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arXiv:2511.01313

Light-induced Frequency Shift and Relaxation of Ground-State 3He via Metastability-Exchange Collisions

L. Y. Wu, H. Yan

quant-phphysics.atom-phSubmitted Nov 3, 2025• Announced Nov 4, 2025
arXivHTMLPDF

Abstract

Metastability-exchange collisions (MECs) lie at the heart of metastability-exchange optical pumping (MEOP) in 3He, enabling the transfer of polarization from the metastable state to the ground state, as well as the optical detection of nuclear magnetic resonance. Leveraging MECs, optically pumped 3He nuclear magnetometers have been developed since the earliest demonstrations of MEOP. However, it also induces an additional frequency shift and relaxation of the nuclear spin precession, thereby limiting the sensitivity of the magnetometer. In this work, we identify a new source of frequency shift and relaxation in the 3He nuclear spin, arising from the light shift. This effect arises from an MEC-mediated interaction between light and the nucleon spin. We develop a theoretical model to describe this light-induced effect and highlight its significance in low magnetic fields. This effect is experimentally demonstrated, and its dependence on various parameters -- including magnetic field strength, light intensity, and wavelength -- is investigated. Our result provides a better understanding of the frequency shift and relaxation of 3He spin precession under MEOP conditions. Moreover, our experiment reveals an MEC-mediated coupling between the 3He nuclear spin and light, which may indicate the feasibility of MEC-assisted optical manipulation of 3He nuclear spins at the quantum level, as proposed in several theoretical schemes.

Comments
9 pages, 5 figures

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Metastability-exchange collisions (MECs) lie at the heart of metastability-exchange optical pumping (MEOP) in 3He, enabling the transfer of polarization from the metastable state to the ground state, as well as the optical detection of nuclear magnetic resonance. Leveraging MECs, optically pumped 3He nuclear magnetometers have been developed since the earliest demonstrations of MEOP. However, it also induces an additional frequency shift and relaxation of the nuclear spin precession, thereby limiting the sensitivity of the magnetometer. In this work, we identify a new source of frequency shift and relaxation in the 3He nuclear spin, arising from the light shift. This effect arises from an MEC-mediated interaction between light and the nucleon spin. We develop a theoretical model to describe this light-induced effect and highlight its significance in low magnetic fields. This effect is experimentally demonstrated, and its dependence on various parameters -- including magnetic field strength, light intensity, and wavelength -- is investigated. Our result provides a better understanding of the frequency shift and relaxation of 3He spin precession under MEOP conditions. Moreover, our experiment reveals an MEC-mediated coupling between the 3He nuclear spin and light, which may indicate the feasibility of MEC-assisted optical manipulation of 3He nuclear spins at the quantum level, as proposed in several theoretical schemes.
Highly polarized 3He ensembles prepared by metastability-exchange optical pumping (MEOP) have been widely used in precision measurements and fundamental physics. Metastability-exchange (ME) collisions, serving as the basis of MEOP, are traditionally described in terms of atomic orientation, while the significant contributions of metastable alignment tensor at high polarization remain unexplored. In this work, we develop a linearized model under mean-field approximation to investigate alignment tensor effects in highly polarized 3He, which originate from the metastable F = 3/2 manifold and are revealed through ME-induced relaxation and frequency shift. By means of free-induction-decay measurements, a pronounced dependence on nuclear polarization is experimentally observed in the response of the ground-state-metastable hybrid 3He ensembles to the external magnetic field. Furthermore, after obtaining the characteristics of tensor-induced phenomena, we demonstrate good agreement between the experiment and the theory. This work advances the understanding of nuclear spin dynamics in highly polarized 3He using MEOP. It further provides applications in systematic error correction of high-accuracy magnetometry, as well as in optimal protocol for the generation of nuclear spin-squeezed states.
Highly polarized 3He ensembles prepared by metastability-exchange optical pumping (MEOP) have been widely used in precision measurements and fundamental physics. Metastability-exchange (ME) collisions, serving as the basis of MEOP, are traditionally described in terms of atomic orientation, while the significant contributions of metastable alignment tensor at high polarization remain unexplored. In this work, we develop a linearized model under mean-field approximation to investigate alignment tensor effects in highly polarized 3He , which originate from the metastable F = 3/2 manifold and are revealed through ME-induced relaxation and frequency shift. By means of free-induction-decay (FID) measurements, a pronounced dependence on nuclear polarization is experimentally observed in the response of the ground-state-metastable hybrid 3He ensembles to the external magnetic field. Furthermore, after obtaining the characteristics of tensor-induced phenomena, we demonstrate good agreement between the experiment and the theory. This work advances the understanding of nuclear spin dynamics in highly polarized 3He using MEOP. It further provides applications in systematic error correction of high-accuracy magnetometry, as well as in optimal protocol for the generation of nuclear spin-squeezed states.
Abstract Highly polarized 3 He ensembles prepared by metastability-exchange optical pumping (MEOP) have been widely used in precision measurements and fundamental physics. Metastability-exchange (ME) collisions, serving as the basis of MEOP, are traditionally described in terms of atomic orientation, while the significant contributions of metastable alignment tensor at high polarization remain unexplored. In this work, we develop a linearized model under mean-field approximation to investigate alignment tensor effects in highly polarized 3 He , which originate from the metastable F = 3 / 2 manifold and are revealed through ME-induced relaxation and frequency shift. By means of free-induction-decay measurements, a pronounced dependence on nuclear polarization is experimentally observed in the response of the ground-state-metastable hybrid 3 He ensembles to the external magnetic field. Furthermore, after obtaining the characteristics of tensor-induced phenomena, we demonstrate good agreement between the experiment and the theory. This work advances the understanding of nuclear spin dynamics in highly polarized 3 He using MEOP. It further provides applications in systematic error correction of high-accuracy magnetometry, as well as in optimal protocol for the generation of nuclear spin-squeezed states.
We study the dressed states of 3He atoms and experimentally observe the Mollow triplet (MT) induced with an ultra-low-frequency (ULF) oscillating magnetic field as low as 4 Hz. The ULF MT signatures from the ground states of 3He atoms are transferred to the metastable states by metastability-exchange collisions (MECs) and measured optically, which demonstrates 2 s coherence time in the dressed ground states. The result shows the possibility of ULF magnetic field amplitude measurement and a new scheme for optical frequency modulation.
Helium-3 nuclear spins form an exceptionally stable quantum system with extremely long coherence time, offering exciting opportunities for quantum technologies. In particular, nuclear spin-squeezed states promise enhanced precision for sensing tasks and tests of new physics. A central challenge for all these applications is the realization of a controllable light-nuclear spin interface. Here we experimentally demonstrate such an interface by exploiting metastability-exchange collisions in a low-pressure helium-3 gas cell at room temperature. A radio-frequency discharge produces a small population of metastable atoms that both enables efficient optical pumping and mediates an effective Faraday interaction between the collective nuclear spin and an optical probe. We quantitatively characterize the strength of this interaction as a function of the nuclear polarization, applied magnetic field, and probe-beam parameters. Moreover, we show that using a multi-pass cell enhances this interaction by effectively increasing the optical depth. Extrapolating to a tenfold increase of the probe power used in the present experiment, we project a measurement-induced squeezing rate of 0.52 s−1^{-1}−1. Our results provide a practical pathway for optical access to helium-3 nuclear spins and open prospects for generating long-lived, macroscopic nuclear spin-squeezed states for quantum metrology.
Advances in metastability exchange optical pumping (MEOP) at high laser powers, but also at high gas pressures and high magnetic field strengths, has provided strong motivation for revisiting the understanding of the limitations of this powerful technique. A comprehensive model has been developed for improved description of the combined effects of OP, ME, and relaxation, and of detailed MEOP features observed over the broad range of operating conditions. A brief description is provided, with illustrative comparisons of computed and experimental results. This improved tool is used to explain the excellent photon efficiency of OP obtained at all field strengths. It is combined with an angular momentum budget approach to quantitatively investigate the newly discovered strong OP-enhanced polarisation losses that currently limits MEOP performance.