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Optics Letters

Zero-quantum dual-comb spectroscopy of collective resonances in rubidium vapor

Bachana Lomsadze, Johnason Yao, Hankang Gao, Roman Junes

Published Oct 9, 2026• 0 citations
Publisher

Abstract

We report dual-comb spectroscopy of the collective zero-quantum response of rubidium atoms. The observed signals include two-atom collective resonances at 2( ω D 2 − ω D 1 ), ω 5 P 3/2 →5 D − ω D 2 , ω 5 P 3/2 →5 D − ω D 1 , and ( ω D 2 − ω D 1 )+( ω 5 P 3/2 →5 D − ω D 1 ), as well as higher-order three-atom resonances. Unlike double-quantum spectroscopy, which probes sum-frequency resonances of multiple atoms, the zero-quantum pathway probes difference-frequency correlations between optical transitions. In a dual-comb implementation, these signals are independent of the carrier-envelope offset frequencies of both combs, enabling rapid measurements without active carrier-envelope offset stabilization. These results show that zero-quantum dual-comb spectroscopy is a powerful approach for probing collective coherences and many-body correlations in atomic systems.

DOI
10.1364/ol.612562

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We report dual-comb spectroscopy of the collective zero-quantum response of rubidium atoms. The observed signals include two-atom collective resonances at 2( ω D 2 − ω D 1 ), ω 5 P 3/2 →5 D − ω D 2 , ω 5 P 3/2 →5 D − ω D 1 , and ( ω D 2 − ω D 1 )+( ω 5 P 3/2 →5 D − ω D 1 ), as well as higher-order three-atom resonances. Unlike double-quantum spectroscopy, which probes sum-frequency resonances of multiple atoms, the zero-quantum pathway probes difference-frequency correlations between optical transitions. In a dual-comb implementation, these signals are independent of the carrier-envelope offset frequencies of both combs, enabling rapid measurements without active carrier-envelope offset stabilization. These results show that zero-quantum dual-comb spectroscopy is a powerful approach for probing collective coherences and many-body correlations in atomic systems.
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Abstract Two-dimensional coherent spectroscopy (2DCS) combined with dual-comb technology offers unprecedented resolution for probing many-body interactions and correlations in atomic vapors, yet its application to high-order multi-quantum transitions remains challenging due to weaker nonlinear signals and phase instability. Here, we demonstrate a triple-quantum dual-comb 2DCS technique that achieves λ/110 phase stability through digital correction, enabling the observation of velocity-synchronized Dicke states in a thermal rubidium vapor. By resolving collective hyperfine resonances of ⁸⁵Rb and ⁸⁷Rb isotopes with 100 MHz spectral resolution, we reveal that triple-quantum dipole-dipole correlations (0.95) surpass double-quantum counterparts (0.90), indicating tighter velocity matching in higher-order Dicke states. This work establishes a pathway for manipulating multi-atom correlations in Doppler-broadened systems and extends 2DCS to research the many-body interaction in semiconductor exciton and 2D materials.
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.
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.
A multichannel dual-comb spectroscopy (DCS) approach for high-resolution, broadband spectral measurements is presented, demonstrating its effectiveness in studying complex atomic systems. By implementing a photodetector array, we enhance DCS capabilities, addressing the fundamental trade-off between signal-to-noise ratio and spectral coverage. To resolve ambiguities in frequency conversion, we introduced a relative offset in beat-note frequency, ensuring accurate spectral reconstruction. As a proof of concept, the absorption spectrum of samarium ( Sm ) vapor is investigated over a 52-nm range, and several previously unreported absorption lines are detected. This is a step toward “Spectroscopy 2.0,” enabling massively parallel spectroscopic measurements (including those at > 100 T magnetic fields) crucial for atomic physics and fundamental interactions research.
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.