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Extended Förster theory for determining intraprotein distances: Part III. Partial donor–donor energy migration among reorienting fluorophores
Umeå University, Faculty of Science and Technology, Chemistry.
Umeå University, Faculty of Science and Technology, Chemistry.
Umeå University, Faculty of Science and Technology, Chemistry.
Umeå University, Faculty of Science and Technology, Chemistry.
2008 (English)In: Physical Chemistry Chemical Physics, Vol. 10, 6962-70 p.Article in journal (Refereed) Published
Abstract [en]

An extended Förster theory (EFT) is derived and outlined for electronic energy migration between two fluorescent molecules which are chemically identical, but photophysically non-identical. These molecules exhibit identical absorption and fluorescence spectra, while their fluorescence lifetimes differ. The latter means that the excitation probability becomes irreversible. Unlike the case of equal lifetimes, which is often referred to as, donor–donor energy migration (DDEM), the observed fluorescence relaxation is then no longer invariant to the energy migration process. To distinguish, the present case is therefore referred to as partial donor–donor energy migration (PDDEM). The EFT of PPDEM is described by a stochastic master equation (SME), which has been derived from the stochastic Liouville equation (SLE) of motion. The SME accounts for the reorienting as well as the translational motions of the interacting chromophores. Synthetic fluorescence lifetime and depolarisation data that mimics time-correlated single photon counting experiments have been generated and re-analysed. The rates of reorientation, as well as the orientational configurations of the interacting D-groups were examined. Moreover the EFT of PPDEM overcomes the classical 2-problem and the frequently applied approximation of 2 = 2/3 in the data analyses. An outline for the analyses of fluorescence lifetime and depolarisation data is also given, which might prove applicable to structural studies of D-labelled macromolecules, e.g. proteins. The EFT presented here brings the analyses of PDDEM data to the same level of molecular detail as that used in ESR- and NMR-spectroscopy.

Place, publisher, year, edition, pages
2008. Vol. 10, 6962-70 p.
Identifiers
URN: urn:nbn:se:umu:diva-10693DOI: doi:10.1039/b810661dOAI: oai:DiVA.org:umu-10693DiVA: diva2:150364
Available from: 2008-12-02 Created: 2008-12-02 Last updated: 2011-01-10Bibliographically approved
In thesis
1. Extended Förster Theory of Electronic Energy Transport within Pairs of Reorienting Chromophoric Molecules
Open this publication in new window or tab >>Extended Förster Theory of Electronic Energy Transport within Pairs of Reorienting Chromophoric Molecules
2009 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

An extended Förster theory (EFT), previously derived (L. B.-Å. Johansson et al. J. Chem. Phys., 1996,105) has theoretically been adapted and used in simulations of donor-acceptor energy transfer (DAET), which is a process often referred to as FRET. It was shown that the classical Förster theory is only valid in the initial part of the fluorescence decay. In this thesis an EFT is derived and outlined for electronic energy transport between two fluorescent molecules which are chemically identical, but photophysically non-identical. The energy migration within such asymmetric pairs is partially reversible and therefore referred to as partial donor-donor energy migration (PDDEM). The previously derived model of PDDEM (S. V. Kalinin et al. Spectrochim Acta Part A, 2002,58) is an approximation of the EFT. In particular, the EFT accounts for the time-dependent reorientations as well as the distance that influence the rate of electronic energy migration. The reorientation of the fluorophores transition dipole moments has been simulated using Brownian dynamics. As a result, the related “k2-problem” has been solved. The EFT of PDDEM has also been studied regarding the effect of PDDEM on experimental observables e.g. quantum yield of fluorescence and steady-state anisotropies

Place, publisher, year, edition, pages
Umeå: VMC-KBC, 2009. 37 p.
Keyword
electronic energy migration/transfer, extended Förster theory, orientation factor, DDEM, PDDEM, time-resolved fluorescence anisotropy, time-correlated single photon counting, Brownian dynamics
Research subject
Physical Chemistry
Identifiers
urn:nbn:se:umu:diva-22471 (URN)978-91-7264-783-1 (ISBN)
Public defence
2009-06-05, KB3A9, KBC huset, Umeå Universitet, 13:15 (English)
Opponent
Supervisors
Available from: 2009-05-15 Created: 2009-05-11 Last updated: 2009-05-15Bibliographically approved

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