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Using fluorescence detected two-dimensional spectroscopy to investigate initial exciton delocalization between coupled chromophores

Schröter, Marco ; Pullerits, Tõnu ; Kühn, Oliver

The Journal of chemical physics, 2018-09, Vol.149 (11), p.114107-114107 [Periódico revisado por pares]

United States: American Institute of Physics

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Título:
Using fluorescence detected two-dimensional spectroscopy to investigate initial exciton delocalization between coupled chromophores
Autor: Schröter, Marco ; Pullerits, Tõnu ; Kühn, Oliver
Assuntos: Absorption spectra ; Atom and Molecular Physics and Optics ; Atom- och molekylfysik och optik ; Chemical Sciences ; Chemistry Techniques, Analytical - instrumentation ; Chromophore-Assisted Light Inactivation ; Chromophores ; Excitons ; Fluorescence ; Fysik ; Fysikalisk kemi ; Kemi ; Migration ; Models, Chemical ; Natural Sciences ; Naturvetenskap ; Organic Chemicals - chemistry ; Perturbation theory ; Photosynthesis ; Physical Chemistry ; Physical Sciences ; Spectrometry, Fluorescence ; Spectroscopy ; Spectrum analysis
É parte de: The Journal of chemical physics, 2018-09, Vol.149 (11), p.114107-114107
Notas: ObjectType-Article-1
SourceType-Scholarly Journals-1
ObjectType-Feature-2
content type line 23
Descrição: Förster theory describes electronic exciton energy migration in molecular assemblies as an incoherent hopping process between donor and acceptor molecules. The rate is expressed in terms of the overlap integral between donor fluorescence and acceptor absorption spectra. Typical time scales for systems like photosynthetic antennae are on the order of a few picoseconds. Prior to transfer, it is assumed that the initially excited donor molecule has equilibrated with respect to the local environment. However, upon excitation and during the equilibration phase, the state of the system needs to be described by the full density matrix, including coherences between donor and acceptor states. While being intuitively clear, addressing this regime experimentally has been a challenge until the recently reported advances in fluorescence detected two-dimensional spectroscopy. Here, we demonstrate using fourth order perturbation theory the conditions for the presence of donor-acceptor coherence induced cross-peaks at zero waiting time between the first and the second pair of pulses. The approach is illustrated for a heterodimer model which facilitates an analytical solution.
Editor: United States: American Institute of Physics
Idioma: Inglês

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Using fluorescence detected two-dimensional spectroscopy to investigate initial exciton delocalization between coupled chromophores

Schröter, Marco ; Pullerits, Tõnu ; Kühn, Oliver

United States: American Institute of Physics

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