Optical Stark spectroscopy of molecular aggregates

Mukamel, Shaul; Rott, P.; Chernyak, Vladimir

doi:10.1063/1.471781

Cited by 6 publications

(3 citation statements)

References 53 publications

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“…In the presence of static disorder (disorder of the site energies E n and couplings M nm ) the homogeneous FL profiles should be averaged over a random distribution of E n and M nm that will perturb energies and eigenfunctions of the exciton states. Nonlinear spectral responses can be expressed in terms of the line-broadening functions (eqn (4)) as well, for example pump-probe, 65,[71][72][73][74]88 Stark spectra, 76,89 three-pulse photon echoes, 87 and 2D echoes. 83 The spectral density needed to evaluate the spectral responses can be obtained from molecular dynamics simulations 26 or can be extracted from experiments, for example from hole-burning 20 or fluorescence line-narrowing (FLN) spectra.…”

Section: Exciton-phonon Coupling and Spectral Line Shapesmentioning

confidence: 99%

Physical origins and models of energy transfer in photosynthetic light-harvesting

Novoderezhkin

Grondelle

2010

Phys. Chem. Chem. Phys.

205

271

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We perform a quantitative comparison of different energy transfer theories, i.e. modified Redfield, standard and generalized Förster theories, as well as combined Redfield-Förster approach. Physical limitations of these approaches are illustrated and critical values of the key parameters indicating their validity are found. We model at a quantitative level the spectra and dynamics in two photosynthetic antenna complexes: in phycoerythrin 545 from cryptophyte algae and in trimeric LHCII complex from higher plants. These two examples show how the structural organization determines a directed energy transfer and how equilibration within antenna subunits and migration between subunits are superimposed.

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Section: Exciton-phonon Coupling and Spectral Line Shapesmentioning

confidence: 99%

Physical origins and models of energy transfer in photosynthetic light-harvesting

Novoderezhkin

Grondelle

2010

Phys. Chem. Chem. Phys.

205

271

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“…In the presence of static disorder (disorder of the site energies E n and couplings M nm ), the homogeneous FL profiles should be averaged over a random distribution of E n and M nm that will perturb energies and eigenfunctions of the exciton states. Nonlinear spectral responses can be expressed in terms of the line-broadening functions (Equation 13.4) as well, for example, pump-probe, 74,83,84,87,88,117 Stark spectra, 90,118 three-pulse photon echoes, 116 and 2D echoes. 98 The spectral density needed to evaluate the spectral responses can be obtained from molecular dynamics simulations 35 or can be extracted from experiments, for example, from hole-burning 29 or fluorescence line-narrowing (FLN) spectra.…”

Section: Exciton-phonon Coupling and Spectral Line Shapesmentioning

confidence: 99%

Modeling of energy transfer in photosynthetic light harvesting

Novoderezhkin¹,

Grondelle²

2018

Light Harvesting in Photosynthesis

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“…[3][4][5][6][7][8] The blue shift of the J-band may be understood on the basis of the optical transitions between one-and two-exciton states, 12,13 invoking the concept of onedimensional Fermi-excitons: 14 The analysis of such transitions 12,13 demonstrated an increase of energy of the excited-state absorption, as compared with the ground-state absorption. The influence of static disorder 15,16 and phonons 16 on the phenomenon has also been considered. It is noteworthy that the shiftlike optical changes have been observed in the transient absorption for other molecular complexes as well, including the bacteriochlorophyll ͑BChl͒ molecules in the light harvesting antenna of the photosynthetic purple bacteria.…”

Section: Introductionmentioning

confidence: 99%

Influence of exciton–exciton interaction on one-to-two exciton transitions in molecular aggregates with linear and circular geometries

Juzeliūnas

Reineker

1997

The Journal of Chemical Physics

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One-to two-exciton transitions have been examined in molecular aggregates with linear and circular geometries at various strengths of the exciton-exciton interaction. For the interaction parameter a sufficiently different from its critical value a crit ϭ1, the exciton-exciton interaction has been shown to have little influence on the transition dipole moments, as well as on the corresponding transition energies between the one-exciton states and the dissociated two-exciton states. The interaction between the excitons then may be represented in an effective manner by the replacement of the actual number N of molecules per aggregate by a nearby effective number N eff , the latter being a-dependent. Hence, inclusion of the exciton-exciton coupling does not affect substantially the previous analysis of one-to two-exciton transitions based on the model of noninteracting one-dimensional excitons. That is, effects such as the blue shift of the excited-state absorption and the enhancement of nonlinear susceptibilities are not sensitive to the exciton-exciton interaction. These findings are relevant, inter alia, to J-aggregates in which there is no evidence for the coupling parameter a to be in the critical region or beyond. On the other hand, for the critical value of the exciton-exciton interaction (aϭa crit), the blue shift is either totally absent in the excited-state absorption, or extremely small compared with the ordinary case. The above is in full agreement with earlier calculation of the pump-probe spectrum showing a weak dependence on the exciton-exciton interaction for aϽ1, as well as a strong bleaching of the exciton band in the critical region.

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Optical Stark spectroscopy of molecular aggregates

Cited by 6 publications

References 53 publications

Physical origins and models of energy transfer in photosynthetic light-harvesting

Physical origins and models of energy transfer in photosynthetic light-harvesting

Modeling of energy transfer in photosynthetic light harvesting

Influence of exciton–exciton interaction on one-to-two exciton transitions in molecular aggregates with linear and circular geometries

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