Two-dimensional electronic-Raman spectroscopy

Abstract

We present a new technique, two-dimensional electronic-Raman spectroscopy (2DER), which combines femtosecond stimulated Raman spectroscopy and a pulse-shaper-assisted 2D spectroscopic scheme for the actinic pump. The 2DER spectrum presents the initial actinic excitation wavelength with nanometer spectral resolution in the first axis and the detected stimulated Raman spectra in the second axis. We measured the correlation of the electronic and vibrational states in the photosynthetic accessory pigment β-carotene and reveal its photoexcited state manifold.