We describe a potentially powerful multidimensional coherent technique based on spectrally resolved two-color three-pulse femtosecond photon echoes in the visible for probing vibrational and electronic dynamics in the ground and excited states of complex molecular systems. Spectral analysis of the photon echo signals yields detailed information about the temporal evolution of the amplitude of the nonlinear polarization induced in the sample by the three femtosecond pulses, while suitable selection of the wavelengths of the laser pulses allows different sets of energy levels to be selected and the dynamics of vibrational levels in the ground and excited electronic states to be separated and investigated. Two-color photon echo spectra are presented for a range of molecular systems, including the dye molecules Rhodamine 101 and cresyl violet, the biological molecules lycopene and myoglobin, the blue-emitting semiconductor gallium nitride, and semiconductor CdTe/ZnSe quantum dots.
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