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Solvent effects on two-photon absorption of dialkylamino substituted distyrylbenzene chromophore
KTH, School of Biotechnology (BIO), Theoretical Chemistry.
Centre for Theoretical and Computational Chemistry, Department of Chemistry, University of Tromsø.
Centre for Theoretical and Computational Chemistry, Department of Chemistry, University of Tromsø.
College of Physics and Electronics, Shandong Normal University, Jinan .
Show others and affiliations
2007 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 126, no 20Article in journal (Refereed) Published
Abstract [en]

Solvent effects on the two-photon absorption of a symmetrical diamino substituted distyrylbenzene chromophore have been studied using the density functional response theory in combination with the polarizable continuum model. It is shown that the dielectric medium has a rather small effect both on the bond length alternation and on the one-photon absorption spectrum, but it affects significantly the two-photon absorption cross section. It is found that both one- and two-photon absorptions are extremely sensitive to the planarity of the molecule, and the absorption intensity can be dramatically reduced by the conformation distortion. It has led to the conclusion that the experimentally observed anomalous solvent effect on the two-photon absorption of dialkylamino substituted distyrylbenzene chromophores cannot be attributed to the intrinsic properties of a single molecule and its interaction with solvents.

Place, publisher, year, edition, pages
2007. Vol. 126, no 20
Keyword [en]
density-functional theory, polarizable continuum model, cross-sections, organic chromophores, electronic-structure, molecules, derivatives
National Category
Industrial Biotechnology
Identifiers
URN: urn:nbn:se:kth:diva-13829DOI: 10.1063/1.2740641ISI: 000246891700037Scopus ID: 2-s2.0-34249864511OAI: oai:DiVA.org:kth-13829DiVA: diva2:327653
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2017-12-12Bibliographically approved
In thesis
1. Theoretical study on nonlinearoptical properties of organicchromophores in solutions
Open this publication in new window or tab >>Theoretical study on nonlinearoptical properties of organicchromophores in solutions
2010 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Inter-molecular interactions have significant influences on linear and nonlinear optical properties of molecules including one- and two-photon absorptions, emissions, and various high order nonlinear polarizations. The related investigation has become an active and challenging research area. The theoretical structure-to-property relationship obtained from quantum chemical calculations of single organic conjugated molecules often can not be directly applied to real materials in condensed phases. One has to consider the effect of environment, that is, inter-molecular interactions, where the model systems experience in real experiments or applications. The change of molecular conformations under all kinds of interactions and its effects on linear and nonlinear optical properties are the central issue of this thesis.

Special attentions have been paid to symmetrical diamino substituted distyrylbenzene chromophores with different torsional angles, two dipolar merocyanine dyes of various orientations, two isomers of a V-shaped 2-hydroxypyrimidine derivative and their various dimers, and the structural fluctuations of interacting polar chromophores in solutions. Quantum chemical methods in combination with molecular dynamics simulations have been employed to study molecular conformations and optical properties in solutions, in particular the solvent and aggregation effects on one- and two-photon absorption. More specifically, time-dependent density functional theory has been used for all electronic calculations, while the polarizable continuum model and supermolecule approach have also been employed to take into account solvent effects.

Moreover, the propagation of an ultrashort laser pulse through a one-dimensional asymmetric organic molecular medium which possesses large permanent dipole moments has been simulated by solving full Maxwell-Bloch equations using predictor-corrector finite-difference time-domain method. We have focused on the supercontinuum generation of spectra and the formation of attosecond pulses.

Place, publisher, year, edition, pages
Stockholm: KTH, 2010. 80 p.
Series
Trita-BIO-Report, ISSN 1654-2312 ; 2010:9
Keyword
two-photon absorption, solvent effects, aggregation effects, molecular dynamics simulation
National Category
Theoretical Chemistry
Identifiers
urn:nbn:se:kth:diva-12748 (URN)978-91-7415-630-0 (ISBN)
Public defence
2010-06-07, FA 31, Roslagstullsbacken 21, Stockholm, 10:00 (English)
Opponent
Supervisors
Note
QC20100630Available from: 2010-05-12 Created: 2010-05-07 Last updated: 2011-01-21Bibliographically approved
2. Theoretical study of light-molecule nonlinear interactions
Open this publication in new window or tab >>Theoretical study of light-molecule nonlinear interactions
2007 (English)Licentiate thesis, comprehensive summary (Other scientific)
Abstract [en]

The work presented in the thesis concerned theoretical study of light-matter nonlinear interactions. Two important aspects of such interactions have been examined, namely the nonlinear optical properties of a series of organic charge transfer molecules in solutions induced by the laser light and the propagation of the ultrafast high power laser through the nonlinear molecular medium.

Special attention has been paid to understand the solvent effects on the two-photon absorption of a symmetrical diamino substituted distyrylbenzene chromophore, for which time-dependent density functional theory in combination with polarizable continuum model (PCM) have been employed. The dielectric medium alone has a rather small effect both on the bond length alternation and on the one-photon absorption spectrum, but noticeable effects on the two-photon absorption cross section. Both one- and two-photon absorptions are found to be extremely sensitive to the planarity of the molecule. Our calculations indicate that the experimentally observed anomalous solvent effect on the two-photon absorption of dialkylamino substituted distyrylbenzene chromophores can not be attributed to the intrinsic properties of a single molecule and its interaction with solvents. With the same theoretical approaches, two-photon absorption properties of interacting polar chromophores have been investigated to examine the validity of the widely used exciton model. Our first principles calculations have shown that the exciton model offers a conceptually simple interpretation for experimental observations, but is lack of predictability.

The second part of the thesis is to investigate the propagation of ultrashort laser pulse through a one-dimensional asymmetric organic molecular medium by solving full Maxwell-Bloch equations using predictor-corrector finite-difference time-domain method. It focuses on the supercontinuum generation of spectra and the formation of attosecond pulses. It is shown that the supercontinuum generation is strongly modulated by both area and width of the pulse, which results from the interference between the splitting pulses in time-domain and is the implication of the time-energy uncertainty relation. The presence of permanent dipole moment in molecular medium has noticeable effects on the supercontinuum generation. Our calculations show that a well-shaped 132 attosecond pulse can be generated from a two femtosecond incoming pulse under certain conditions. Influences of carrier-envelope phase and time-dependent ionization on the spectral and temporal evolutions of the ultrashort pulses have also been discussed.

Place, publisher, year, edition, pages
Stockholm: KTH, 2007. 49 p.
National Category
Industrial Biotechnology
Identifiers
urn:nbn:se:kth:diva-4364 (URN)978-91-7178-642-5 (ISBN)
Presentation
2007-05-16, FD41, AlbaNova, Stockholm, 10:10
Opponent
Supervisors
Note
QC 20101122Available from: 2007-05-10 Created: 2007-05-10 Last updated: 2011-11-23Bibliographically approved

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