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Time-dependent density functional theory for non-linear properties of open-shell systems
KTH, School of Biotechnology (BIO), Theoretical Chemistry (closed 20110512).ORCID iD: 0000-0003-2729-0290
KTH, School of Biotechnology (BIO), Theoretical Chemistry (closed 20110512).
KTH, School of Biotechnology (BIO), Theoretical Chemistry (closed 20110512).
KTH, School of Biotechnology (BIO), Theoretical Chemistry (closed 20110512).ORCID iD: 0000-0002-9123-8174
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2007 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 127, no 11, 114101- p.Article in journal (Refereed) Published
Abstract [en]

This paper presents response theory based on a spin-restricted Kohn-Sham formalism for computation of time-dependent and time-independent nonlinear properties of molecules with a high spin ground state. The developed approach is capable to handle arbitrary perturbations and constitutes an efficient procedure for evaluation of electric, magnetic, and mixed properties. Apart from presenting the derivation of the proposed approach, we show results from illustrating calculations of static and dynamic hyperpolarizabilities of small Si(3n+1)H(6n+3) (n=0,1,2) clusters which mimic Si(111) surfaces with dangling bond defects. The results indicate that the first hyperpolarizability tensor components of Si(3n+1)H(6n+3) have an ordering compatible with the measurements of second harmonic generation in SiO2/Si(111) interfaces and, therefore, support the hypothesis that silicon surface defects with dangling bonds are responsible for this phenomenon. The results exhibit a strong dependence on the quality of basis set and exchange-correlation functional, showing that an appropriate set of diffuse functions is required for reliable predictions of the first hyperpolarizability of open-shell compounds.

Place, publisher, year, edition, pages
2007. Vol. 127, no 11, 114101- p.
National Category
Theoretical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-7069DOI: 10.1063/1.2768357ISI: 000249667400007Scopus ID: 2-s2.0-34648828833OAI: oai:DiVA.org:kth-7069DiVA: diva2:11971
Note
QC 20100811Available from: 2007-05-11 Created: 2007-05-11 Last updated: 2011-11-07Bibliographically approved
In thesis
1. Density Functional Response Theory with Applications to Electron and Nuclear Magnetic Resonance
Open this publication in new window or tab >>Density Functional Response Theory with Applications to Electron and Nuclear Magnetic Resonance
2007 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

This thesis presents quantum chemical calculations, applications of the response function formalism recently implemented within the framework of density functional theory by our research group. The purpose of the calculations is to assess the performance of this perturbative approach to determining heavy atom effects on magnetic resonance parameters. Relativistic corrections can be generated by spin-orbit interactions or by scalar relativistic effects due to high velocity electrons in the atomic core region of heavy atoms. In this work, the evaluation of nuclear magnetic resonance parameters is considered, the nuclear shielding tensor and the indirect nuclear spin-spin coupling tensor. For series of homologous compounds, it is found that both types of corrections to these parameters are increasing in size upon substitution of a constituent atom by a heavier element, but that their relative importance is system dependent. The obtained results are compatible with the ones provided by electron correlated ab initio methods, and a qualitative agreement with experimentally determined parameters is overall achieved. The methodology presented in this thesis aims to be a practical approach which can be applied in the study of molecular properties of large systems.

This thesis also addresses the calculation of hyperfine coupling constants, and evaluates a novel approach to the treatment of spin-polarization in spin restricted calculations without the spin contamination associated with spin unrestricted calculations

Place, publisher, year, edition, pages
Stockholm: KTH, 2007. v, 51 p.
Keyword
biochemistry, molecular physics, computer science
National Category
Theoretical Chemistry
Identifiers
urn:nbn:se:kth:diva-4367 (URN)978-91-7178-675-3 (ISBN)
Public defence
2007-05-25, FA32, AlbaNova, Roslagstullsbacken, Stockholm, 10:00
Opponent
Supervisors
Note
QC 20100811Available from: 2007-05-11 Created: 2007-05-11 Last updated: 2010-08-11Bibliographically approved

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Vahtras, OlavÅgren, Hans

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