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A density functional theory study of magneto-electric Jones birefringence of noble gases, furan homologues, and mono-substituted benzenes
Linköping University, Department of Physics, Chemistry and Biology, Computational Physics. Linköping University, The Institute of Technology.
Linköping University, Department of Physics, Chemistry and Biology, Computational Physics. Linköping University, The Institute of Technology.
University of Trieste, Italy .
UOS Pisa, Italy .
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2013 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 139, no 19, 194311- p.Article in journal (Refereed) Published
Abstract [en]

We report on the results of a systematic ab initio study of the Jones birefringence of noble gases, of furan homologues, and of monosubstituted benzenes, in the gas phase, with the aim of analyzing the behavior and the trends within a list of systems of varying size and complexity, and of identifying candidates for a combined experimental/theoretical study of the effect. We resort here to analytic linear and nonlinear response functions in the framework of time-dependent density functional theory. A correlation is made between the observable (the Jones constant) and the atomic radius for noble gases, or the permanent electric dipole and a structure/chemical reactivity descriptor as the para Hammett constant for substituted benzenes.

Place, publisher, year, edition, pages
American Institute of Physics (AIP) , 2013. Vol. 139, no 19, 194311- p.
National Category
Engineering and Technology
URN: urn:nbn:se:liu:diva-102851DOI: 10.1063/1.4830412ISI: 000327714900024OAI: diva2:683826

Funding Agencies|EuroMagNET II, under EU|228043|Swedish Research Council|621-2010-5014|Italian Ministero dellIstruzione, Universita e Ricerca|2009C28YBF_001|National Supercomputer Centre (NSC), Sweden||Italian CINECA||

Available from: 2014-01-07 Created: 2014-01-02 Last updated: 2016-01-15
In thesis
1. Development and characterization of damped cubic response functions with application to two-photon absorption
Open this publication in new window or tab >>Development and characterization of damped cubic response functions with application to two-photon absorption
2015 (English)Licentiate thesis, comprehensive summary (Other academic)
Abstract [en]

Molecular response to electromagnetic fields - static or optical - within a framework of perturbation theory diverges close to resonance with molecular transitionen energies, and need work-around solutions for real-valued response functions. This licentiate thesis deals with nonlinear response, with focus being on cubic polarizaibilities, and outlines the underlying mathematics for exact-state and approximatestate, complex-valued response functions applicable to quantum chemical computation. Such a complex-valued response theory is commonly known as dampedresponse theory, for which the response functions consists of a real and an imaginary component, each of them representing various spectroscopies in nature. In addition to the mathematics, the formulas have been implemented in the quantum chemical package DALTON, and several tests determining the integrity of the implementation has been conducted.

The fourth and final major part of the thesis is concerned with applied nonlinear response theory, including not only cubic response functions, but also quadratic and linear response functions, some of which are of the more exotic character. Three spectroscopies have been investigated for small and medium-sized organic molecules and the neon atom: two-photon absorption (TPA), Jones birefringence (JB), and magnetic circular dichroism (MCD).

The TPA part is a simple demonstration of capability of the damped cubic response code, for which neon is the example system. Perfect agreement is shown for the Ehrenfest approach and an independent implementation based on the quasienergy formalism.

JB is an optical eect in which induced refractive anisotropy, by means of external electric and magnetic static elds, results in ellipticity of linearly polarized light beams. This part mainly discuss implications from a paper which the current author took part in. The paper ultimately attempts to indentify the general observable strength of the effect, and coincidentaly pin-point some particular system suitable for experiments. Among other finds, JB is found to be correlated to the electric dipole moment, and for monosubstituted benzenes, the para-Hammett constant.

Finally, MCD is discussed based on three papers in which the present author is included. The elegant MCD solution to broad absorption peaks, for which it is desired to distinguish individual states, is demonstrated on adenine and three additional purine derivatives. A drawn out debate regarding relative stability of certain low-lying states could be settled by this method. Furthermore, appropriate description of solvation environment in conjunction with the exchange-correlation functionals B3LYP and CAM-B3LYP is investigated on purine and pyrimidine derivatives. CAM-B3LYP is found to be superior in terms of general prole shapes, while results regarding solvation model are rather inconclusive, although the results suggests some level of solvation model is appropriate, such as a polarizable continuum model or explicit solvation molecules.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2015. 67 p.
Linköping Studies in Science and Technology. Thesis, ISSN 0280-7971 ; 1742
National Category
Theoretical Chemistry Chemical Sciences
urn:nbn:se:liu:diva-123972 (URN)978-91-7685-844-8 (Print) (ISBN)
Available from: 2016-01-15 Created: 2016-01-15 Last updated: 2016-01-15Bibliographically approved

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