A theoretical description of two-dimensional circularly polarized pump-probe spectroscopy was carried out. The 2D CP-PP is an extension of the 2D LP-PP method by replacing the linearly polarized pump field with a circularly polarized one. Although the conceptual generalization was found to be rather straightforward, the CP-PP signal was found to be complicated due to the additional contribution from the quadrupole-pump field interaction. However, by using the specific beam configuration with magic angle beam geometry, it was shown that only the magnetic dipole-pump field interaction contribution can be selectively measured. For a couple of model systems, the 2D CP-PP spectra were numerically calculated and compared with the absorption, CD, and 2D LP-PP spectra.
ASJC Scopus subject areas
- Physics and Astronomy(all)
- Physical and Theoretical Chemistry