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Physical Review A

Magnetic-resonance linewidth of alkali-metal vapor in the unresolved Zeeman-resonance regime

Feng Tang, Nan Zhao

Published Jan 6, 2025• 6 citations
Publisher

Abstract

The study of magnetic-resonance linewidth is crucial in magnetic-resonance physics and its applications. Previous studies focused on the linewidth of alkali metal atoms within the spin-exchange relaxation-free regime near zero magnetic field and in strong magnetic fields where Zeeman resonances are well resolved due to the quadratic Zeeman effect. However, the linewidth in the unresolved-Zeeman-resonance regime, which is prevalent in various magnetometer and comagnetometer applications, is not well understood. To address this, we developed a theoretical framework based on the master equation for alkali metal atoms and solved it under the rotating-wave approximation and weak-driving conditions. Our numerical calculations and analytical expressions reveal that the light-narrowing effect occurs only when the ratio of the spin-exchange rate to the spin destruction rate exceeds a critical value. Additionally, we show that the linewidth in the unresolved Zeeman-resonance regime is significantly influenced by the mutual coupling of quantum coherence between different Zeeman sublevels. These findings provide a theoretical tool for understanding spin relaxation in alkali-metal atoms and optimizing the performance of atomic magnetometers and comagnetometers operating in this regime.

DOI
10.1103/physreva.111.013103

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The study of magnetic-resonance linewidth is crucial in magnetic-resonance physics and its applications. Previous studies focused on the linewidth of alkali metal atoms within the spin-exchange relaxation-free regime near zero magnetic field and in strong magnetic fields where Zeeman resonances are well resolved due to the quadratic Zeeman effect. However, the linewidth in the unresolved-Zeeman-resonance regime, which is prevalent in various magnetometer and comagnetometer applications, is not well understood. To address this, we developed a theoretical framework based on the master equation for alkali metal atoms and solved it under the rotating-wave approximation and weak-driving conditions. Our numerical calculations and analytical expressions reveal that the light-narrowing effect occurs only when the ratio of the spin-exchange rate to the spin destruction rate exceeds a critical value. Additionally, we show that the linewidth in the unresolved Zeeman-resonance regime is significantly influenced by the mutual coupling of quantum coherence between different Zeeman sublevels. These findings provide a theoretical tool for understanding spin relaxation in alkali-metal atoms and optimizing the performance of atomic magnetometers and comagnetometers operating in this regime.
Spin-exchange collisions often play a dominant role in the broadening of Zeeman resonances in an alkali-metal vapor. Contrary to intuitive expectations, at high alkali-metal densities this broadening can be completely eliminated by operating in a low magnetic field, allowing construction of ultrasensitive atomic magnetometers. We describe a detailed study of the Zeeman resonance frequencies and linewidths as a function of the magnetic field, alkali-metal density, and the degree of spin polarization of the atoms. Due to the nonlinear nature of the density matrix equations describing the spin-exchange collisions both the gyromagnetic ratio and the linewidth change as a function of the polarization. The results of experimental measurements are in excellent agreement with analytical and numerical solutions of the density matrix equations.
Nuclear magnetic resonance gyroscopes (NMRGs) employ noble-gas nuclear spins as inertial sensors and alkali-metal atoms as in-situ magnetometers. Heavy noble gases, particularly xenon, are widely used due to their large nuclear spin and strong spin-exchange coupling with alkali-metal atoms. However, their presence introduces additional collisional mechanisms that affect the alkali-metal magnetic resonance linewidth, thereby influencing magnetometer sensitivity and overall gyro performance. In this work, we develop a theoretical framework based on the density matrix formalism and master equation approach to quantitatively study how xenon-induced two-body and three-body interactions modify the linewidth of alkali-metal atoms under realistic NMRG conditions. Our analysis reveals that Xe atoms primarily broaden the linewidth via binary spindestruction collisions and van der Waals (vdW)-mediated F-damping processes, while the effect of Xe nuclear polarization is negligible at the ~1% level. We further demonstrate that nitrogen buffer gas plays a dual role: it directly contributes to alkali-metal spin relaxation through binary collisions and indirectly modulates vdW collision rates by altering molecular lifetimes. The interplay between these processes leads to an optimal nitrogen density that minimizes the linewidth. Additionally, we identify a temperature threshold above which light-narrowing emerges, with this threshold increasing alongside Xe density. These findings provide theoretical insight for optimizing spin relaxation control in alkali-metal magnetometers and improving NMRG performance.
Alkali-metal-vapor magnetometers, using coherent precession of polarized atomic spins for magnetic-field measurement, have become one of the most sensitive magnetic-field detectors. Their application areas range from practical uses such as NMR signal detection to fundamental physics research such as searches for permanent electric dipole moments. One of the main noise sources of atomic magnetometers comes from the light shift that depends on the frequency of the pump laser. In this work, we theoretically study the light shift, taking into account the relaxation due to the optical pumping and the collision between alkali-metal atoms and between alkali-metal atoms and the buffer gas. Starting from a full master equation containing both the ground and excited states, we adiabatically eliminate the excited states and obtain an effective master equation in the ground-state subspace that shows an intuitive picture and dramatically accelerates the numerical simulation. Solving this effective master equation, we find that in the light-narrowing regime, where the linewidth is reduced while the coherent precession signal is enhanced, the frequency dependence of the light shift is largely reduced, which agrees with experimental observations in cesium magnetometers. Since this effective master equation is general and is easily solved, it can be applied to an extensive parameter regime, and also to study other physical problems in alkali-metal-vapor magnetometers, such as heading errors.
Abstract Nuclear magnetic resonance gyroscopes (NMRGs) employ noble-gas nuclear spins as inertial sensors and alkali-metal atoms as in-situ magnetometers. Heavy noble gases, particularly xenon, are widely used due to their long nuclear spin relaxation time and strong spin-exchange coupling with alkali-metal atoms. However, their presence introduces additional collisional mechanisms that affect the alkali-metal magnetic resonance linewidth, thereby influencing magnetometer sensitivity and overall gyro performance. In this work, we employ a theoretical framework based on the density matrix formalism and master equation approach to quantitatively study how xenon-induced two-body and three-body interactions modify the linewidth of alkali-metal atoms under realistic NMRG conditions. Our analysis reveals that Xe atoms primarily broaden the linewidth via binary spin-destruction collisions and van der Waals (vdW)-mediated F-damping processes, while the effect of Xe nuclear polarization is negligible at the ∼ 1 % level. We further demonstrate that nitrogen buffer gas plays a dual role: it directly contributes to alkali-metal spin relaxation through binary collisions and indirectly modulates vdW collision rates by altering molecular lifetimes. The interplay between these processes leads to an optimal nitrogen density that minimizes the linewidth. Additionally, we identify a temperature threshold above which light-narrowing emerges, with this threshold increasing alongside Xe density. These findings provide theoretical insight for optimizing spin relaxation control in alkali-metal magnetometers and improving NMRG performance.
Alkali metal-noble gas comagnetometers operated in the regime of spin-exchange relaxation-free (SERF) have been widely used in fundamental physics tests and rotation sensing as gyroscope. Spin-exchange relaxation is an important systematic bias of the comagnetometer, which could limit sensitivity significantly. However, the suppression effect of the spin-exchange relaxation has not been examined quantitatively so far. Herein, we systematically investigate the relaxation of the alkali metal atoms and find that the spin-exchange relaxation is not completely eliminated under the normal operating condition of the K-Rb-21Ne comagnetometer. In addition to the optical pumping rate, the spin-exchange relaxation still plays a dominant role in the broadening of electron Zeeman resonances due to the large electron magnetic field. This is the first demonstration that the alkali metal atoms are operated in the near-SERF regime in the alkali metal-noble gas comagnetometer with a large election magnetic field, which will shed light on the way to reduce the relaxation of the alkali metal atoms and enhance the sensitivity of the comagnetometer.
Abstract We present a theoretical study of the optical-radio-frequency (rf) double resonance on hyperfine ground states of alkali-metal atoms in the geophysical magnetic-field range, in which resonance circularly polarized laser light is used in the optical pumping and detection processes. The analytical expressions of the rf resonance signals corresponding to two ground states are obtained based on atomic multipole moments, where the alignment effect is considered and that is responsible for the resonance shape and linewidth especially when the optical power is relatively strong. In addition, we also obtain the analytical expressions of the linewidths of two separated resonance peaks and one presenting the competition process of the optical pumping, rf field and spin-exchange collision. Two different types of light narrowing phenomena are investigated by comparing the longitudinal relaxation rates of atomic multipole moments for two ground states. Applied to rubidium and cesium atoms, we show a particularly close agreement of our analytical results with more elaborate calculations using density-matrix theory. Our theoretical model is relevant for optimizing the sensitivity of magnetometers.