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Vibrational wave packet induced oscillations in two-dimensional electronic spectra. I. Experiments
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10.1063/1.3404404
/content/aip/journal/jcp/132/18/10.1063/1.3404404
http://aip.metastore.ingenta.com/content/aip/journal/jcp/132/18/10.1063/1.3404404
View: Figures

Figures

Image of FIG. 1.
FIG. 1.

(a) Linear absorption spectrum of PERY in toluene (black solid line) and spectrum of the excitation pulses (green dashed line). The red line indicates the position of the lowest energy transition obtained from ZINDO/S calculations. The inset shows the chemical structure of PERY. (b) Huang–Rhys factors determined from semiemprical AM1 calculations. Only modes that posses Huang–Rhys factors larger than 0.005 are plotted.

Image of FIG. 2.
FIG. 2.

(a) Side and front views on the B3LYP/SV(P) optimal structure of PERY in the electronic ground state. (b) Visualization of the HOMO (bottom) and LUMO (top) obtained from ZINDO/S//B3LYP/SV(P) calculations.

Image of FIG. 3.
FIG. 3.

(a) Schematic setup for recording 2D electronic spectra. (BS) beamsplitter, (CP) compensation plate, (SM) spherical mirror, (DOE) diffractive optical element, (WP) wedge pair, (ND) neutral density filter, (S) sample, (L) lens, (CCD) charge-coupled-device camera. (b) Designation of pulses and time delays in four wave mixing experiments.

Image of FIG. 4.
FIG. 4.

(a) Real and (b) imaginary part of the 2D spectra of PERY in toluene for -delays of 100, 200, 300, 450, 550, 650, and 800 fs. The first, second, and third column of each panel display the corresponding total signal, the rephasing, and the nonrephasing part, respectively. All total spectra are normalized to their absolute maximum value, whereas the rephasing and nonrephasing parts are plotted with their respective contribution to the total signal. Contour lines are drawn at 5% intervals starting at ±10%. Red lines indicate positive signals, blue lines negative ones. The solid line in the real part indicates the diagonal, whereas the black lines in the imaginary part are drawn at the zero crossings between the positive and negative features.

Image of FIG. 5.
FIG. 5.

(a) Amplitude and (b) phase of the 2D spectra of PERY in toluene recorded at -delays of 100, 200, 300, 450, 550, 650, and 800 fs. The first, second, and third column of each panel display the corresponding total signal, the rephasing and the nonrephasing part, respectively. The amplitude part total spectra are normalized to their absolute maximum value, whereas the rephasing and nonrephasing parts are plotted with their respective contribution to the total signal. Contour lines are drawn at 5% intervals starting at 10% in the amplitude part spectra and at intervals in the phase spectra. The zero-phase line is indicated in each phase spectrum. Note the different spectral range in the representation of the phase spectra.

Image of FIG. 6.
FIG. 6.

The four Feynman diagrams graphically illustrating the Liouville space pathways for a two-level system within the rotating wave approximation. and denote ground and excited state, respectively.

Image of FIG. 7.
FIG. 7.

Oscillating features extracted from the 2D spectra of PERY in toluene. (a) Ellipticity (filled circles) and CLS (open circles) of the peak in the real 2D spectra. (b) Relative amplitudes of the rephasing (filled circles) and the nonrephasing (open circles) part of the real 2D spectra. (c) Inhomogeneity index extracted from the real part 2D spectra as defined in Eq. (4). (d) Slope of the nodal line separating the positive and negative feature in the imaginary 2D spectra. (e) Slope of the phase line in the phase 2D spectra.

Image of FIG. 8.
FIG. 8.

One-dimensional four-wave mixing signals of PERY in toluene. Top and bottom panels share the same abscissa, color scales are shown as insets in the bottom panels. (a) Three-pulse photon echo peak-shift trace (top) and the corresponding frequency integrated three-pulse photon echo signal as a function of delay and . (b) Frequency integrated (top) and frequency resolved (bottom) TG signal. (c) Frequency integrated (top) and frequency resolved (bottom) PP signal.

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/content/aip/journal/jcp/132/18/10.1063/1.3404404
2010-05-14
2014-04-20
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Vibrational wave packet induced oscillations in two-dimensional electronic spectra. I. Experiments
http://aip.metastore.ingenta.com/content/aip/journal/jcp/132/18/10.1063/1.3404404
10.1063/1.3404404
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