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Physical Review A

Light narrowing of magnetic resonance lines in dense, optically pumped alkali-metal vapor

Natarajan D. Bhaskar, James C. Camparo, W. Happer, Animesh Sharma

Published Jun 1, 1981• 53 citations
Publisher

Abstract

A new and unusual phenomenon which we call light narrowing is reported and discussed in this paper. We discovered this effect in dense, spin-polarized cesium vapor optically pumped with a cw blue dye laser beam tuned to the second resonance ${D}_{1}$ line (4593 \AA{}). We observe a significant narrowing of the radio-frequency power-broadened magnetic resonance lines (linewidths narrow by as much as a factor of 2.5) when the intensity of the circularly polarized incident dye laser beam is increased by either focusing the beam or by the removal of attenuating filters from the focused beam. The magnetic resonance linewidths in spin-polarized cesium vapor were measured over a wide range of cesium number densities (5\ifmmode\times\else\texttimes\fi{}${10}^{12}$ ${\mathrm{cm}}^{\ensuremath{-}3}$ \ensuremath{\le}[Cs]\ensuremath{\le}1\ifmmode\times\else\texttimes\fi{}${10}^{16}$ ${\mathrm{cm}}^{\ensuremath{-}3}$). This corresponds to cesium spinexchange rates of 4.5\ifmmode\times\else\texttimes\fi{}${10}^{3}$ to 9\ifmmode\times\else\texttimes\fi{}${10}^{6}$ ${\mathrm{sec}}^{\ensuremath{-}1}$. For low cesium number densities (5\ifmmode\times\else\texttimes\fi{}${10}^{12}$ [Cs]3\ifmmode\times\else\texttimes\fi{}${10}^{14}$ ${\mathrm{cm}}^{\ensuremath{-}3}$) the light-narrowing effect is large (a factor of 2.5) and independent of [Cs]. In the region of 3\ifmmode\times\else\texttimes\fi{}${10}^{14}$ to 1\ifmmode\times\else\texttimes\fi{}${10}^{15}$ ${\mathrm{cm}}^{\ensuremath{-}3}$ in number densities, the light-narrowing effect decreases with increasing [Cs]. At high cesium number densities ([Cs]> 1\ifmmode\times\else\texttimes\fi{}${10}^{15}$ ${\mathrm{cm}}^{\ensuremath{-}3}$) this light-narrowing effect almost completely disappears. In the limit of low-radio-frequency power the magnetic resonance linewidths for focused and unfocused dye laser beam are nearly the same. Experimental observations on this new effect are presented in detail. In the latter part of this paper a self-contained theoretical treatment of the light-narrowing effect is developed. Using Bloch equations in the presence of optical pumping, spin relaxation (diffusion, electron randomization), rapid spin exchange, and radio-frequency magnetic field, expressions for magnetic resonance line shapes are derived. In general, we find good agreement between our experimental results and the theory.

DOI
10.1103/physreva.23.3048

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A new and unusual phenomenon which we call light narrowing is reported and discussed in this paper. We discovered this effect in dense, spin-polarized cesium vapor optically pumped with a cw blue dye laser beam tuned to the second resonance D1{D}_{1}D1​ line (4593 \AA{}). We observe a significant narrowing of the radio-frequency power-broadened magnetic resonance lines (linewidths narrow by as much as a factor of 2.5) when the intensity of the circularly polarized incident dye laser beam is increased by either focusing the beam or by the removal of attenuating filters from the focused beam. The magnetic resonance linewidths in spin-polarized cesium vapor were measured over a wide range of cesium number densities (5\ifmmode\times\else\texttimes\fi{}1012{10}^{12}1012 cm\ensuremath−3{\mathrm{cm}}^{\ensuremath{-}3}cm\ensuremath−3 \ensuremath{\le}[Cs]\ensuremath{\le}1\ifmmode\times\else\texttimes\fi{}1016{10}^{16}1016 cm\ensuremath−3{\mathrm{cm}}^{\ensuremath{-}3}cm\ensuremath−3). This corresponds to cesium spinexchange rates of 4.5\ifmmode\times\else\texttimes\fi{}103{10}^{3}103 to 9\ifmmode\times\else\texttimes\fi{}106{10}^{6}106 sec\ensuremath−1{\mathrm{sec}}^{\ensuremath{-}1}sec\ensuremath−1. For low cesium number densities (5\ifmmode\times\else\texttimes\fi{}1012{10}^{12}1012 [Cs]3\ifmmode\times\else\texttimes\fi{}1014{10}^{14}1014 cm\ensuremath−3{\mathrm{cm}}^{\ensuremath{-}3}cm\ensuremath−3) the light-narrowing effect is large (a factor of 2.5) and independent of [Cs]. In the region of 3\ifmmode\times\else\texttimes\fi{}1014{10}^{14}1014 to 1\ifmmode\times\else\texttimes\fi{}1015{10}^{15}1015 cm\ensuremath−3{\mathrm{cm}}^{\ensuremath{-}3}cm\ensuremath−3 in number densities, the light-narrowing effect decreases with increasing [Cs]. At high cesium number densities ([Cs]> 1\ifmmode\times\else\texttimes\fi{}1015{10}^{15}1015 cm\ensuremath−3{\mathrm{cm}}^{\ensuremath{-}3}cm\ensuremath−3) this light-narrowing effect almost completely disappears. In the limit of low-radio-frequency power the magnetic resonance linewidths for focused and unfocused dye laser beam are nearly the same. Experimental observations on this new effect are presented in detail. In the latter part of this paper a self-contained theoretical treatment of the light-narrowing effect is developed. Using Bloch equations in the presence of optical pumping, spin relaxation (diffusion, electron randomization), rapid spin exchange, and radio-frequency magnetic field, expressions for magnetic resonance line shapes are derived. In general, we find good agreement between our experimental results and the theory.
The magnetic-resonance lines of alkali atoms are broadened considerably by the spin-exchange collisions for a radio-frequency magnetometer operating at high temperature. The resonance linewidths of cesium atoms are derived by solving the relaxation equations. When spin-exchange relaxation dominates, a light narrowing effect is predicted. For the cesium atomic radio-frequency magnetometer operates at high temperature, a remarkable narrowing of the cesium magnetic-resonance lines are observed by increasing the pump power. The Cs-Cs spin-exchange relaxation is partially suppressed by light narrowing. This study helps to expand the applications of radio-frequency magnetometers in the high-sensitivity radio-frequency magnetic-field detection.
Narrowing of magnetic-resonance lines in a dense optically pumped alkali-metal vapor (87{(}^{87}(87Rb) has been observed. This observation is shown to be a result of optical pumping with a monochromatic light source tuned such that the real part of the vapor polarizability, which is responsible for light shifts, is essentially zero. A model based on the Bloch equations is used to describe the observed narrowing effect, and results of numerical calculations based on this model are presented. The results agree qualitatively with observations, and show correctly the disappearance of the effect at low light levels. This narrowing effect is of importance to the development of precision frequency standards and magnetometers utilizing monochromatic light sources (such as semiconductor lasers).
We report on some unusual magnetic-resonance phenomena of optically pumped Rb vapor in high-pressure gas cells. When Rb-Rb spin exchange is the fastest spin-relaxation rate, we observe a considerable narrowing of the magnetic-resonance linewidths with increasing pump-laser power. The experimentally measured Rb magnetic-resonance linewidths are in excellent agreement with a theoretical model, which includes the processes of Rb-He and Rb-Xe spin destruction, Rb-Rb spin exchange, and Rb optical pumping.
We observe very narrow (\ensuremath{\sim}200 Hz) magnetic resonance lines in alkali vapors with atomic densities much greater than usual and with cell dimensions much smaller than usual. The Zeeman resonance frequency is shifted downward by a large factor, but the spin-exchange broadening vanishes in the high-density limit. This new regime affords important new possibilities for investigating basic interactions in dense alkali vapors, and it also opens the way to miniaturized optically pumped devices.
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.
The ground-state Hanle effect (GSHE) in alkali-metal atomic vapor using a single circularly polarized light wave underlies one of the most reliable and simple techniques of modern atomic magnetometry. This effect causes a narrow (subnatural-width) resonance in the light wave intensity passing through the vapor cell. The GSHE-based sensors typically operate in the so-called spin-exchange relaxation-free (SERF) regime to reduce the resonance linewidth. However, this regime requires a relatively high temperature of vapors (approximately equal to $150{\phantom{\rule{0.16em}{0ex}}}^{\ensuremath{\circ}}\mathrm{C}$), leading to high heat release and power consumption of the sensor head. In addition, without applying special measures, the SERF regime significantly limits the dynamic range of measurements. Here we study a pump-probe scheme involving a single elliptically polarized light wave and a polarimetric detection technique. The wave is in resonance with two adjacent optical transitions in the cesium D1{D}_{1}D1​ line ($\ensuremath{\lambda}\phantom{\rule{0.16em}{0ex}}\ensuremath{\approx}\phantom{\rule{0.16em}{0ex}}894.5$ nm) due to their overlap in the presence of a buffer gas (130 Torr neon). Using a small ($V\ensuremath{\approx}0.1\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{3}$) glass vapor cell, we demonstrate the possibility to observe subnatural-width resonances with a high contrast-to-width ratio (up to 45%/mG) in low-temperature ($60{\phantom{\rule{0.16em}{0ex}}}^{\ensuremath{\circ}}\mathrm{C}$) operation due to strong light-induced circular dichroism in the medium. Based on the $\mathrm{\ensuremath{\Lambda}}$ scheme of atomic energy levels, we obtain explicit analytical expressions for the shape of the resonance line. The model reveals a linewidth narrowing effect due to openness of the level scheme. The observed bright features are unusual for magneto-optical atomic spectroscopy as openness is commonly considered to be an undesirable effect that degrades resonance characteristics. Measuring the noise voltage, we estimate the sensitivity of the magnetic-field measurements to be 1.8 pT/Hz\mathrm{pT}/\sqrt{\mathrm{Hz}}pT/Hz​ with a sensitivity of 60 fT/Hz\mathrm{fT}/\sqrt{\mathrm{Hz}}fT/Hz​ in the photon-shot-noise limit. In general, the results contribute to the theory of GSHE resonances and also can be applied to development of a low-temperature high-sensitivity miniaturized magnetic-field sensor with an extended dynamic range.