Two-Color Two-Dimensional Electronic Spectroscopy Using Dual Acousto-Optic Pulse Shapers for Complete Amplitude, Phase, and Polarization Control of Femtosecond Laser Pulses

Abstract

We demonstrate a dual pulse-shaper setup capable of independent polarization, phase, and amplitude control over each pulse. By using active phase stabilization, we achieve a phase stability of ~λ/314 between the two pulse shapers, making the dual-shaper setup suitable for both two-quantum and one-quantum measurements. The setup is compact and easily switchable between pump-probe and collinear geometries. We further illustrate the functionality of the dual-shaper setup by performing two-color 2D visible spectroscopy on colloidal CdSe quantum dots in pump-probe geometry.

Frequency-domain two-dimensional infrared spectroscopy using an acousto-optic programmable dispersive filter

“…The two leading pulse-shaping technologies rely either on a zero-dispersion line (ZDL) including a liquid-crystal [9] or acousto-optic [10] modulator placed in the Fourier plane, or on a more compact acousto-optic programmable dispersive filter (AOPDF) [11]. Applications to 2DES have been successfully demonstrated both with ZDL [12,13] and AOPDF [7,14] pulse shapers. In the mid-infrared (MIR) spectral domain, pulse shaping technologies have matured more recently due to an initial lack of suitable modulators.…”

Dispersion-free continuum two-dimensional electronic spectrometer

“…The delay between pulses 1 and 2 can also be encoded along a spatial dimension, where multiple time delays are directly imaged on a camera in a single experiment [32,33]. Moreover, delays can be set using spatial light modulators [34] or acousto-optic modulators [19,35–38]. Finally, the Soleil–Babinet compensator has recently been used for generating a time delay between two pulses [39].…”

Phase and polarization changes of pulsed Gaussian beams during focusing and propagation

“…Using pulses with more complex polarization states than linear can yield polarization-formed terahertz fields [64], or can help to reach optimal control on the irradiated molecules or other materials, which is often mentioned as a way of coherent control [65][66][67][68][69]. On a similar basis, polarization control showed to be advantageous in pump-probe measurements of two-dimensional spectroscopy techniques [70,71]. A femtosecond pulse with a given time-dependent polarization state is also a widely used tool for isolated attosecond pulse generation [41], and a polarization-shaped pulse has been proposed as a tool for CEP determination [72].…”

“…While in the majority of laser applications the polarization state is not considered -because the generated pulsed light is usually linearly polarized and can be treated theoretically as a scalar -, more and more studies are published where pulsed waves with complex polarization states are used [41,[64][65][66][67][68][69][70][71][72].…”

“…As it was detailed in the introduction, tailoring the temporal variation of the polarization state of few-cycle pulses has been introduced recently as a new way of coherent control [64][65][66][67][68][69][70][71][72]. In the experiments, these polarization-shaped pulses are also focused.…”