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Ultrafast optical multidimensional spectroscopy without interferometry
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View: Figures


Image of FIG. 1.
FIG. 1.

The flow diagram showing the basic phase retrieval algorithm, as described in the text and previously. (See Ref. 15.)

Image of FIG. 2.
FIG. 2.

The simulated results for a three-level system, as described in the text is shown in part (a). The phase information was discarded and the phase retrieval algorithm was iterated using the data in the domain as pseudoexperimental data. The retrieved 2D data using just the basic error-reduction algorithm (b) reproduce the general features, but there are clearly problems with this recovery. Part (c) shows significant improvement in the recovered 2D spectrum with exponential decay outside the support and smooth initial guesses used. By incorporating several iterations of HIO every 100 iterations, the further improved 2D spectrum, shown in part (d), was recovered.

Image of FIG. 3.
FIG. 3.

The inclusion of several HIO iterations can kick the algorithm out of local minima and into another solution with a lower (or higher) error value. The full red line shows the error metric as a function of iteration number with no HIO iterations. The dashed green line shows the error metric for three HIO iterations after 100 error-reduction iterations, followed by another 297 iterations of the error-reduction algorithm. The dash–dot blue line shows the error following 400 iterations, with three HIO iterations after the first and second 100 error-reduction iterations. The dotted black curve shows the error for 400 iterations, with three iterations of HIO every 100 iterations of error reduction. It can be seen that the first two applications of HIO lead to a lower error, but the final HIO application leads to a solution with a slightly higher error.

Image of FIG. 4.
FIG. 4.

(a) The energy level diagram shows the three-level system used and the energy and interactions of the three incident pulses. (b) The double-sided diagram for the main off-diagonal peak under examination.

Image of FIG. 5.
FIG. 5.

The 2D spectra for simulations with two-color excitation are shown together with the 2D spectra recovered from the intensity data alone. Parts (a) and (b) represent data that have been Fourier transformed with respect to the delay τ, for the case of (a) no inhomogeneous broadening and (b) 20 meV of inhomogeneous broadening. Parts (c) and (d) represent data that have been Fourier transformed with respect to the delay T, for the case of (c) no inhomogeneous broadening and (d) 20 meV of inhomogeneous broadening. In each case, the recovered spectrum agrees very well with the calculated 2D spectrum and different information is obtained in each case. The interpretation of such two-color correlation diagrams is somewhat different to their one-color counterparts, as discussed in the text.

Image of FIG. 6.
FIG. 6.

These two 2D spectra represent nearly homometric solutions for simulated data where it is nearly impossible to arbitrarily determine which solution is the correct one, as both satisfy the support constraints and give equally good fits to the measured intensities. In this case, knowledge about the system acquired from other complementary experiments may be able to assist in the determination of the correct solution. (The vertically elongated peaks seen here correspond to a nonresonant final interaction, as in Raman scattering, and reflect the pulse bandwidth.)

Image of FIG. 7.
FIG. 7.

The laser spectrum, (a), and linear absorption spectrum, (b), for the carotenoid in LHCII used for the 2D experiments. Part (c) shows the spectrally resolved intensity acquired as a function of τ, with the phase information discarded, as used as the input for the phase retrieval algorithm. The 2D spectrum determined from interferometry (see Ref. 31), (d), compares well with the 2D spectrum determined using phase retrieval algorithm, with no prior knowledge of the phase information (e).


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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Ultrafast optical multidimensional spectroscopy without interferometry