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<p>Two-dimensional coherent spectroscopy (2DCS) combined with dual-comb technology offers unprecedented resolution for probing many-body interactions 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, the titled and elongated ellipticity of the three-quantum peak line shape (0.94) is higher than that of the two-quantum (0.84), reveals that triple-quantum 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.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月4日

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  • Zejiang Deng,
  • Shiping Xiong,
  • Daping Luo,
  • Jiayi Pan,
  • Zilin Zhao,
  • Liyuan Hou,
  • Gehui Xie,
  • Zhong Zuo,
  • Shaogang Yu,
  • Zhiwei Zhu,
  • Chenglin Gu,
  • Jian Wu,
  • Wenxue Li,
  • Heping Zeng

摘要

Two-dimensional coherent spectroscopy (2DCS) combined with dual-comb technology offers unprecedented resolution for probing many-body interactions 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, the titled and elongated ellipticity of the three-quantum peak line shape (0.94) is higher than that of the two-quantum (0.84), reveals that triple-quantum 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.