Toward Broad Bandwidth 2-D Electronic Spectroscopy: Correction of Chirp From a Continuum Probe

Abstract

Recent implementations of 2-D spectroscopy in the pump-probe geometry using a pulse-shaper demonstrate the ease with which frequency-resolved pump-probe experiments can be readily adapted to 2-D methods. Many frequency-resolved pump-probe experiments employ continuum probes to observe a broad range of electronic transitions. These continuum probes are often chirped, leading to distortions that can be post corrected by characterizing the chirp and appropriately adjusting the observed wavelength-dependent pump-probe time delay. We present an analogous chirp-correction scheme for 2-D spectroscopy, facilitating the use of continuum probing to expand the frequency information available in 2-D spectroscopy experiments. We demonstrate the method through experiments and simulations of a laser dye in solution.