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This research advances quantum spectroscopy by introducing a computation-assisted method to isolate weak higher-order nonlinear signals from dominant lower-order noise in rubidium vapor experiments. By successfully extracting 7th-order contributions alongside standard 3rd-order components, the technique enables direct observation of many-body dynamics previously obscured by spectral overlap without requiring reduced pulse intensities. The approach offers a scalable solution for probing ultrafast collective quantum behaviors using existing multidimensional spectroscopy platforms.
Beyond-Third-Order Quantum Coherence in Two-Dimensional Spectroscopy via Order-Selective Isolation
arXiv:2606.12794v1 Announce Type: new Abstract: A central challenge in nonlinear spectroscopy is the order-selective readout of weak higher-order responses that spectrally overlap with dominant lower-order signals. This bottleneck is particularly severe in two-dimensional (2D) spectroscopy, where extending conventional phase-cycling schemes to higher orders rapidly increases measurement and analysis complexity. Here we introduce a computation-assisted strategy that combines rotating-frame acquisition with a frame-shift tracking algorithm to separate signals by their frame-dependent spectral shifts. In a rubidium vapor experiment, we use this approach to isolate a 7th-order nonlinear contribution from coexisting 3rd-order components, enabling direct access to higher-order quantum-coherence dynamics without sacrificing operation at comparatively high pulse intensities. The method is broadly compatible with multidimensional spectroscopy platforms and provides a practical route to probing many-body and collective ultrafast dynamics beyond third order.
Abstract:A central challenge in nonlinear spectroscopy is the order-selective readout of weak higher-order responses that spectrally overlap with dominant lower-order signals. This bottleneck is particularly severe in two-dimensional (2D) spectroscopy, where extending conventional phase-cycling schemes to higher orders rapidly increases measurement and analysis complexity. Here we introduce a computation-assisted strategy that combines rotating-frame acquisition with a frame-shift tracking algorithm to separate signals by their frame-dependent spectral shifts. In a rubidium vapor experiment, we use this approach to isolate a 7th-order nonlinear contribution from coexisting 3rd-order components, enabling direct access to higher-order quantum-coherence dynamics without sacrificing operation at comparatively high pulse intensities. The method is broadly compatible with multidimensional spectroscopy platforms and provides a practical route to probing many-body and collective ultrafast dynamics beyond third order.
Quantum Physics (quant-ph); Optics (physics.optics)
arXiv:2606.12794 [quant-ph]
(or arXiv:2606.12794v1 [quant-ph] for this version)
https://doi.org/10.48550/arXiv.2606.12794 Focus to learn more arXiv-issued DOI via DataCite (pending registration)
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