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arXiv:2112.04642 · Physical Review Letters

Collective Resonance of D States in Rubidium Atoms Probed by Optical Two-Dimensional Coherent Spectroscopy

Danfu Liang, Yifu Zhu, Hebin Li

Published Mar 7, 2022• 16 citations
arXivHTMLPDF

Abstract

Collective resonance of interacting particles has important implications in many-body quantum systems and their applications. Strong interactions can lead to a blockade that prohibits the excitation of a collective resonance of two or more nearby atoms. However, a collective resonance can be excited with the presence of weak interaction and has been observed for atoms in the first excited state (P state). Here, we report the observation of collective resonance of rubidium atoms in a higher excited state (D state) in addition to the first excited state. The collective resonance is excited by a double-quantum four-pulse excitation sequence. The resulting double-quantum two-dimensional (2D) spectrum displays well-isolated peaks that can be attributed to collective resonances of atoms in P and D states. The experimental one-quantum and double-quantum 2D spectra can be reproduced by a simulation based on the perturbative solutions to the optical Bloch equations, confirming collective resonances as the origin of the measured spectra. The experimental technique provides a new approach for preparing and probing collective resonances of atoms in highly excited states.

DOI
10.1103/physrevlett.128.103601

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Collective resonance of interacting particles has important implications in many-body quantum systems and their applications. Strong interactions can lead to a blockade that prohibits the excitation of a collective resonance of two or more nearby atoms. However, a collective resonance can be excited with the presence of weak interaction and has been observed for atoms in the first excited state (P state). Here, we report the observation of collective resonance of rubidium atoms in a higher excited state (D state) in addition to the first excited state. The collective resonance is excited by a double-quantum four-pulse excitation sequence. The resulting double-quantum two-dimensional (2D) spectrum displays well-isolated peaks that can be attributed to collective resonances of atoms in P and D states. The experimental one-quantum and double-quantum 2D spectra can be reproduced by a simulation based on the perturbative solutions to the optical Bloch equations, confirming collective resonances as the origin of the measured spectra. The experimental technique provides a new approach for preparing and probing collective resonances of atoms in highly excited states.
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.
We report a novel, to the best of our knowledge, double-quantum-zero-quantum two-dimensional coherent spectroscopy (2DCS) that allows direct detection of the quantum coherence between multiparticle collective states. Through correlating the double-quantum coherence and the zero-quantum coherence, signatures for coherence between collective states can be well isolated as side peaks and readily identified in the 2D spectrum. The experiment is implemented in a vapor of rubidium atoms in a collinear 2DCS setup. Good agreement with a theoretical simulation using density matrix confirms the essential role of the interatomic correlation effect in generating the side peak signals. This 2D spectrum technique paves a new avenue for studying the coherent coupling of highly excited states and many-body properties.
Quantum coherence of collective states plays a pivotal role in understanding many-body cooperative behaviors. Collective coherences between the ground state and excited states in potassium atoms were previously revealed; however, the coherence between collectively excited states has hitherto been overlooked, and its observation has remained challenging. Here we present a joint experimental and theoretical investigation of coherence effects in K atomic vapor using two-dimensional coherent spectroscopy. By collecting zero-quantum, double-quantum, and double-quantum--zero-quantum two-dimensional spectra, distinct coherence signatures are spectroscopically accessible. The experimental spectra are well reproduced by numerically solving the time dependence of the Lindblad equation, and further analyses unveil nonradiative coherence as the origin of the observations. Our work provides comprehensive insight into the collective coherence effect in multiatom systems.
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.