Broadband visible two-dimensional spectroscopy of molecular dyes

Two-dimensional Fourier transform spectroscopy is a promising technique to study ultrafast molecular dynamics. Similar transient absorption spectroscopy, more complete picture of the dynamics requires broadband laser pulses observe changes over large enough bandwidth, exceeding inhomogeneous width electronic transitions, as well separation between or vibronic transitions interest. Here, we present visible 2D spectra series dye molecules and report vibrational coherences with frequencies up ∼1400 cm−1 that were obtained after improvements our existing two-dimensional setup [Al Haddad et al., Opt. Lett. 40, 312–315 (2015)]. The experiment uses white light from hollow core fiber, allowing us acquire bandwidth 200 nm, in range 500 800 temporal resolution 10–15 fs. nile blue, rhodamine 800, terylene diimide, pinacyanol iodide show spectral features at least one mode reveal information about structural motion via coherent oscillations signals during population time. For case iodide, these observations are complemented by its Raman spectrum, calculated activity ground- excited-state geometry.