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The nature of the low energy band of the Fenna-Matthews-Olson complex: vibronic signatures | | Felipe Caycedo-Soler
; Alex W. Chin
; Javier Almeida
; Susana F. Huelga
; Martin B. Plenio
; | | Date: |
30 Dec 2011 | | Abstract: | Based entirely upon actual experimental observations on electron-phonon
coupling, we develop a theoretical framework to show that the lowest energy
band of the Fenna- Matthews-Olson (FMO) complex exhibits observable features
due to the quantum nature of the vibrational manifolds present in its
chromophores. The study of linear spectra provides us with the basis to
understand the dynamical features arising from the vibronic structure in
non-linear spectra in a progressive fashion, starting from a microscopic model
to finally performing an inhomogenous average. We show that the discreteness of
the vibronic structure can be witnessed by probing the diagonal peaks of the
non-linear spectra by means of a relative phase shift in the waiting time
resolved signal. Moreover, we demonstrate the photon-echo and non-rephasing
paths are sensitive to different harmonics in the vibrational manifold when
static disorder is taken into account. Supported by analytical and numerical
calculations, we show that nondiagonal resonances in the 2D spectra in the
waiting time, further capture the discreteness of vibrations through a
modulation of the amplitude without any effect in the signal intrinsic
frequency. This fact generates a signal that is highly sensitive to
correlations in the static disorder of the excitonic energy albeit protected
against dephasing due to inhomogeneities of the vibrational ensemble. | | Source: | arXiv, 1201.0156 | | Services: | Forum | Review | PDF | Favorites | |
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