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Energy-transfer and charge-separation pathways in the reaction center of photosystem II revealed by coherent two-dimensional optical spectroscopy
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10.1063/1.3493580
/content/aip/journal/jcp/133/18/10.1063/1.3493580
http://aip.metastore.ingenta.com/content/aip/journal/jcp/133/18/10.1063/1.3493580

Figures

Image of FIG. 1.
FIG. 1.

Tight-binding model of molecular aggregates. Two molecules are shown. First row: the ground state. Second row: excitation of molecule 2 corresponds to creation of hole and electron on that molecule. Third row: CT state corresponds to creation of hole on molecule 2 and an electron on molecule 1. Electrons are marked by solid circles and holes by open circles.

Image of FIG. 2.
FIG. 2.

Ground state, donor, and acceptor state potentials along the reaction coordinate. and are defined with respect to the ground state. and are optical absorption reorganization energies. and used in Marcus theory are defined with respect to equilibrium of the donor and the acceptor states.

Image of FIG. 3.
FIG. 3.

Left: the RC of PS-II. Transition dipoles are represented by arrows. Right: the bath spectral density used in the simulations (Refs. 6 and 7).

Image of FIG. 4.
FIG. 4.

Left: simulated absorption spectra of PS-II RC core at 77 K. Solid black—full model; dotted black—model without CT states. Red curve—square root of pulse power spectrum used in nonlinear optical signal simulations. Vertical lines denote positions of single excitons after reorganization. Contributions of CT states to these eigenstates (from left to right) are 0.94, 0.98, 0.63, 0.07, 0.35, 0, 0.03, 0, and 0. Right: the single-exciton eigenstates below and their reorganization shifts; three additional dark CT states at are not shown. Exciton eigenenergies, , and reorganization-energy shifts, , are shown.

Image of FIG. 5.
FIG. 5.

Exciton population dynamics when all states are initially equally populated, (the three high-energy, CT states are not shown). The states are numbered by their energy ; color code is the same as in Fig. 4.

Image of FIG. 6.
FIG. 6.

2D photon echo (rephasing) signal. Left—full model, middle—Frenkel model (no CT states), and right—the difference. Each plot is scaled according to Eq. (51) and normalized [Eq. (50)] as follows: for left and middle columns, is the maximum at zero delay time; for the right column, is the maximum of each signal.

Image of FIG. 7.
FIG. 7.

Time dependence of integrated amplitudes in regions A–C and their cross-peaks (marked by squares in Fig. 6). The traces are shifted vertically to make the initial amplitude 0.

Image of FIG. 8.
FIG. 8.

The three components contributing to the 2D spectra at two delay times. The amplitudes of the ESE and ESA components have been multiplied by the factors given in each panel. The signal is scaled according to Eq. (51) and [Eq. (50)] is the maximum of each plot.

Image of FIG. 9.
FIG. 9.

2D photon echo (nonrephasing) signal . Left—full model, middle—Frenkel model (no CT states), and right—the difference. The signal is scaled according to Eq. (51) and normalized [Eq. (50)] as follows: for left and middle columns, is the maximum at zero delay time; for the right column, is the maximum of the signal of each plot.

Image of FIG. 10.
FIG. 10.

The three components contributing to the 2D spectra at two delay times. The numbers inside the plots are the relative amplitudes of the component, compared to GSB. Each plot is scaled according to Eq. (51) and normalized [ in Eq. (50)] to the maximum.

Image of FIG. 11.
FIG. 11.

2D double-quantum-coherence signals. Left—full model, middle—Frenkel exciton model (no CT states), and right—the difference. Each plot is scaled according to Eq. (51) and normalized [ in Eq. (50)] to the maximum.

Image of FIG. 12.
FIG. 12.

The two pathways of the signals and their corresponding Feynman diagrams. Each plot is scaled according to Eq. (51) and normalized [ in Eq. (50)] to the maximum.

Tables

Generic image for table
Table I.

Single-exciton Hamiltonian in calculated using 2.9 resolution structure parameters (Ref. 3) [Protein Data Bank (PDB) database file 3BZ1.pdb]. The intermolecular dipole-dipole interactions were computed using transition dipole directions taken from Ref. 27 and transition amplitudes and .

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/content/aip/journal/jcp/133/18/10.1063/1.3493580
2010-11-10
2014-04-20
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Energy-transfer and charge-separation pathways in the reaction center of photosystem II revealed by coherent two-dimensional optical spectroscopy
http://aip.metastore.ingenta.com/content/aip/journal/jcp/133/18/10.1063/1.3493580
10.1063/1.3493580
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