Spiridoula Matsika and {Do Monte}, {Silmar A.} and Dana Nachtigallov{\'a} and Reed Nieman and Markus Oppel and Parish, {Carol A.} and Felix Plasser and Spada, {Rene F.K.} and Stahlberg, {Eric A.} and Elizete Ventura and Yarkony, {David R.} and Zhiyong Zhang",
note = "Funding Information: R.S. and S.R.B. were supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Gas Phase Chemical Physics Program, through Argonne National Laboratory under Contract No. DE-AC02-06CH11357. E.A.C. is grateful for support from the U.S. Department of Energy, Office of Science, Offices of Basic Energy Sciences and Advanced Scientific Computing Research, Scientific Discovery through Advanced Computing, via Award No. DE-AC02-05CH11231. S.M. was funded by the Department of Energy, Award No. DEFG02-08ER15983. L.T.B. was funded by the High-Energy Laser Joint Technology Office, Albuquerque, NM. D.R.Y was supported by the US Department of Energy (Grant No. DE-SC0015997). C.P. acknowledges support from the Department of Energy (Grant No. DE-SC0001093), the National Science Foundation (Grant Nos. CHE-1213271 and CHE-18800014), and the donors of the American Chemical Society Petroleum Research Fund. P.G.S. was supported by the National Research, Innovation and Development Fund (NKFIA), Grant No. 124018. H.L. and A.J.A.A. are grateful for support from the School of Pharmaceutical Science and Technology (SPST), Tianjin University, Tianjin, China, including computer time on the SPST computer cluster Arran. M.B. and F.K. thank the support of the Excellence Initiative of Aix-Marseille University (AMIDEX), the project Equip@Meso (Grant No. ANR-10-EQPX-29-01), and the WSPLIT project (Grant No. ANR-17-CE05-0005-01). D.N. acknowledges support from the Czech Science Foundation (Grant No. GA18-09914S). S.A.d.M., E.V., and M.M.A.d.N. were funded by the Brazilian agencies: Coordination for the Improvement of Higher Education Personnel (CAPES); Conselho Nacional de Desenvolvimento Cient{\'i}fico e Tecnol{\'o}gico (CNPq), Project Nos. 303884/2018-5 and 423112/2018-0; and Financier of Innovation and Research (FINEP). The authors also acknowledge computer time at the Supercomputer Center of the Federal University of Rio Grande do Sul (CESUP-UFRGS). R.F.K.S. acknowledges Fundac{\~a}o de Amparo {\`a} Pesquisa do Estado de S{\~a}o Paulo (FAPESP) under Grant No. 2019/07671-4 and CNPq under Grant Nos. 407760/2018-0 and 305788/2018-3. I.B. thanks CNPq through research Grant Nos. 304148/2018-0 and 409447/2018-8. F.B.C.M. gratefully acknowledges the financial assistance of the Brazilian agency CNPq under Project Nos. 307052/2016-8 and 404337/2016-3. F.B.C.M., A.J.A.A., and H.L. thank the FAPESP/Tianjin University SPRINT program (Project No. 2017/50157-4) for travel support. H.L., F.P., M.O., and L.G. acknowledge gratefully computer time at the computer cluster of the Vienna Scientific Cluster, Austria, under Project Nos. 70376, 70726, and 70264. * Publisher Copyright: {\textcopyright} 2020 Author(s).",
year = "2020",
month = apr,
day = "7",
doi = "10.1063/1.5144267",
language = "English (US)",
volume = "152",
journal = "Journal of Chemical Physics",
issn = "0021-9606",
publisher = "American Institute of Physics Publising LLC",
number = "13",
}