Vis enkel innførsel

dc.contributor.authorDi Remigio, Roberto
dc.contributor.authorBeerepoot, Maarten
dc.contributor.authorCornaton, Yann
dc.contributor.authorRingholm, Magnus
dc.contributor.authorSteindal, Arnfinn Hykkerud
dc.contributor.authorRuud, Kenneth
dc.contributor.authorFrediani, Luca
dc.date.accessioned2017-03-29T13:37:32Z
dc.date.available2017-03-29T13:37:32Z
dc.date.issued2016-11-15
dc.description.abstractThe study of high-order absorption properties of molecules is a field of growing importance. Quantumchemical studies can help design chromophores with desirable characteristics. Given that most experiments are performed in solution, it is important to devise a cost-effective strategy to include solvation effects in quantum-chemical studies of these properties. We here present an open-ended formulation of selfconsistent field (SCF) response theory for a molecular solute coupled to a polarizable continuum model (PCM) description of the solvent. Our formulation relies on the open-ended, density matrix-based quasienergy formulation of SCF response theory of Thorvaldsen, et al., [J. Chem. Phys., 2008, 129, 214108] and the variational formulation of the PCM, as presented by Lipparini et al., [J. Chem. Phys., 2010, 133, 014106]. Within the PCM approach to solvation, the mutual solute–solvent polarization is represented by means of an apparent surface charge (ASC) spread over the molecular cavity defining the solute–solvent boundary. In the variational formulation, the ASC is an independent, variational degree of freedom. This allows us to formulate response theory for molecular solutes in the fixed-cavity approximation up to arbitrary order and with arbitrary perturbation operators. For electric dipole perturbations, pole and residue analyses of the response functions naturally lead to the identification of excitation energies and transition moments. We document the implementation of this approach in the Dalton program package using a recently developed open-ended response code and the PCMSolver libraries and present results for one-, two-, three-, four- and five-photon absorption processes of three small molecules in solution.en_US
dc.description.sponsorshipThe authors acknowledge support from the Research Council of Norway through a Centre of Excellence Grant (Grant No. 179568/V30), from the European Research Council through a Starting Grant (Grant No. 279619) and from the Norwegian Supercomputer Program through a grant for computer time (Grant No. NN4654K). A. H. S. acknowledges financial support from Tromsø Forskningsstiftelse (SurfInt grant)en_US
dc.descriptionPublished version. Source at <a href=http://doi.org/10.1039/C6CP06814F>http://doi.org/10.1039/C6CP06814F</a>. License – <a href= https://creativecommons.org/licenses/by/3.0/>CC BY 3.0</a>.en_US
dc.identifier.citationPhys. Chem. Chem. Phys., 2017,19, 366-379en_US
dc.identifier.issn1463-9084
dc.identifier.issn1463-9076
dc.identifier.otherFRIDAID 1407184
dc.identifier.other10.1039/C6CP06814F
dc.identifier.urihttp://hdl.handle.net/10037/10892
dc.language.isoengen_US
dc.publisherRoyal Society of Chemistryen_US
dc.relation.projectIDinfo:eu-repo/grantAgreement/RCN/FundingProgram/179568/Norway///en_US
dc.relation.projectIDinfo:eu-repo/grantAgreement/EC/FundingProgram/279619/EU///en_US
dc.rights.accessRightsopenAccessen_US
dc.subjectVDP::Matematikk og Naturvitenskap: 400::Kjemi: 440en_US
dc.subjectVDP::Mathematics and natural science: 400::Chemistry: 440en_US
dc.titleOpen-ended formulation of self-consistent field response theory with the polarizable continuum model for solvationen_US
dc.typeJournal articleen_US
dc.typeTidsskriftartikkelen_US
dc.typePeer revieweden_US


Tilhørende fil(er)

Denne innførselen finnes i følgende samling(er)

Vis enkel innførsel