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Cell Reports Physical Science

Dynamic manipulation of atom spins via AC Stark effect in ultra-sensitive quantum magnetic sensing

Chenyi Zhou, Y. H. Yan, Ying Zhou, Yuesong Wu, Xiaoshu Ding, Kaixuan Zhang, Zhuo Wang, Jixi Lu

Published Mar 26, 2026• 0 citations
Publisher

Abstract

Although the AC Stark effect has long been viewed as a detrimental perturbation in atomic spin-based quantum sensing, recent work shows that all-optical dynamic spin manipulation based on this effect eliminates the need for auxiliary magnetic fields and extracts more comprehensive information. Nevertheless, the AC Stark effect and optical pumping are intrinsically coupled due to their dependence on shared optical parameters, inducing unintended dynamic pumping that disturbs the desired spin manipulation. This work presents a symmetric dual-sideband detuning-modulated optical excitation scheme, which decouples the two mechanisms and enables independent dynamic optical spin manipulation with stable pumping. The suppression of dynamic pumping-induced perturbations achieved by our method enables all-optical control while allowing simultaneous multi-axis measurement of magnetic fields. This achieves a two-order-of-magnitude suppression of inter-axis crosstalk in the SERF regime. This work provides a new method for broadening quantum sensing using the AC Stark effect in optical pumping atomic devices.

DOI
10.1016/j.xcrp.2026.103209

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Although the AC Stark effect has long been viewed as a detrimental perturbation in atomic spin-based quantum sensing, recent work shows that all-optical dynamic spin manipulation based on this effect eliminates the need for auxiliary magnetic fields and extracts more comprehensive information. Nevertheless, the AC Stark effect and optical pumping are intrinsically coupled due to their dependence on shared optical parameters, inducing unintended dynamic pumping that disturbs the desired spin manipulation. This work presents a symmetric dual-sideband detuning-modulated optical excitation scheme, which decouples the two mechanisms and enables independent dynamic optical spin manipulation with stable pumping. The suppression of dynamic pumping-induced perturbations achieved by our method enables all-optical control while allowing simultaneous multi-axis measurement of magnetic fields. This achieves a two-order-of-magnitude suppression of inter-axis crosstalk in the SERF regime. This work provides a new method for broadening quantum sensing using the AC Stark effect in optical pumping atomic devices.
In a spin-exchange-relaxation-free (SERF) atomic magnetometer with ultrahigh sensitivity, the ac-Stark shift generated by circularly polarized light results in the attenuation of the SERF atomic magnetometer response, and the virtual magnetic field gradient induced by the ac-Stark shift can reduce the sensitivity of the SERF atomic magnetometer. In this paper, we use a hybrid optical pumping method to address the ac-Stark shift problem. By switching between left-hand and right-hand circularly polarized lights and compensating the residual magnetic field of the magnetometer, the ac-Stark shift could be reduced and then suppressed effectively.
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In atomic spin sensors based on optical pumping, pump beam instabilities can drive atomic spin polarization fluctuations, referred to here as pump-induced spin polarization noise, which may limit sensitivity and long-term stability. Because the local pump field inside the cell can differ from that inferred from external optical diagnostics, it remains difficult to directly quantify the actual in situ spin polarization noise and to evaluate and suppress its contribution to the sensor noise floor. Here, we propose an in situ decoupling method based on spin dynamics, in which a large longitudinal detuning field suppresses magnetic field and rotation responses, while a transverse projection field converts pump-induced fluctuations in longitudinal spin polarization into a measurable transverse spin signal. Demonstrated in a K-Rb-21Ne spin exchange relaxation free (SERF) comagnetometer, the proposed method suppresses the magnetic-field response by approximately 180-fold and enhances the pump-power-noise response by approximately 380-fold, thereby enabling effective separation and evaluation of pump-induced spin polarization noise. The method employs the atomic ensemble as an in situ probe of the spin dynamic response to the local pump optical field. It enables quantitative identification of pump fluctuation associated noise and direct evaluation of optical field stability under actual operating conditions, thereby providing an experimental basis for optical field stabilization and noise suppression assessment in SERF comagnetometers and related alkali atomic spin sensors.
The sensitivity of existing all-optical atomic magnetometers is significantly compromised due to the simultaneous influence of optical parameters on both optical pumping and optical modulation of atoms. The tight interlinkage of these processes poses challenges for their individual optimization, thereby restricting the achievable sensitivity. To address this issue, we developed a comprehensive optical modulation analytical model that fully considers the effects of dynamic optical pumping. Building upon this model, we introduced a multi-objective optimization method for optical parameters, leading to minimal non-sensitive axis crosstalk and optimal sensitivity. Experimental results demonstrated a femtotesla all-optical spin-exchange relaxation-free magnetometer with sensitivities of 2 fT/Hz1/2 along the y-axis and 4 fT/Hz1/2 along the x-axis, respectively. This advancement surpasses the sensitivity of existing optically modulated magnetometers and bears profound implications for the advancement and application of arrayed magnetometers.
The coherent control of carrier spin states in semiconductor quantum dots (QDs) is a key requirement for certain quantum information applications, particularly where lightmatter interactions are involved such as in the generation of spin-photon entangled states. A widely used approach for spin control involves Larmor precession in an externally applied magnetic field. Increasing the magnetic field strength enhances the spin precession rate, thus improving the photon generation rate. However, this also introduces Zeeman splitting, which lifts the spin-state degeneracy. As a result frequency distinguishability is introduced, reducing the fidelity of the entangled spinphoton states. This work explores a novel approach to mitigate the Zeeman splitting by employing the AC Stark effect via a red-detuned laser. The Stark shift counteracts the Zeeman energy difference, effectively restoring transition degeneracy within the transition linewidth while allowing for an increased magnetic field strength and consequently a faster precession rate. Theoretical modelling demonstrates that this technique enables an almost doubling of the current spin precession frequency while maintaining nearly degenerate optical transitions. To validate this approach, a high-precision optical system is under development to probe QD emission under simultaneous magnetic and optical fields. Simulations incorporating both effects confirm the feasibility of this method for eliminating frequency distinguishability. These results lay the groundwork for the development of scalable quantum dot-based photonic platforms for quantum communication and information processing.