Two-dimensional electronic spectroscopy with a continuum probe

We report 2D Fourier transform electronic spectroscopy obtained in the pump-probe geometry using a continuum probe. An acousto-optic pulse shaper placed in the pump arm of a standard pump-continuum probe experiment permits 2D spectroscopy that probes a broad spectral range. We demonstrate the method on a simple dye system exhibiting vibrational wavepacket dynamics that modulate the peak shapes of the 2D spectra. The broad spectral range of the continuum probe allows us to observe vibronic cross peaks in the 2D spectra. (C) 2009 Optical Society of America