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arXiv:1912.12100 · Physical Review Research

Giant spin-noise gain enables magnetic resonance spectroscopy of impurity crystals

A. N. Kamenskii, A. Greilich, I. I. Ryzhov, G. G. Kozlov, M. Bayer, Valerii S Zapasskii

Published Jun 11, 2020• 16 citations
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Abstract

The authors show that optical transitions in solids could reveal a Faraday rotation noise, despite a weak Faraday rotation. Such noise gain can be observed in inhomogeneously broadened transitions with small homogeneous width. Using this effect, the authors use spin noise spectroscopy to detect magnetic resonance in rare-earth-activated dielectrics.

DOI
10.1103/physrevresearch.2.023317

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The authors show that optical transitions in solids could reveal a Faraday rotation noise, despite a weak Faraday rotation. Such noise gain can be observed in inhomogeneously broadened transitions with small homogeneous width. Using this effect, the authors use spin noise spectroscopy to detect magnetic resonance in rare-earth-activated dielectrics.
The spin-noise spectroscopy (SNS) method implies high efficiency of conversion of the spin-system magnetization to the Faraday rotation angle. Generally, this efficiency cannot be estimated using the characteristics of the regular magnetooptical activity of a paramagnet. However, it may be drastically enhanced in systems with strong inhomogeneous broadening of the optical transitions. This enhancement leads to the giant spin-noise gain effect and previously allowed one to apply the SNS to rare-earth activated crystals. We show that the nonlinear resonant Faraday effect can be used to measure the homogeneous width of the inhomogeneously broadened transition and, thus, to estimate the applicability of the SNS to this type of paramagnet. We present the theoretical description of the effect and perform measurements on intraconfigurational ($4f\text{\ensuremath{-}}4f$) transitions of the trivalent rare-earth ions of neodymium and ytterbium in fluorite-based crystals. The proposed experimental approach establishes new links between the effects of nonlinear optics and spin-noise characteristics of crystals with paramagnetic impurities and offers new methods of research in the physics of impurity crystals.
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.
Highly sensitive Faraday rotation spectroscopy is used to measure the fluctuating magnetization noise of noninteracting rubidium atoms under resonant and nonresonant optical probing conditions. The spin-noise frequency spectra, in conjunction with the probe light detuning with respect to the D2{D}_{2}D2​ transition, reveal clear signatures of coherent coupling of the participating electronic levels. The results are explained by extended Bloch equations, including homogeneous and inhomogeneous broadening mechanisms. Our measurements further indicate that spin noise originating from excited states is governed at high intensities by collective effects.
Spontaneous fluctuations of the magnetization of a spin system in thermodynamic equilibrium (spin noise) manifest themselves as noise in the Faraday rotation of probe light. We show that the correlation properties of this noise over the optical spectrum can provide clear information about the composition of the spin system that is largely inaccessible for conventional linear optics. Such optical spectroscopy of spin noise, e.g., allows us to clearly distinguish between optical transitions associated with different spin subsystems, to resolve optical transitions that are unresolvable in the usual optical spectra, to unambiguously distinguish between homogeneously and inhomogeneously broadened optical bands, and to evaluate the degree of inhomogeneous broadening. These new possibilities are illustrated by theoretical calculations and by experiments on paramagnets with different degrees of inhomogeneous broadening of optical transitions [atomic vapors of 41K and singly charged (In,Ga)As quantum dots].
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.
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.