Broadband two-dimensional electronic spectroscopy in an actively phase stabilized pump-probe configuration

TLDR: A novel configuration for two-dimensional electronic spectroscopy (2DES) that combines the partially collinear pump-probe geometry with active phase locking is introduced and is demonstrated on a solution sample of CdSe/ZnS nanocrystals by employing two non-collinear optical parametric amplifiers as the pump and probe sources.

Abstract: We introduce a novel configuration for two-dimensional electronic spectroscopy (2DES) that combines the partially collinear pump-probe geometry with active phase locking. We demonstrate the method on a solution sample of CdSe/ZnS nanocrystals by employing two non-collinear optical parametric amplifiers as the pump and probe sources. The two collinear pump pulse replicas are created using a Mach-Zehnder interferometer phase stabilized by active feedback electronics. Taking the advantage of separated paths of the two pump pulses in the interferometer, we improve the signal-to-noise ratio with double modulation of the individual pump beams. In addition, a quartz wedge pair manipulates the phase difference between the two pump pulses, enabling the recovery of the rephasing and non-rephasing signals. Our setup integrates many advantages of available 2DES techniques with robust phase stabilization, ultrafast time resolution, two-color operation, long delay scan, individual polarization manipulation and the ease of implementation.