Phase-locked pulses for two-dimensional spectroscopy by a birefringent delay line

Two-dimensional electronic spectroscopy (2DES) allows fundamentally new insights into the structure and dynamics of multi-chromophore systems. So far two schemes have been successfully used to implement 2DES in the visible range: the heterodyne detected three-pulse photon echo and the partially collinear pump-probe geometry. The latter employs two phase-locked collinear pump pulses and a non-collinear probe pulse which is dispersed on a spectrometer. Advantages of this configuration are its simplicity, its applicability to standard pump-probe systems and the fact that it automatically measures absorptive spectra.