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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Resonant nonlinear magneto-optical effects of atoms in vapors, beams, and quantum crystals

Antoine Weis, G. Bison, Daniel Nettels, Ulrich Rasbach, R. Müller-Siebert

Published May 30, 2002• 2 citations
Publisher

Abstract

We describe the basic principles underlying resonant nonlinear magneto-optical spectroscopy of alkali atoms and show how the technique can be applied for high resolution investigations of weak and strongly suppressed processes in spin coherent atomic ensembles. We illustrate this by a detailed discussion of four distinct applications, viz. the detection of small biomagnetic fields, the space and time resolved tomographic study of gas phase diffusion, the measurement of linear and quadratic Stark effects in atomic ground states and the study of (quantum) crystal field effects on solid helium-isolated atomic defect structures.

DOI
10.1117/12.468930

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We describe the basic principles underlying resonant nonlinear magneto-optical spectroscopy of alkali atoms and show how the technique can be applied for high resolution investigations of weak and strongly suppressed processes in spin coherent atomic ensembles. We illustrate this by a detailed discussion of four distinct applications, viz. the detection of small biomagnetic fields, the space and time resolved tomographic study of gas phase diffusion, the measurement of linear and quadratic Stark effects in atomic ground states and the study of (quantum) crystal field effects on solid helium-isolated atomic defect structures.
The aim of this book is to present new results in rapidly developing fields of nonlinear optics such as atomic coherence, magneto-optics of atomic media, Doppler-free spectroscopy, time-domain spectroscopy of dense atomic vapors, frequency comb spectroscopy and atom-surface interactions. The discovery of such coherent effects as coherent population trapping (CPT), electromagnetically induced transparency (EIT) and electromagnetically induced absorption (EIA) opened a new avenue for development in many fields of nonlinear optics. Investigations during the last decade have shown many related new results and approaches in nonlinear optics. These include nonlinear magneto-optical processes (NMOP) in the context of high precision magnetometry, quantum information storage and processing, magnetic resonance imaging and magnetic particle detection; the use of ultra-thin (nanometric length) atomic vapor cells in magneto-optical experiments, which show new peculiarities of both coherent effects and NMOP; the use of frequency and amplitude modulated laser beams for NMOP studies in atomic vapors with the aim of extending the range of ultra-precise magnetometers to stronger, particularly geomagnetic fields; application of the counter-propagating beam technique to reveal the Doppler free nonlinear Faraday rotation signals, as a spectroscopic tool and for applications; enhanced nonlinearity due to atomic coherence in multi-state systems; experimental study of EIT in solids; the use of the phase stabilized frequency domain combs of femtosecond laser pulses for velocity selective optical pumping of atomic hyperfine levels, as a direct frequency comb spectroscopy; time-domain nonlinear spectroscopy of dense atomic vapors; atom-surface interactions and laser induced adsorption and desorption of alkali atoms on the surface of solid materials for nanotechnology applications
Laser-atom interactions create atomic coherence and large nonlinear atomic polarization.\nWe investigate resonant laser-atom interactions to generate large nonlinearities\nand control them using magneto-optical fields. Coherent control of high-order\nsusceptibilities and magneto-optical rotation are demonstrated. Experiments are supported\nby theoretical studies that effectively describe the observed phenomena.\nIt is shown that a new coherent field, with polarization orthogonal to a weak\nsignal field, can be parametrically generated via an all-resonant four-wave-mixing\nprocess. This is demonstrated in a double-ladder system having two intermediate\nstates between a ground and an excited state. It is shown that the parametricgeneration\nprocess can be coherently controlled by coupling lasers and magnetic fields.\nIt is theoretically established that the underlying physics is a resonant three-photon\nprocess with a wide domain of control parameters.\nElectromagnetically induced transparency (EIT), where absorption of a weak\nprobe is suppressed via quantum interference, is demonstrated in a usual three-level\nladder system. It is observed that in contrast with EIT in a usual ladder system,\naddition of a second channel helps to suppress the absorption of two weak probe\nfields in the double-ladder system. The resulting enhancement of transmission in two\ndifferent channels is due to gain caused by three-photon processes.\nCoherent control is strongly limited by coherence lifetime, which is the inverse of\nthe dephasing rate. A lambda-system, having two ground states coupled to a common\nexcited state by lasers, can generate a new eigen (dark)-state that is transparent to incoming fields and hence suppresses fluorescence. However, ground-state dephasing\nperturbs the dark state. A new method for measuring the ground-state dephasing\nrate from fluorescence signals is proposed and a proof-of-principle experiment demonstrated.\nWhile two laser fields in a lambda-system are resonant with their respective\ntransitions, the atomic polarizations are very sensitive to an applied magnetic field.\nThis effect can be used for optical magnetometry. The degree of sensitivity of the\nmagnetometer is determined by two competing parameters–atomic density and laser\nintensity. It is shown experimentally that the optimal sensitivity reaches saturation,\nwhich is contrary to the idea that sensitivity increases indefinitely with an increase\nin the above parameters.
The creation and detection of atomic polarization is examined theoretically through the study of basic optical-pumping mechanisms and absorption and fluorescence measurements and the dependence of these processes on the size of ground- and excited-state hyperfine splittings is determined. The consequences of this dependence are studied in more detail for the case of nonlinear magneto-optical rotation in the Faraday geometry (an effect requiring the creation and detection of rank-two polarization in the ground state) with alkali-metal atoms. Analytic formulas for the optical rotation signal under various experimental conditions are presented.
Nonlinear magneto-optical resonances occurring for near-zero magnetic field are studied in Rb vapor using light-noise spectroscopy. With a balanced detection polarimeter, we observe high contrast variations of the noise power (at fixed analysis frequency) carried by diode laser light resonant with the $5{\mathrm{S}}_{1∕2}\phantom{\rule{0.2em}{0ex}}(F=2)\ensuremath{\rightarrow}5{\mathrm{P}}_{1∕2}\phantom{\rule{0.2em}{0ex}}(F=1)$ transition 87Rb^{87}\mathrm{Rb}87Rb and transmitted through a rubidium vapor cell as a function of magnetic field BBB. A symmetric resonance doublet of anticorrelated noise is observed for orthogonal polarizations around B=0B=0B=0 as a manifestation of ground-state coherence. We also observe sideband noise resonances when the magnetic field produces an atomic Larmor precession at a frequency corresponding to one-half of the analysis frequency. The resonances on the light fluctuations are the consequence of phase to amplitude noise conversion owing to nonlinear coherence effects in the response of the atomic medium to the fluctuating field. A theoretical model (derived from linearized Bloch equations) is presented that reproduces the main qualitative features of the experimental signals under simple assumptions.
Nonlinear magneto-optical effects, originated from atomic coherence, are studied both theoretically and experimentally in thermal Rb vapor. The analytical description of the fundamental properties of coherent media are based on the simplified three- and four-level systems, and then verified using numerical simulations and experimental measurements. In particular, we analyze the modification of the long-lived atomic coherence due to various physical effects, such as reabsorption of \nspontaneous radiation, collisions with a buffer gas atoms, etc. We also discuss the importance of the high-order nonlinearities in the description of the polarization rotation for the elliptically polarized light. The effect of self-rotation of the elliptical polarization is also analyzed. \nPractical applications of nonlinear magneto-optical effects are considered in precision metrology and magnetometery, and for the generation of non-classical states of electromagnetic field.
Results of a fairly straightforward experiment on resonant magneto-optical rotation by rubidium-87 atoms revealed strong time-dependence of the polarization plane of light emerging from atomic vapors following a sudden irradiation with a laser beam. The rotation of the plane appears as a not direct consequence of the influence of the magnetic field on atoms. Reported measurements conducted using a vapor cell without any buffer gas or an anti-relaxation wall coating show that transmitted light has initially the same (linear) polarization as the incident one. Rotation of the polarization plane caused by an axial magnetic field develops in time scales similar to the pace of establishing the optical pumping/relaxation equilibrium in the atomic ensemble. The traditional passive Faraday rotation picture providing working description for the resonant magneto-optical effects in steady-state conditions does not explain the observed sequence of evolution of the polarization. The picture has to be augmented with analysis of time dependence in the spatial distribution of relevant quantum states within the atomic ensemble as well as longitudinal and transversal intensity profiles of the light beam. Isolation of external effects caused by the optical pumping and relaxation processes from consequences of internal atomic coherences should uncover more details of mechanisms of the latter in the presence of magnetic field. Plentitude of data available from time-dependent polarization measurements provides strong incentives for further development and tests of comprehensive models of coherent interactions of atomic ensembles with radiation and possibly a base for additional advance in understanding and applications of these phenomena.