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Two-Photon Excited Fluorescence Depolarisation [Elektronisk resurs] Experimental and Theoretical Development

Ryderfors, Linus, 1977- (författare)
Mukhtar, Emad (preses)
Johansson, Lennart B.-Å. (preses)
Levine, Yehudi K. (opponent)
Uppsala universitet Teknisk-naturvetenskapliga vetenskapsområdet (utgivare)
Publicerad: Uppsala : Universitetsbiblioteket, 2008
Engelska 78
Serie: Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, 1651-6214 1651-6214 ; 552
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  • E-bokAvhandling(Diss. (sammanfattning) Uppsala : Uppsala universitet, 2008)
Sammanfattning Ämnesord
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  • 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 D 2h , D 2 and C 2v are given. Preliminary experiments are finally also reported on a two-photon excited donor-donor energy migration system consisting of a bisanthryl-bisteroid. 

Ämnesord

Natural Sciences  (hsv)
Physical Sciences  (hsv)
Atom and Molecular Physics and Optics  (hsv)
Naturvetenskap  (hsv)
Fysik  (hsv)
Atom- och molekylfysik och optik  (hsv)
NATURAL SCIENCES  (svep)
Physics  (svep)
Atomic and molecular physics  (svep)
Chemical physics  (svep)
NATURVETENSKAP  (svep)
Fysik  (svep)
Atom- och molekylfysik  (svep)
Kemisk fysik  (svep)

Genre

government publication  (marcgt)

Indexterm och SAB-rubrik

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)
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