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Exciton coherence length fluctuations in chromophore aggregates probed by multidimensional optical spectroscopy
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10.1063/1.3442415
/content/aip/journal/jcp/133/1/10.1063/1.3442415
http://aip.metastore.ingenta.com/content/aip/journal/jcp/133/1/10.1063/1.3442415

Figures

Image of FIG. 1.
FIG. 1.

Dipole-dipole intermolecular coupling [Eq. (25), ] for various configurations of transition dipole moments.

Image of FIG. 2.
FIG. 2.

Sample configuration of model in Sec. III A.

Image of FIG. 3.
FIG. 3.

Absorption spectra of weakly coupled tetramer [Eqs. (11), (21), and (22)] in the slow bath limit . Top: two groups of peaks are formed around and . Central: fine peak structure around (left) and around (right) is shown on an expanded scale. Peaks A–D are absorption of clusters of one to four -states (-states). Bottom: peak A on an expanded scale is further structured for very slow bath .

Image of FIG. 4.
FIG. 4.

The 2D photon echo signal [Eq. (12)] from weakly coupled tetramer (parameters correspond to Fig. 3). Both diagonal , and off-diagonal , regions are shown.

Image of FIG. 5.
FIG. 5.

Same as in Fig. 4 but for delay time .

Image of FIG. 6.
FIG. 6.

Moderately coupled (top panels) and strongly coupled (bottom) tetramer in the slow bath limit . From left: absorption spectrum [ Eq. (11)], the 2D photon echo signal [, Eq. (12)] for delay times and .

Image of FIG. 7.
FIG. 7.

Effect of bath timescale in absorption (left panel) and 2D spectrum at delay times (from left to right) , , , of weakly coupled tetramer. Top: Bottom: .

Image of FIG. 8.
FIG. 8.

Sample configuration of transition dipoles of model in Sec. III B.

Image of FIG. 9.
FIG. 9.

Tensor components of the absorption spectrum , Eq. (11)] of a weakly coupled tetramer [Eqs. (24) and (25) and Fig. 8] in the slow bath limit . Top panel: averaged spectrum. Central panels: and components. Bottom panels: component.

Image of FIG. 10.
FIG. 10.

signal (27) for tetramer (Fig. 8) at zero delay times . Molecular tensor components show up in different regions of 2D spectra as marked. Parameters: and .

Image of FIG. 11.
FIG. 11.

Same signal and system as in Fig. 10 but at longer delay time .

Image of FIG. 12.
FIG. 12.

signal (27) for tetramer (Fig. 8) at zero delay time . Parameters and correspond to Figs. 10 and 11. Molecular tensor components show up in different regions of 2D spectra as marked.

Image of FIG. 13.
FIG. 13.

Intensity oscillations at the peak marked at Fig. 12 at short delay times: top (from left): , 0.4, and 0.8; bottom (from left): , 2.2, and 2.8.

Image of FIG. 14.
FIG. 14.

Same signal as in Fig. 12 but at long delay time .

Tables

Generic image for table
Table I.

Spectral analysis of the one-particle Hamiltonian [Eq. (15)] of a tetramer (Fig. 2). For each bath configuration (first column), eigenfrequencies are given as a function of . Solutions (Ferrari–Cardano quartic formula) for characteristic equation of configuration and characteristic equation of configuration are complicated; we designate them by I–IV. Peaks in weak-coupling absorption spectra (Fig. 3) are assigned in the third column along with oscillator strength in the fourth column. Peaks of strong coupling absorption spectrum (bottom panels of Fig. 6) are assigned in the fifth column. Numerical values of and for intermediate coupling (top panels of Fig. 6) are given oscillator strength in the sixth and last columns, respectively.

Generic image for table
Table II.

Density of clusters in aggregate at high temperatures. Combinatorial weight of all-parallel clusters in the chain with random or orientation of dipoles.

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/content/aip/journal/jcp/133/1/10.1063/1.3442415
2010-07-02
2014-04-23
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Exciton coherence length fluctuations in chromophore aggregates probed by multidimensional optical spectroscopy
http://aip.metastore.ingenta.com/content/aip/journal/jcp/133/1/10.1063/1.3442415
10.1063/1.3442415
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