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On the analyses of fluorescence depolarisation data in the presence of electronic energy migration: Part I. Theory and general description
Umeå University, Faculty of Science and Technology, Department of Chemistry. (Prof. Lennart B.-Å. Johansson)
Umeå University, Faculty of Science and Technology, Department of Chemistry.
2012 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 14, 1907-1916 p.Article in journal (Refereed) Published
Abstract [en]

A new and general procedure is described for a detailed analysis of time-resolved fluorescence depolarisation data in the presence of electronic energy migration. An isotropic ensemble of bifluorophoric molecules (D1-R-D2) has been studied to demonstrate its utility. Intramolecular donor-donor energy migration occurs between the two donor groups (D), which are covalently connected to a rigid linker group (R). These groups undergo restricted reorientational motions with respect to the R group. The analysis of depolarisation data basically involves the search for best-fit parameters which describe the local reorienting motions, the intermolecular D1-D2 distance, as well as the mutual orientations of the donors. For this, the analysis is partly performed in the Fourier domain and the best-fit parameters are determined by using an approach based on a Genetic Algorithm. The energy migration process has been described by using Monte Carlo simulations and an extended Förster theory (EFT). It is found that the EFT provides the least time-consuming computational method. Since one-photon and two-photon excited fluorescence experiments can be applied for energy migration studies, a general and unified theoretical formulation is given.

Place, publisher, year, edition, pages
Cambridge: RSC Publishing, 2012. Vol. 14, 1907-1916 p.
Keyword [en]
Extended Förster theory, Genetic algorithm, Monte Carlo simulations, two-photon excitation
National Category
Physical Chemistry Atom and Molecular Physics and Optics
Identifiers
URN: urn:nbn:se:umu:diva-50048DOI: 10.1039/c1cp22483bOAI: oai:DiVA.org:umu-50048DiVA: diva2:458797
Available from: 2011-11-24 Created: 2011-11-24 Last updated: 2017-12-08Bibliographically approved
In thesis
1. A new approach to the analyses of fluorescence depolarisation experiments in the presence of electronic energy transport
Open this publication in new window or tab >>A new approach to the analyses of fluorescence depolarisation experiments in the presence of electronic energy transport
2011 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

A new and general procedure is described for a detailed analysis of time-resolved fluorescence depolarisation data in the presence of electronic energy migration. An isotropic ensemble of bifluorophoric molecules (D1-R-D2) has been studied to demonstrate its utility. Intramolecular donor-donor energy migration occurs between the two donor groups (D), which are covalently connected to a rigid linker group (R). These groups undergo restricted reorientational motions with respect to the R group. The analysis of depolarisation data basically involves the search for best-fit parameters which describe the local reorienting motions, the interfluorophore D1-D2 distance, as well as the mutual orientations of the donors. For this, the analysis is partly performed in the Fourier domain and the best-fit parameters are determined by using an approach based on a Genetic Algorithm. The energy migration process has been described by using Monte Carlo simulations and an extended Förster theory. It is found that this theory provides the least time-consuming computational method. Since one-photon and two-photon excited fluorescence experiments can be applied for energy migration studies, a general and unified theoretical formulation is given.

To exemplify the developed quantitative approach the depolarisation of the fluorescence in the presence of electronic energy migration within a bis-(9-anthrylmethylphosphonate) bisteroid molecule has been studied by time-resolved two-photon excited fluorescence depolarisation experiments. To solely obtain information about local reorientations of the 9-anthrylmethyl group, also the mono-(9-anthrylmethylphosphonate) bisteroid was studied, which enabled modelling of the ordering potential of the donor. Values of the two-photon absorption tensor components were obtained. To describe the discrepancy between the measured values of the initial anisotropy and fundamental anisotropy predicted by theory the distribution of absorption tensor caused by fast processes have been introduced. An angular parameter of absorption tensor was determined. Reasonable values of the distance between the 9-anthrylmethyl groups, as well as for their mutual orientation were obtained.

Place, publisher, year, edition, pages
Umeå: Kemiska institutionen, Umeå University, 2011. 46 p.
Keyword
electronic energy transfer, donor-donor energy migration, extended Förster theory, fluorescence depolarisation, two-photon excitation, computer simulations, genetic algorithms
National Category
Physical Chemistry Atom and Molecular Physics and Optics
Research subject
Physical Chemistry
Identifiers
urn:nbn:se:umu:diva-50050 (URN)978-91-7459-331-0 (ISBN)
Public defence
2011-12-16, KBC-huset, KB3A9, "Lilla hörsalen", Umeå Universitet, Umeå, 10:00 (English)
Opponent
Supervisors
Available from: 2011-11-25 Created: 2011-11-24 Last updated: 2011-11-24Bibliographically approved

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Opanasyuk, OlegJohansson, Lennart B-Å

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