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Physical Review A

Multiatom dipole-dipole correlations in rubidium vapor revealed by dual-comb spectroscopy

Anonymous, Roman Junes, Johnason Yao

Published Aug 13, 2026• 1 citation
Publisher
DOI
10.1103/gl56-rx8h

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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.
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.
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.