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Two-photon absorption in the relativistic four-component Hartree-Fock approximation
Linköpings universitet, Institutionen för fysik, kemi och biologi, Beräkningsfysik. Linköpings universitet, Tekniska högskolan.
Linköpings universitet, Institutionen för fysik, kemi och biologi, Beräkningsfysik. Linköpings universitet, Tekniska högskolan.
Department of Chemistry, University of Southern Denmark, Odense M, Denmark.
2005 (engelsk)Inngår i: The Journal of Chemical Physics, ISSN 0021-9606, Vol. 122, nr 11, s. 114106-Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

A first implementation of the single residue of the quadratic response function in the four-component Hartree–Fock approximation is presented. The implementation is based on a Kramers paired molecular orbital basis and takes full advantage of time and spatial symmetry reductions in a quaternion formulation—in analogy with the previous work on the quadratic response function [J. Chem. Phys. 121, 6145 (2004)]. Sample calculations are given in terms of the monochromatic and coherent two-photon absorption cross sections in the noble gases. The relativistic two-photon selection rule J={0,±2} allows for nonrelativistically spin-forbidden transitions, and, even in neon, strong two-photon absorption is shown to occur for the X  1S02  3P2 transition. It is argued that relevant comparisons between nonrelativistic and relativistic calculations must be performed at the level of integrated absorption cross sections.

sted, utgiver, år, opplag, sider
2005. Vol. 122, nr 11, s. 114106-
Emneord [en]
two-photon processes, absorption, HF calculations, neon
HSV kategori
Identifikatorer
URN: urn:nbn:se:liu:diva-13998DOI: 10.1063/1.1869469OAI: oai:DiVA.org:liu-13998DiVA, id: diva2:22428
Tilgjengelig fra: 2006-10-05 Laget: 2006-10-05
Inngår i avhandling
1. Molecular Quadratic Response Properties with Inclusion of Relativity
Åpne denne publikasjonen i ny fane eller vindu >>Molecular Quadratic Response Properties with Inclusion of Relativity
2008 (engelsk)Doktoravhandling, med artikler (Annet vitenskapelig)
Abstract [en]

This thesis concerns quadratic response properties and their application to properties in Jablonski diagrams such as resonant two-photon absorption and excited state absorption. Our main interest lies in optical power limiting applications, and in this context, molecules containing heavy metal atoms prove superior. Therefore, we are interested in how relativity affects these properties, and in order to assess this, a four-component relativistic framework is adopted.

To properly address the molecular properties of interest, both relativistic effects and electron correlation need to be accounted for. These two properties are not additive, and, therefore, correlation needs to be incorporated into the four-component framework. We present the implementation of quadratic response properties at the four-component density functional level of theory. For second-harmonic generation, we have, with numerical examples, demonstrated that correlation and relativity are indeed not additive and that the inclusion of noncollinear magnetization is of little importance. We report that both electron correlation as well as relativity strongly affect results for second-harmonic generation. For example, relativity alone reduces the µβ-response signal by 62% and 75% for meta- and ortho-bromobenzene, respectively, and enhances the same response by 17% and 21% for meta- and ortho-iodobenzene, respectively.

In the four-component framework, we present the implementations of single and double residues of the quadratic response function, which allows for the evaluation of resonant two-photon absorption cross sections and excited state properties. Using these tools, we discuss different levels of approximation to the relativistic Hamiltonian and we demonstrate that for two-photon absorption, a proper treatment of relativistic effects qualitatively alters the spectrum. For example, already for an element as light as neon, significant differences are seen between the relativistic and nonrelativistic spectra as triplet transitions acquire substantial absorption cross sections in the former case.

Finally, quantum mechanics in conjunction with electrodynamics is applied to determine clamping levels in macroscopic samples. The microscopic properties of the optically active chromophores are determined by response theory, and then, electrodynamics is used to describe the interactions between the chromophores and incident laser pulses. Using this approach a series of molecules have been investigated and their performances have been compared and ranked in order to find novel materials for optical power limiting applications.

sted, utgiver, år, opplag, sider
Institutionen för fysik, kemi och biologi, 2008. s. 36
Serie
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1167
Emneord
relativistic quantum chemistry, molecular physics, clamping levels, four-component Hartree-Fock theory, Kohn-Sham density functional theory, response theory, nonlinear optics, second-harmonic generation, two-photon absorption, excited state properties, optical power limiting
HSV kategori
Identifikatorer
urn:nbn:se:liu:diva-11035 (URN)978-91-7393-957-7 (ISBN)
Disputas
2008-04-11, Planck, Hus E, Campus Valla, Linköping University, Linköping, 10:15 (engelsk)
Opponent
Veileder
Tilgjengelig fra: 2008-03-05 Laget: 2008-03-05 Sist oppdatert: 2020-03-24
2. Light Control using Organometallic Chromophores
Åpne denne publikasjonen i ny fane eller vindu >>Light Control using Organometallic Chromophores
2006 (engelsk)Licentiatavhandling, med artikler (Annet vitenskapelig)
Abstract [en]

The interaction between light and organometallic chromophores has been investigated theoretically in a strive for fast optical filters. The main emphasis is on two-photon absorption and excited state absorption as illustrated in the Jablonski diagram. We stress the need for relativistic calculations and have developed methods to address this issue. Furthermore, we present how quantum chemical calculations can be combined with Maxwell's equations in order to simulate propagation of laser pulses through a materials doped with chromophores with high two-photon absorption cross sections. Finally, we also discuss how fast agile filters using spin-transition materials can be modeled in order to accomplish theoretical material design.

sted, utgiver, år, opplag, sider
Institutionen för fysik, kemi och biologi, 2006. s. 108
Serie
Linköping Studies in Science and Technology. Thesis, ISSN 0280-7971 ; 1274
Emneord
organometallic chromophores, two-photon absorption, excited state absorption, excited state dipole moment, four-component formalism, clamping levels, spin-transition
HSV kategori
Identifikatorer
urn:nbn:se:liu:diva-17232 (URN)91-85643-77-7 (ISBN)
Presentation
(engelsk)
Opponent
Veileder
Merknad

Report code: LIU-TEK-LIC-2006:55. On the day of the defence date the status on article III was Manuscript, article IV was Accepted and article V was Submitted.

Tilgjengelig fra: 2009-03-12 Laget: 2009-03-12 Sist oppdatert: 2020-04-01bibliografisk kontrollert

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