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 .
Monomer 2D spectra (absorptive parts) calculated for a model of PBI dyes. Panels (a) and (b) show spectra calculated with different resolutions.
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).
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.
Same as Fig. 4 but for an antiparallel transition dipole moment configuration with .
Same as Fig. 4 but for an orthogonal transition dipole moment configuration with .
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.
Phases for the calculation of the third-order polarization.
Article metrics loading...
Full text loading...