Extending the capabilities of Multi-Configurational short-range Density Functional Theory based methods

Erik Kjellgren

doi:10.21996/zt8y-x461

Extending the capabilities of Multi-Configurational short-range Density Functional Theory based methods

Erik Kjellgren

Publikation: Afhandling › Ph.d.-afhandling

267 Downloads (Pure)

Abstract

MC-srDFT modellen er en lovende model med hensyn til at give en god beskrivelse af komplekse molekylære systemer, der kræver både en multi-konfigurationel bølgefunktion samt en nøjagtig beskrivelse af kortrækkende interaktioner. Inden denne PhD afhandling kunne MC-srDFT modellen beskrive molekylære egenskaber inden for singlets lineære-respons teorien, samt udføre aben-skal beregninger. Alt sammen inden for srGGA tilnærmelsen.
Mulighederne for MC-srDFT-modellen er blevet udvidet til molekylære egenskaber, der kræver triplet lineær-respons. Denne nye mulighed er begrænset til singlet-reference bølgefunktioner. Desuden, er MC-srDFT modellen blevet udvidet til at gøre brug af MGGA tilnærmelsen. Indenfor denne tilnærmelse er der afledt og implementereret singlet lineær-respons, triplet lineær-respons og åben-skal bølgefunktions optimeringer.
Disse nyudviklede MC-srDFT metoder er blevet testet for systemer bestående af små molekyler samt for en række overgangsmetalkomplekser.
Gennem disse test-beregninger er det blevet vist, at MC-srDFT modellen er i stand til at give nøjagtige beregnede molekylære egenskaber. Overraskende nok blev det for de fleste testberegninger fundet at srLDA -funktionalet var lige så godt eller bedre end både srPBE- og srTPSS-funktionalerne.

Originalsprog	Engelsk
Bevilgende institution	Syddansk Universitet
Vejledere/rådgivere	Jensen, Hans Jørgen Aagaard, Hovedvejleder
Dato for forsvar	27. okt. 2021
Udgiver	Syddansk Universitet. Det Naturvidenskabelige Fakultet
DOI	https://doi.org/10.21996/zt8y-x461
Status	Udgivet - 11. apr. 2022

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10.21996/zt8y-x461

Thesis_erik_kjellgrenForlagets udgivne version, 9,88 MB

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Multi-configurational short-range density functional theory can describe spin–spin coupling constants of transition metal complexes
Kjellgren, E. R. & Jensen, H. J. A., 28. aug. 2021, I: The Journal of Chemical Physics. 155, 8, 13 s., 084102.
Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › peer review

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Dalton Project: A Python platform for molecular- and electronic-structure simulations of complex systems
Olsen, J. M. H., Reine, S., Vahtras, O., Kjellgren, E., Reinholdt, P., Hjorth Dundas, K. O., Li, X., Cukras, J., Ringholm, M., Hedegård, E. D., Di Remigio, R., List, N. H., Faber, R., Cabral Tenorio, B. N., Bast, R., Pedersen, T. B., Rinkevicius, Z., Sauer, S. P. A., Mikkelsen, K. V. & Kongsted, J. & 5 flere, Coriani, S., Ruud, K., Helgaker, T., Jensen, H. J. A. & Norman, P., 2020, I: The Journal of Chemical Physics. 152, 21, 18 s., 214115.
Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › peer review

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Triplet excitation energies from multiconfigurational short-range density-functional theory response calculations
Kjellgren, E. R., Hedegård, E. D. & Jensen, H. J. A., 2019, I: The Journal of Chemical Physics. 151, 12, 124113.
Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › peer review

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Citationsformater

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title = "Extending the capabilities of Multi-Configurational short-range Density Functional Theory based methods",

abstract = "The MC–srDFT model is a promising model in regards of giving a good description of complex molecular systems, that requires both a multi-configurational wavefunction, aswell as an accurate description of short-range interactions. Before this PhD thesis, the MC–srDFT model was able to describe molecular properties within the singlet linear-response framework, as well as performing open-shell calculations. All within the srGGA framework. The capabilities of the MC–srDFT model have been extended to molecular properties that requires triplet linear-response. This extension is restricted to singlet reference wavefunction. Furthermore, the MC–srDFT model have been extended to the framework of MGGA, which have been derived an implemented for singlet linear-response, triplet linear-response and open-shell wavefunction optimizations. These newly developed MC–srDFT methods have been benchmarked for system consisting of small molecules, as well for a series of transition-metal complexes. Through these benchmark calculations, it have been shown that the MC–srDFT model is capable of giving accurate calculated molecular properties. Surprisingly, for most of the benchmark calculations it was found that the srLDA functional was as good or better than both the srPBE and srTPSS functionals.",

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doi = "10.21996/zt8y-x461",

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publisher = "Syddansk Universitet. Det Naturvidenskabelige Fakultet",

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AB - The MC–srDFT model is a promising model in regards of giving a good description of complex molecular systems, that requires both a multi-configurational wavefunction, aswell as an accurate description of short-range interactions. Before this PhD thesis, the MC–srDFT model was able to describe molecular properties within the singlet linear-response framework, as well as performing open-shell calculations. All within the srGGA framework. The capabilities of the MC–srDFT model have been extended to molecular properties that requires triplet linear-response. This extension is restricted to singlet reference wavefunction. Furthermore, the MC–srDFT model have been extended to the framework of MGGA, which have been derived an implemented for singlet linear-response, triplet linear-response and open-shell wavefunction optimizations. These newly developed MC–srDFT methods have been benchmarked for system consisting of small molecules, as well for a series of transition-metal complexes. Through these benchmark calculations, it have been shown that the MC–srDFT model is capable of giving accurate calculated molecular properties. Surprisingly, for most of the benchmark calculations it was found that the srLDA functional was as good or better than both the srPBE and srTPSS functionals.

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M3 - Ph.D. thesis

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Extending the capabilities of Multi-Configurational short-range Density Functional Theory based methods

Abstract

Dokumenter og links

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Fingeraftryk

Relaterede publikationer

Multi-configurational short-range density functional theory can describe spin–spin coupling constants of transition metal complexes

Dalton Project: A Python platform for molecular- and electronic-structure simulations of complex systems

Triplet excitation energies from multiconfigurational short-range density-functional theory response calculations

Citationsformater