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Two-Photon Excited Fluorescence and Molecular Reorientations in Liquid Solutions
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Photochemistry and Molecular Science.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Photochemistry and Molecular Science.
2007 (English)In: Journal of Fluorescence, ISSN 1053-0509, E-ISSN 1573-4994, Vol. 17, no 5, 466-480 p.Article in journal (Refereed) Published
Abstract [en]

Theoretical expressions are derived that relate the two-photon excited fluorescence depolarisation experiments to the molecular symmetry and the rotational motions of fluorescent molecules. Diffusive rotational motions in liquid solvents are considered, as well as the influence of fast unresolved motions (e.g. librations). The results obtained are compared with one-photon excited fluorescence depolarisation experiments. The derived theoretical expressions can be applied for detailed analyses of the molecular rotation in solvent. Several of the results are useful for determining and assigning the components of two-photon absorption tensors.

Place, publisher, year, edition, pages
2007. Vol. 17, no 5, 466-480 p.
Keyword [en]
Two-photon excited fluorescence, Two-photon excited fluorescence depolarisation, Two-photon excited anisotropy, Theory of rotational motion, Rotational diffusion, Librations, Perylene
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:uu:diva-97539DOI: 10.1007/s10895-007-0189-xISI: 000248912100003PubMedID: 17578656OAI: oai:DiVA.org:uu-97539DiVA: diva2:172527
Available from: 2008-09-18 Created: 2008-09-18 Last updated: 2011-01-27Bibliographically approved
In thesis
1. Two-Photon Excited Fluorescence Depolarisation: Experimental and Theoretical Development
Open this publication in new window or tab >>Two-Photon Excited Fluorescence Depolarisation: Experimental and Theoretical Development
2008 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

We have studied fundamental aspects of time-resolved two-photon excited fluorescence depolarisation. The thesis presents experimental as well as theoretical progress. We show that a multi-photon induced instrumental response function obtained from a suspension of gold nanoparticles is appropriate for the analysis of two-photon excited fluorescence decays obtained using time-correlated single photon counting detection. Theoretical expressions have been derived for the fluorescence anisotropy decay obtained upon two-photon excitation of various molecular systems in liquid solutions: a) an anisotropic rigid rotor that undergoes rotational diffusion in the presence of ultrafast unresolved restricted reorientations, e.g. librations. b) a molecular group covalently attached to a stationary macromolecule, and undergoing local reorientation in a uniaxial ordering potential. A new approach to the analysis of two-photon excited fluorescence depolarisation experiments was developed, which combines data obtained by using linearly and circularly polarised excitation light, in a global manner. In the analysis, knowledge about unresolved reorientations was obtained from one-photon excitation studies of the corresponding systems. By means of this procedure it has been possible to obtain quantitative information about the molecular two-photon absorption tensor for perylene and two of its derivatives. Thereby the symmetry of the final excited and intermediate vibronic states could be assigned. The analysis reveals that the two-photon transition studied with the 800 nm laser exhibits mixed character. An important finding from the experiments was that the two-photon absorption tensor appears to be solvent dependent. Furthermore, the thesis presents the first theoretical treatment of two-photon excited donor-donor energy migration in the presence of molecular reorientation and which applies the extended Förster theory. Explicit expressions for molecules that belong to the point groups D2h, D2 and C2v are given. Preliminary experiments are finally also reported on a two-photon excited donor-donor energy migration system consisting of a bisanthryl-bisteroid.

Place, publisher, year, edition, pages
Uppsala: Universitetsbiblioteket, 2008. 78 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 552
Keyword
Two-photon excitation, Fluorescence, Fluorescence depolarisation, Fluorescence anisotropy, Time-correlated single photon counting, Gold nanoparticles, Rotational diffusion, Excited state symmetry, Extended Förster theory, Orientation correlation functions, Donor-donor energy migration (DDEM)
National Category
Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:uu:diva-9285 (URN)978-91-554-7282-5 (ISBN)
Public defence
2008-10-10, Häggsalen, Ångströmslaboratoriet, Lägerhyddsvägen 1, 752 37 UPPSALA, Uppsala, 10:15
Opponent
Supervisors
Available from: 2008-09-18 Created: 2008-09-18Bibliographically approved

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Ryderfors, LinusMukhtar, Emad

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