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dc.contributor.authorKonecny, Lukas
dc.contributor.authorKadek, Marius
dc.contributor.authorKomorovsky, Stanislav
dc.contributor.authorRuud, Kenneth
dc.contributor.authorRepisky, Michal
dc.date.accessioned2018-12-17T14:36:00Z
dc.date.available2018-12-17T14:36:00Z
dc.date.issued2018-11-27
dc.description.abstractWe present an implementation and application of electron dynamics based on real-time time-dependent density functional theory (RT-TDDFT) and relativistic 2-component X2C and 4-component Dirac–Coulomb (4c) Hamiltonians to the calculation of electron circular dichroism and optical rotatory dispersion spectra. In addition, the resolution-of-identity approximation for the Coulomb term (RI-J) is introduced into RT-TDDFT and formulated entirely in terms of complex quaternion algebra. The proposed methodology was assessed on the dimethylchalcogenirane series, C<sub>4</sub>H<sub>8</sub>X (X = O, S, Se, Te, Po, Lv), and the spectra obtained by non-relativistic and relativistic methods start to disagree for Se and Te, while dramatic differences are observed for Po and Lv. The X2C approach, even in its simplest one-particle form, reproduces the reference 4c results surprisingly well across the entire series while offering an 8-fold speed-up of the simulations. An overall acceleration of RT-TDDFT by means of X2C and RI-J increases with system size and approaches a factor of almost 25 when compared to the full 4c treatment, without compromising the accuracy of the final spectra. These results suggest that one-particle X2C electron dynamics with RI-J acceleration is an attractive method for the calculation of chiroptical spectra in the valence region.en_US
dc.description.sponsorshipMinistry of Education of the Slovak Republic Slovak Academy of Sciences VEGA The Ministry of Education, Youth and Sports of the Czech Republic Slovak Research and Development Agency European Union Slovak Academy of Sciencesen_US
dc.descriptionThis article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. The following article, Konecny, L., Kadek, M., Komorovsky, S., Ruud, K. & Repisky, M. (2018). Resolution-of-identity accelerated relativistic two- and four-component electron dynamics approach to chiroptical spectroscopies. <i>Journal of Chemical Physics</i>, 149, 204104, appeared in <i>Journal of Chemical Physics</i> and may be found at <a href=https://doi.org/10.1063/1.5051032> https://doi.org/10.1063/1.5051032</a>.en_US
dc.identifier.citationKonecny, L., Kadek, M., Komorovsky, S., Ruud, K. & Repisky, M. (2018). Resolution-of-identity accelerated relativistic two- and four-component electron dynamics approach to chiroptical spectroscopies. <i>Journal of Chemical Physics</i>, 149, 204104. https://doi.org/10.1063/1.5051032en_US
dc.identifier.cristinIDFRIDAID 1628085
dc.identifier.issn0021-9606
dc.identifier.issn1089-7690
dc.identifier.urihttps://hdl.handle.net/10037/14363
dc.language.isoengen_US
dc.publisherAIP Publishingen_US
dc.relation.journalJournal of Chemical Physics
dc.relation.projectIDinfo:eu-repo/grantAgreement/RCN/SFF /262695/Norway/Hylleraas Centre for Quantum Molecular Sciences//en_US
dc.rights.accessRightsopenAccessen_US
dc.subjectVDP::Mathematics and natural science: 400::Chemistry: 440en_US
dc.subjectVDP::Matematikk og Naturvitenskap: 400::Kjemi: 440en_US
dc.titleResolution-of-identity accelerated relativistic two- and four-component electron dynamics approach to chiroptical spectroscopiesen_US
dc.typeJournal articleen_US
dc.typeTidsskriftartikkelen_US
dc.typePeer revieweden_US


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