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Probing the geometry dependence of molecular dimers with two-dimensional-vibronic spectroscopy
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Image of FIG. 1.
FIG. 1.

The pulse sequence examined in this paper: three ultrashort laser pulses of equal center frequencies interact at different times to induce a time-dependent polarization in an ensemble of molecules. The second and third pulses are identical and time delayed by time with respect to the first pulse . The time variable is defined to have its origin at the delay time . The combined interaction of the three pulses results in the emission of a signal pulse .

Image of FIG. 2.
FIG. 2.

Monomer 2D spectra (absorptive parts) calculated for a model of PBI dyes. Panels (a) and (b) show spectra calculated with different resolutions.

Image of FIG. 3.
FIG. 3.

Geometry dependent excitation scheme for three choices of the orientational angle , as indicated. This angle measures the relative orientation of the transition dipole moments and . The respective orientations are sketched for the three angles in the respective panels. The electric fields couple the electronic ground state with the coupled one-exciton state and the one-exciton state with the two-exciton state , respectively. Also shown are the linear absorption spectra (solid lines) and the monomer spectrum (dashed line).

Image of FIG. 4.
FIG. 4.

Dimer spectra for a parallel transition dipole moment configuration . Panel (b) shows the spectrum for the four-level electronic system illustrated in Fig. 3. Panel (a) shows the complete vibronic 2D spectrum.

Image of FIG. 5.
FIG. 5.

Same as Fig. 4 but for an antiparallel transition dipole moment configuration with .

Image of FIG. 6.
FIG. 6.

Same as Fig. 4 but for an orthogonal transition dipole moment configuration with .

Image of FIG. 7.
FIG. 7.

Simulated 2D spectra of the PBI dimer. Panels (a) and (b) differ by their resolution. In the case of the higher resolution [panel (a)] the vibrational substructure is visible.


Generic image for table
Table I.

Phases for the calculation of the third-order polarization.


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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Probing the geometry dependence of molecular dimers with two-dimensional-vibronic spectroscopy