© 2026 Aqora Quantum S.A.S.

Terms Privacy Legal Notice

arXiv:1711.03659 · Physical Review Letters

Frequency-Comb Based Double-Quantum Two-Dimensional Spectrum Identifies Collective Hyperfine Resonances in Atomic Vapor Induced by Dipole-Dipole Interactions

Bachana Lomsadze, Steven T. Cundiff

Published Jun 8, 2018• 74 citations

Abstract

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.

DOI: 10.1103/physrevlett.120.233401

Related papers

Triple-quantum dual-comb two-dimensional coherent spectroscopy resolves velocity-synchronized Dicke states in hot atomic vapors

Zejing Deng, Zilin Zhao, Wenxue Li +5 more

Two-dimensional coherent spectroscopy (2DCS) combined with dual-comb technology offers unprecedented resolutionfor probing many-body interactions in atomic vapors, yet its application to high-order multi-quantumtransitions remainschallenging due to weaker nonlinear signals and phase instability. Here, we demonstrate a triple-quantumdual-comb2DCS 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 and87Rbisotopes with 100 MHz spectral resolution, the titled and elongated ellipticity of the three-quantum peak line shape (0.94)is higher than that of the double-quantum (0.84), reveals that triple-quantum (TQS) correlations (0.95) surpass double-quantum counterparts (0.90), indicating tighter velocity matching in higher-order Dicke states. This work provides a pathway for manipulating multi-atom correlations in Doppler-broadened systems, and greatly assists to characterize complex hyperfine many-body interaction in semiconductor exciton and two-dimensional materials.

Optical and Quantum Sensing and Precision Metrology II•Mar 5, 2026•0 citations

Triple-quantum dual-comb two-dimensional coherent spectroscopy resolves velocity-synchronized Dicke states in hot atomic vapors

Zejiang Deng, Shiping Xiong, Daping Luo +11 more

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.

Communications Physics•Dec 4, 2025•1 citation

Frequency comb-based multidimensional coherent spectroscopy

T. Cundiff Steven, Bachana Lomsadze

We present multidimensional coherent spectroscopy that utilizes frequency combs and multi-heterodyne detection. We demonstrate its capability to measure collective hyperfine resonances in atomic vapor induced by long-range dipole-dipole interactions.

EPJ Web of Conferences•Jan 1, 2019•0 citations

Tri-Comb Multidimensional Coherent Spectroscopy

Bachana Lomsadze, Steven T. Cundiff

We review tri-comb spectroscopy, a novel optical approach to nonlinear spectroscopy. This optical method that we have recently developed enables the measurement of comb resolution multidimensional coherent spectra in under one second. We show the improvement in resolution and acquisition speed by applying the method to Doppler broadened rubidium vapor. We also show how this method can be used for real-time chemical sensing applications.

IEEE Photonics Technology Letters•Oct 18, 2019•29 citations

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

Bachana Lomsadze, Johnason Yao, Hankang Gao +1 more

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.

Optics Letters•Oct 9, 2026•0 citations

Multidimensional coherent spectroscopy of atomic ensembles

Hebin Li, Bachana Lomsadze, Galan Moody +2 more

Abstract Multidimensional coherent spectroscopy (MDCS) of atomic ensembles is discussed in this chapter. Atomic vapors such as potassium and rubidium atomic vapors are used a model system for demonstrating MDCS. The technique of MDCS can also be used to probe many-body dipole-dipole interaction and correlation in atoms by using double-quantum 2D spectroscopy. Multi-quantum 2D spectroscopy can detect many-body correlations associated with coherent states of multiple atoms in atoms.

•Feb 28, 2023•0 citations

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.

Two-dimensional coherent spectroscopy (2DCS) combined with dual-comb technology offers unprecedented resolutionfor probing many-body interactions in atomic vapors, yet its application to high-order multi-quantumtransitions remainschallenging due to weaker nonlinear signals and phase instability. Here, we demonstrate a triple-quantumdual-comb2DCS 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 and87Rbisotopes with 100 MHz spectral resolution, the titled and elongated ellipticity of the three-quantum peak line shape (0.94)is higher than that of the double-quantum (0.84), reveals that triple-quantum (TQS) correlations (0.95) surpass double-quantum counterparts (0.90), indicating tighter velocity matching in higher-order Dicke states. This work provides a pathway for manipulating multi-atom correlations in Doppler-broadened systems, and greatly assists to characterize complex hyperfine many-body interaction in semiconductor exciton and two-dimensional materials.

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.

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.