Two-dimensional electronic spectroscopy with birefringent wedges.

Abstract

We present a simple experimental setup for performing two-dimensional (2D) electronic spectroscopy in the partially collinear pump-probe geometry. The setup uses a sequence of birefringent wedges to create and delay a pair of phase-locked, collinear pump pulses, with extremely high phase stability and reproducibility. Continuous delay scanning is possible without any active stabilization or position tracking, and allows to record rapidly and easily 2D spectra. The setup works over a broad spectral range from the ultraviolet to the near-IR, it is compatible with few-optical-cycle pulses and can be easily reconfigured to two-colour operation. A simple method for scattering suppression is also introduced. As a proof of principle, we present degenerate and two-color 2D spectra of the light-harvesting complex 1 of purple bacteria.