Abstract
We demonstrate amplitude, phase and polarization shaping of femtosecond mid-IR pulses using a germanium acousto-optical modulator by independently shaping the frequency-dependent amplitudes and phases of two orthogonally polarized pulses which are then collinearly overlapped using a wire-grid polarizer. We use a feedback loop to set and stabilize the relative phase of the orthogonal pulses. We have also used a wire-grid polarizer to implement polarization-based balanced heterodyne detection for improved signal-to-noise of 2D IR spectra collected in a pump-probe geometry. Applications include coherent control of molecular vibrations and improvements in multidimensional IR spectroscopy.
Highlights
Femtosecond pulse shaping is finding use as a tool for collecting multidimensional spectra [1,2,3,4,5,6,7]
We demonstrate polarization pulse shaping in the mid-infrared, which we anticipate will further improve the utility of pulse shaping for 2D infrared (IR) spectroscopy and the control of ground-state vibrational motions [9,10]
The beams were sent through a wiregrid polarizer and focused onto a mercury cadmium telluride (MCT) detector
Summary
Femtosecond pulse shaping is finding use as a tool for collecting multidimensional spectra [1,2,3,4,5,6,7]. Multidimensional optical spectroscopies are a relatively new set of techniques that correlate coupled electronic or vibrational eigenstates, separate lineshapes into their homogeneous and inhomogeneous components, and measure energy transfer, among other capabilities [1]. The relative phases of the pulses are set so that experiments can be performed in the rotating frame or phase cycling can be utilized to remove scatter [3, 8]. The center frequencies and shapes of the pulses can be designed to perform either time- or frequency-domain experiments [3]. We demonstrate polarization pulse shaping in the mid-infrared, which we anticipate will further improve the utility of pulse shaping for 2D infrared (IR) spectroscopy and the control of ground-state vibrational motions [9,10]
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