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arXiv:2201.09775

Spin noise in birefringent and inhomogeneous media

V. O. Kozlov, Н. С. Кузнецов, Dmitry S. Smirnov, I. I. Ryzhov, G. G. Kozlov, Valerii S Zapasskii

Published Jan 24, 2022• 0 citations
arXivHTMLPDF

Abstract

It is known that linear birefringence of the medium essentially hinders measuring the Faraday effect. For this reason, optically anisotropic materials have never been considered as objects of the Faraday-rotation-based spin noise spectroscopy (SNS). We show, both theoretically and experimentally, that strong optical anisotropy that may badly suppress the regular Faraday rotation of the medium, practically does not affect the measurement of the spatially uncorrelated spin fluctuations. An important consequence of this result is that the Faraday-rotation noise should be also insensitive to spatially nonuniform birefringence, which makes the SNS applicable to a wide class of optically anisotropic and inhomogeneous materials. We also show that the birefringent media provide additional opportunity to measure spatial spin correlations. Results of the experimental measurements of the spin-noise spectra performed on 4$f$--4$f$ transitions of Nd$^{3+}$ ions in the CaWO$_4$ and LiYF$_4$ crystals well agree with the theory.

DOI
10.48550/arxiv.2201.09775

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It is known that linear birefringence of the medium essentially hinders measuring the Faraday effect. For this reason, optically anisotropic materials have never been considered as objects of the Faraday-rotation-based spin noise spectroscopy (SNS). We show, both theoretically and experimentally, that strong optical anisotropy that may badly suppress the regular Faraday rotation of the medium, practically does not affect the measurement of the spatially uncorrelated spin fluctuations. An important consequence of this result is that the Faraday-rotation noise should be also insensitive to spatially nonuniform birefringence, which makes the SNS applicable to a wide class of optically anisotropic and inhomogeneous materials. We also show that the birefringent media provide additional opportunity to measure spatial spin correlations. Results of the experimental measurements of the spin-noise spectra performed on 4fff--4fff transitions of Nd3+^{3+}3+ ions in the CaWO4_44​ and LiYF4_44​ crystals well agree with the theory.
It is known that linear birefringence of the medium essentially hinders measuring the Faraday effect. For this reason, optically anisotropic materials have never been considered as objects of the Faraday-rotation-based spin noise spectroscopy. We show, both theoretically and experimentally, that strong optical anisotropy that may badly suppress the regular Faraday rotation of the medium, practically does not affect the measurement of the spatially uncorrelated spin fluctuations. We also show that the birefringent media provide additional opportunity to measure spatial spin correlations. Results of the experimental measurements of the spin-noise spectra performed on Nd^{3+} ions in the uniaxial crystal matrices well agree with the theory.
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Spin noise spectroscopy (SNS) is a new method for studying magnetic resonance and spin dynamics that has gained, in the last several years, a considerable popularity. The method is based on measuring magnetization noise of a paramagnet using the Faraday rotation technique. In strong contrast with methods of nonlinear optics, the spectroscopy of spin noise is considered to be essentially nonperturbative. At the same time, presently, it became clear that the SNS, as an optical technique, demonstrates abilities lying far beyond the bounds of conventional linear optics. Specifically, the SNS allows one to penetrate inside an inhomogeneously broadened absorption band and to determine its homogeneous width, to realize a sort of pump-probe spectroscopy without any optical nonlinearity, to probe a bulk inhomogeneous medium by focal point of a probe beam, etc. This may seem especially puzzling when taken into account that SNS can be considered just as a version of Raman spectroscopy, which is known to be deprived of such abilities. Understanding of these paradoxical features of SNS technique is required for the present-day applications of SNS and its further development. In this paper, we present a general analysis of this apparent inconsistency from the viewpoint of distinction between spectroscopy of the light intensity and of the light field and provide its resolution.
The effect of magnetic resonance in the Faraday-rotation noise, demonstrated for the first time on an atom system more than 40 years ago, laid the foundations of a new research direction, the spin noise spectroscopy, that has been developing extensively in the last 20 years. Currently, the most popular research objects are atom and semiconductor paramagnetic materials, while research subjects are the magnetic resonance spectroscopy, the spin dynamics, the optical spectroscopy, the spectroscopy of light polarization noises. The rapid development of this new research direction laying at the interface between optics and radio spectroscopy continuously extends the field of its applicability and opens new opportunities to use it in the experimental physics. In this article we present a few episodes that are important stages in the spin noise spectroscopy development in the last years. The article was prepared as a report on the XV Russian Conference on the Physics of Semiconductors. Keywords: spin noise spectroscopy, magnetic resonance, optical anisotropy, inhomogeneous broadening.
The mechanism of formation of the polarimetric signal observed in the spin noise spectroscopy (SNS) is analyzed from the viewpoint of the light scattering theory. A rigorous calculation of the polarimetric signal (Faraday rotation or ellipticity) recorded in the SNS is presented in the approximation of single scattering. We show that it is most correctly to consider this noise as a result of scattering of the probe light beam by fluctuating susceptibility of the medium. Fluctuations of the gyrotropic (antisymmetric) part of the susceptibility tensor lead to appearance of the typical for the SNS Faraday rotation noise at the Larmor frequency. At the same time, fluctuations of linear anisotropy of the medium (symmetric part of the susceptibility tensor) give rise to the ellipticity noise of the probe beam spectrally localized at the double Larmor frequency. The results of the theoretical analysis well agree with the experimental data on the ellipticity noise in cesium vapor.
The spin-noise spectroscopy, being a nonperturbative linear optics tool, is still reputed to reveal a number of capabilities specific to nonlinear optics techniques. The effect of the Doppler broadening homogenization discovered in this work essentially widens these unique properties of spin-noise spectroscopy. We investigate spin noise of a classical system---cesium atoms vapor with admixture of buffer gas---by measuring the spin-induced Faraday rotation fluctuations in the region of D2D{}_{2}D2​ line. The line, under our experimental conditions, is strongly inhomogeneously broadened due to the Doppler effect. Despite that, optical spectrum of the spin-noise power has the shape typical for the homogeneously broadened line with a dip at the line center. This fact is in stark contrast with the results of previous studies of inhomogeneous quantum dot ensembles and Doppler broadened atomic systems. In addition, the two-color spin-noise measurements have shown, in a highly spectacular way, that fluctuations of the Faraday rotation within the line are either correlated or anticorrelated depending on whether the two wavelengths lie on the same side or on different sides of the resonance. The experimental data are interpreted in the frame of the developed theoretical model which takes into account both kinetics and spin dynamics of Cs atoms. It is shown that the unexpected behavior of the Faraday rotation noise spectra and effective homogenization of the optical transition in the spin-noise measurements are related to smallness of the momentum relaxation time of the atoms as compared with their spin-relaxation time. Our findings demonstrate abilities of spin-noise spectroscopy for studying dynamic properties of inhomogeneously broadened ensembles of randomly moving spins.