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Frontiers in Optics

Collinear Optical 2D Coherent Spectroscopy with 5-kHz Repetition Rate Femtosecond Laser

Stephen Revesz, Rustam Gatamov, Adolfo Misiara, Hebin Li

Published Jan 1, 2024• 0 citations
Publisher

Abstract

We demonstrate optical two-dimensional coherent spectroscopy in a collinear geometry on rubidium vapor with time-integrated fluorescence detection using a low-repetition rate femtosecond laser for both excitation and as reference with a pulse shaper.
DOI
10.1364/fio.2024.jw5a.61

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Optical two-dimensional coherent spectroscopy (2DCS) is a powerful ultrafast spectroscopic technique that can greatly benefit from the unique features of a femtosecond laser operating at a kHz repetition rate. However, isolating specific nonlinear signal in the collinear geometry, especially with a kHz laser, presents challenges. We present an experimental implementation of optical 2DCS in a collinear geometry using a femtosecond laser operating at a 5 KHz repetition rate. The desired nonlinear signal is selectively extracted in the frequency domain by lock-in detection. Both pump-probe and optical 2DCS experiments were conducted on a rubidium vapor. The signal-to-noise ratio of pump-probe and 2DCS spectra was characterised under various experimental parameters. The study highlights the importance of the lock-in reference frequency in overcoming the limitations imposed by low repetition rates, thereby paving the way for the application of collinear optical 2DCS in material systems requiring kHz femtosecond lasers.
Femtosecond phase-coherent two-dimensional (2D) spectroscopy has been experimentally demonstrated as the direct optical analog of 2D nuclear magnetic resonance. An acousto-optic pulse shaper created a collinear three-pulse sequence with well-controlled and variable interpulse delays and phases,which interacted with a model atomic system of rubidium vapor. The desired nonlinear polarization was selected by phase cycling (coadding experimental results obtained with different interpulse phases). This method may enhance our ability to probe the femtosecond structural dynamics of macromolecules.
We report an experimental demonstration of optical two-dimensional coherent spectroscopy (2DCS) in cold atoms. The experiment integrates a collinear 2DCS setup with a magneto-optical trap (MOT), in which cold rubidium (Rb) atoms are prepared at a temperature of approximately 200 µK and a number density of 10 10 cm −3 . With a sequence of femtosecond laser pulses, we first obtain one-dimensional second- and fourth-order nonlinear signals and then acquire both one-quantum and zero-quantum 2D spectra of cold Rb atoms. The capability of performing optical 2DCS in cold atoms is an important step toward optical 2DCS study of many-body physics in cold atoms and ultimately in atom arrays and trapped ions. Optical 2DCS in cold atoms/molecules can also be a new avenue to probe chemical reaction dynamics in cold molecules.
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As optical two-dimensional coherent spectroscopy (2DCS) is extended to a broader range of applications, it is critical to improve the detection sensitivity of optical 2DCS. We developed a fast phase-cycling scheme in a non-collinear optical 2DCS implementation by using liquid crystal phase retarders to modulate the phases of two excitation pulses. The background in the signal can be eliminated by combining either two or four interferograms measured with a proper phase configuration. The effectiveness of this method was validated in optical 2DCS measurements of an atomic vapor. This fast phase-cycling scheme will enable optical 2DCS in novel emerging applications that require enhanced detection sensitivity.