TY - JOUR
T1 - Triple-quantum dual-comb two-dimensional coherent spectroscopy resolves velocity-synchronized Dicke states in hot atomic vapors
AU - Deng, Zejiang
AU - Xiong, Shiping
AU - Luo, Daping
AU - Pan, Jiayi
AU - Zhao, Zilin
AU - Hou, Liyuan
AU - Xie, Gehui
AU - Zuo, Zhong
AU - Yu, Shaogang
AU - Zhu, Zhiwei
AU - Gu, Chenglin
AU - Wu, Jian
AU - Li, Wenxue
AU - Zeng, Heping
N1 - Publisher Copyright:
© The Author(s) 2025.
PY - 2025/12
Y1 - 2025/12
N2 - 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.
AB - 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.
UR - https://www.scopus.com/pages/publications/105025462138
U2 - 10.1038/s42005-025-02404-7
DO - 10.1038/s42005-025-02404-7
M3 - 文章
AN - SCOPUS:105025462138
SN - 2399-3650
VL - 8
JO - Communications Physics
JF - Communications Physics
IS - 1
M1 - 498
ER -