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.
Highlights
Two-dimensional electronic spectroscopy (2DES) is a powerful tool for studying the excitedstate dynamics in various material systems
We introduce a novel configuration for two-dimensional electronic spectroscopy (2DES) that combines the partially collinear pump-probe geometry with active phase locking
The box geometry can only be implemented with pulses of a same color unless extra modulators are added to shape the spectra of individual pulses [47], limiting the range of accessible optical transitions
Summary
Two-dimensional electronic spectroscopy (2DES) is a powerful tool for studying the excitedstate dynamics in various material systems. By measuring the third-order nonlinear optical response as a function of the excitation and emission frequencies as well as the waiting time, 2DES provides insight about the effect of quantum coherence in the electronic dynamics [1,2,3,4]. The box geometry can only be implemented with pulses of a same color unless extra modulators are added to shape the spectra of individual pulses [47], limiting the range of accessible optical transitions. A pair of quartz wedges and a compensation plate installed in the two arms of the interferometer allow to precisely manipulate the phase difference between the two pump pulses, enabling one to recover the 2DES rephasing and non-rephasing signals. Our setup combines the merits of the two geometries with robust phase stabilization, ultrafast time-resolution (< 10 fs), two-color operation, long delay scans, individual polarization manipulation and the ease of implementation
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