Full visible range two-dimensional electronic spectroscopy with high time resolution.

ABSTRACT

Two-dimensional electronic spectroscopy (2DES) is a powerful method to study coherent and incoherent interactions and dynamics in complex quantum systems by correlating excitation and detection energies in a nonlinear spectroscopy experiment. Such dynamics can be probed with a time resolution limited only by the duration of the employed laser pulses and in a spectral range defined by the pulse spectrum. In the blue spectral range (<500 nm), the generation of sufficiently broadband ultrashort pulses with pulse durations of 10 fs or less has been challenging so far. Here, we present a 2DES setup based on a hollow-core fiber supercontinuum covering the full visible range (400-700 nm). Pulse compression via custom-made chirped mirrors yields a time resolution of <10 fs. The broad spectral coverage, in particular the extension of the pulse spectra into the blue spectral range, unlocks new possibilities for coherent investigations of blue-light absorbing and multichromophoric compounds, as demonstrated by a 2DES measurement of chlorophyll a.