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Extended Förster theory: a quantitative approach to the determination of inter-chromophore distances in biomacromolecules
Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. (Prof. Lennart B.-Å. Johansson)
Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
2010 (Engelska)Ingår i: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 12, nr 28, s. 7758-7767Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

This review highlights recent theoretical and experimental advances in the study of biomacromolecular structure by using electronic transfer. The considered electronic transport in the extended Förster theory occurs within donor–acceptor pairs, donor–donor pairs, as well as within regular arrangements of many donors which may undergo reorienting and translational dynamics. The classical and the extended FoЁ rster theory are compared. Applications concern the determination of structural properties of proteins and non-covalent protein polymers. Studies of energy migration by means of two-photon excited fluorescence spectroscopy, as well as the relevant extension of the Förster theory are presented.

Ort, förlag, år, upplaga, sidor
2010. Vol. 12, nr 28, s. 7758-7767
Nyckelord [en]
Fluorescence, depolarisation, energy transport, donor-donor energy migration, Förster theory
Nationell ämneskategori
Fysikalisk kemi Atom- och molekylfysik och optik
Forskningsämne
fysikalisk kemi
Identifikatorer
URN: urn:nbn:se:umu:diva-50047DOI: 10.1039/b924113bISI: 000279627300003PubMedID: 20520912OAI: oai:DiVA.org:umu-50047DiVA, id: diva2:458794
Tillgänglig från: 2011-11-24 Skapad: 2011-11-24 Senast uppdaterad: 2018-06-08Bibliografiskt granskad
Ingår i avhandling
1. A new approach to the analyses of fluorescence depolarisation experiments in the presence of electronic energy transport
Öppna denna publikation i ny flik eller fönster >>A new approach to the analyses of fluorescence depolarisation experiments in the presence of electronic energy transport
2011 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
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.

Ort, förlag, år, upplaga, sidor
Umeå: Kemiska institutionen, Umeå University, 2011. s. 46
Nyckelord
electronic energy transfer, donor-donor energy migration, extended Förster theory, fluorescence depolarisation, two-photon excitation, computer simulations, genetic algorithms
Nationell ämneskategori
Fysikalisk kemi Atom- och molekylfysik och optik
Forskningsämne
fysikalisk kemi
Identifikatorer
urn:nbn:se:umu:diva-50050 (URN)978-91-7459-331-0 (ISBN)
Disputation
2011-12-16, KBC-huset, KB3A9, "Lilla hörsalen", Umeå Universitet, Umeå, 10:00 (Engelska)
Opponent
Handledare
Tillgänglig från: 2011-11-25 Skapad: 2011-11-24 Senast uppdaterad: 2018-06-08Bibliografiskt granskad

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