Selective Elimination of Homogeneous Broadening by Multidimensional Spectroscopy in the Electromagnetically Induced Transparency Regime.

The key feature of photon echo-based spectroscopies is a selective elimination of the inhomogeneous broadening. Fast homogeneous dephasing typical for large macromolecules makes it difficult to resolve the congested spectra even if the inhomogeneous component is eliminated. We propose a novel two-dimensional spectroscopy in which a series of temporally separated probe pulses are combined with the strong narrowband control pulse. Using electromagnetically induced transparency originating from the interference between the control and probe pulses, we achieve an observation window for molecular response in narrow spectral intervals significantly smaller than the homogeneous dephasing limit.