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Advanced Optical Materials

Phase‐Stable Multidimensional Coherent Spectroscopy Based on Dual‐Comb Interferometry

Zhong Zuo, Chenglin Gu, Siyi Wang, Shiping Xiong, Zejiang Deng, Yuanfeng Di, Daping Luo, Jian Wu, Wenxue Li

Published Jan 4, 2024• 5 citations

Abstract

Abstract Multidimensional coherent spectroscopy (MDCS) is a highly intriguing field for the unique capacities to unravel quantum pathways of microscopic dynamics and discern different dipole–dipole interactions. These capabilities are not simultaneously accessible through any other techniques. The foundation of MDCS lies in the stable phase and accurate time information of the multi‐pulse sequences involved. Achieving the phase stability has traditionally relied on ingenious geometric optical designs and multiple feedback control systems, albeit at the cost of complexity. In this letter, a phase stability scheme for high‐resolution MDCS is proposed by replacing traditional laser sources with two highly coherent frequency combs. By employing dual‐comb interferometry, the phase distribution across a broad spectral range and the time information of all the excitation pulses are precisely measured, even in setups that lack phase stability. In the experiment, a rephasing MDCS of rubidium atoms is obtained by applying this approach, wherein the comb resolution is utilized to differentiate the couplings of hyperfine energy levels. This scheme simplifies the structure of MDCS and holds potential for applications in other MDCS systems involving many‐body interactions and non‐absorptive resonances.

DOI: 10.1002/adom.202303130

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Multidimensional coherent spectroscopy is a powerful method for studying materials’ optical properties. It also has potential to be used for chemical sensing applications as it allows the measurements of samples’ energy level structures as well as couplings between the excited states resonances. This coupling information is the key to identify whether or not the sample contains a mixture of analytes. Coupling information is not easily accessible using one-dimensional linear or non-linear methods, necessitating more complex multidimensional experimental techniques. However, multidimensional techniques require bulky apparatus, complex stabilization schemes, and/or long acquisition times that prevent them from being used outside the lab. Here we propose and demonstrate a new and simple approach that enables the measurements of the main absorption lines as well as the couplings between the excited states resonances extremely fast (tens to hundreds of

\mu \text{s}

) without measuring the full multidimensional spectra. This approach is based on the Fourier-slice theorem and was inspired by frequency comb technology, particularly dual-comb spectroscopy. Our approach uses free-running lasers and co-linear geometry, and with the development of compact lasers this approach can become field-deployable for sensing applications. We demonstrate the concept on rubidium vapor.

Frequency-comb based multidimensional coherent spectroscopy is a novel optical method that enables high-resolution measurement in a short acquisition time. The method's resolution makes multidimensional coherent spectroscopy relevant for atomic systems that have narrow resonances. We use double-quantum multidimensional coherent spectroscopy to reveal collective hyperfine resonances in rubidium vapor at 100 °C induced by dipole-dipole interactions. We observe tilted and elongated line shapes in the double-quantum 2D spectra, which have never been reported for Doppler-broadened systems. The elongated line shapes suggest that the signal is predominately from the interacting atoms that have a near zero relative velocity.

Abstract An introduction to multidimensional coherent spectroscopy (MDCS) is provided in this chapter. We start out by introducing MDCS in qualitative terms, as an extension of transient absorption spectroscopy. We proceed to discuss the meaning and utility of coherent spectroscopy more generally. We go on to discuss the specifics of MDCS as a specific form of coherent spectroscopy. Pulse sequences involved in generating MDCS plots are introduced. Finally, we discuss density matrix perturbation theory and double-sided Feynman diagrams, and the role of this formalism in simulating and interpreting MDCS.