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arXiv:2210.10115 · Optics Letters

Optical two-dimensional coherent spectroscopy of cold atoms

Danfu Liang, Lexter Savio Rodriguez, Haitao Zhou, Yifu Zhu, Hebin Li

Published Nov 21, 2022• 10 citations
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Abstract

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.

DOI
10.1364/ol.478793

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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.
Optical two-dimensional coherent spectroscopy (2DCS) has become a powerful tool for studying energy-level structure, dynamics, and coupling in many systems including atomic ensembles. Various types of two-dimensional (2D) spectra, including the so-called single-quantum, zero-quantum, and double-quantum 2D spectra, of both DDD lines (D1{D}_{1}D1​ and D2{D}_{2}D2​ transitions) of potassium (K) atoms have been reported previously. For rubidium (Rb), a major difference is that the DDD lines are about 15 nm apart as opposed to only about 3 nm for K. Simultaneously exciting both DDD lines of Rb atoms requires a broader laser bandwidth for the experiment. Here, we report a broadband optical 2DCS experiment in a Rb atomic vapor. A complete set of single-quantum, zero-quantum, and double-quantum 2D spectra including both DDD lines of Rb atoms were obtained. The experimental spectra were reproduced by simulated 2D spectra based on the perturbation solutions to the optical Bloch equations. This work in Rb atoms complements previous 2DCS studies of K and Rb with a narrower bandwidth that covers two DDD lines of K or only a single DDD line of Rb. The broadband excitation enables the capability to perform double-quantum and multiquantum 2DCS of both DDD lines of Rb to study many-body interactions and correlations in comparison with K atoms.
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.
Many-body interactions and correlations in atomic ensembles are fundamental in understanding many-body effects such as collective and emergent phenomena and also play an important role in various atom-based applications. Optical two-dimensional coherent spectroscopy (2DCS) provides a powerful tool to measure many-body interactions and correlations. Here, we present the study of many-body dipole-dipole interactions and correlations in potassium and rubidium atomic vapors by using double-quantum and multi-quantum 2DCS. The results show that double-quantum 2DCS provides sensitive and background-free detection of weak dipole-dipole interaction between atoms with a mean separation up to about 16 μm, and multi-quantum 2DCS can excite and detect multi-atom states (Dicke states) with up to eight correlated atoms. The technique of optical 2DCS can provide a new approach to study many-body physics in atomic ensembles and can be potentially implemented to measure many-body effects in cold atoms and other atomic/molecular systems.
We study photoionization of cold rubidium atoms in a strong infrared laser field using a magneto-optical trap (MOT) recoil ion momentum spectrometer. Three types of cold rubidium target are provided, operating in two-dimension (2D) MOT, 2D molasses, and 3D MOT with densities in the orders of 10710^7107 atoms/cm3^33, 10810^8108 atoms/cm3^33, and 10910^9109 atoms/cm3^33, respectively. The density profile and the temperature of 3D MOT are characterized using the absorption imaging and photoionization. The momentum distributions of Rb+^++ created by absorption of two- or three-photon illuminate a dipole-like double-peak structure, in good agreement with the results in the strong field approximation. The yielding momentum resolution of 0.12±0.030.12 \pm 0.030.12±0.03 a.u. is achieved in comparison with theoretical calculations, exhibiting the great prospects for the study of electron correlations in alkali metal atoms through interaction with strong laser pulses.
Femtosecond coherent multidimensional spectroscopy is demonstrated for an ultracold gas. A setup for phase modulation spectroscopy is used to probe the 3 2 S 1/2 –2 2 P 1/2,3/2 transition in an 800 μ K-cold sample of 7 Li atoms confined in a magneto-optical trap. The observation of a double quantum coherence response, a signature of interparticle interactions, paves the way for detailed investigations of few- and many-body effects in ultracold gases using this technique. The experiment combines a frequency resolution of 3 GHz with a potential time resolution of 200 fs, which allows for high-resolution studies of ultracold atoms and molecules both in the frequency and in the time domain.