Probing anomalous relaxation by coherent multidimensional optical spectroscopy.

Focus on multidimensional optical spectroscopy and imaging

Optical spectroscopy using ultrafast light pulses has undergone a revolution in the last decade due to the introduction and development of multidimensional coherent techniques. These methods build on established coherent spectroscopic techniques, such as photon echoes, but go beyond them by correlating the coherent dynamics during two time periods. The resulting multidimensional spectra have a ...

Unravelling coherent dynamics and energy dissipation in photosynthetic complexes by 2D spectroscopy.

Spectroscopic studies of light harvesting and the subsequent energy conversion in photosynthesis can track quantum dynamics happening on the microscopic level. The Fenna-Matthews-Olson complex of the photosynthetic green sulfur bacteria Chlorobium tepidum is a prototype efficient light-harvesting antenna: it stores the captured photon energy in the form of excitons (collective excitations), whi...

Optical multidimensional coherent SPECTROSCOPY

Probing electron correlations in molecules by two-dimensional coherent optical spectroscopy.

The nonlinear optical signal generated in phenol by three femtosecond pulses with wavevectors k1, k2, and k3 in the phase-matching direction k1 + k2 - k3 is simulated. This two-dimensional coherent spectroscopy (2DCS) signal has a rich pattern containing information on double-excitation states. The signal vanishes for uncorrelated electrons due to interference among quantum pathways and, thus, ...

Two-probe study of hot carriers in reduced graphene oxide

The energy relaxation of carriers in reduced graphene oxide thin films is studied using optical pump-probe spectroscopy with two probes of different colors. We measure the time difference between peaks of the carrier density at each probing energy by measuring a time-resolved differential transmission and find that the carrier density at the lower probing energy peaks later than that at the hig...