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Optical magnetization, Part I: Experiments on radiant optical magnetization in solids

Alexander A. Fisher, Elizabeth F. C. Dreyer, Ayan Chakrabarty, and Stephen C. Rand

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Abstract

Linearly-polarized magnetic dipole (MD) scattering as intense as Rayleigh scattering is reported in transparent garnet crystals and fused quartz through a magneto-electric interaction at the molecular level. Radiation patterns in quartz show the strongest optical magnetization relative to electric polarization ever reported. As shown in an accompanying paper, quantitative agreement is achieved with a strong-field, fully-quantized theory of magneto-electric (M-E) interactions in molecular media. The conclusion is reached that magnetic torque enables 2-photon resonance in an EH* process that excites molecular librations and accounts for the observed upper limit on magnetization. Second-order M-E dynamics can also account for unpolarized scattering from high-frequency librations previously ascribed to first-order collision-induced or third-order, all-electric processes.

© 2016 Optical Society of America

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Figures (5)
Fig. 1
Fig. 1 Schematic diagram of the experimental apparatus, showing both the forward beam used to monitor polarization changes due to cross-polarized four-wave mixing in sample transmission and the detection arm at 90 degrees to the incident beam used to observed ED and MD scattering. WC = wavefront controller, IC = Intensity Controller, IF = interference filter, Det = detector, Pol = polarization analyzer.

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Fig. 2
Fig. 2 (a). Measurements of unpolarized ED (open circles) and MD (filled circles) scattering intensity versus input intensity for the reference sample (CCl4) obtained at a repetition rate of 1 kHz. Solid curves are quadratic fits to the intensity dependence. Inset: corresponding data for polarized scattering components on the same intensity scale. (b) Measurements of sample transmission in GGG with polarization parallel (circles) and perpendicular (triangles) to that of the incident beam in the range of input intensities used for scattering experiments.

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Fig. 3
Fig. 3 (a) Polar plot of raw data on co-polarized (open circles) and cross-polarized (filled circles) radiation patterns in GGG at I=1.4× 10 7 W/cm2 obtained at a repetition rate of 1 kHz. Dashed circles anticipate fits to the unpolarized background signal intensities. Residuals from the best fit of a circle plus a squared cosine curve to the raw data are shown below the polar plot. (b) Comparative plots in crystalline GGG of unpolarized ED (open circles) and MD (filled circles) scattering. Solid curves are quadratic fits to the data. Inset: corresponding data for polarized scattering components on the same scale.

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Fig. 4
Fig. 4 Polar plots of the radiation patterns for polarized ED and MD scattering in fused quartz at an input intensity of I~2.2× 10 10 W/cm2 obtained at a repetition rate of 80 MHz. At this intensity, in this sample, the unpolarized component is negligible compared to the polarized component. Note that peak intensities in the two plots are equal. Residuals from the best fit of a squared cosine curve to the raw data are shown below the polar plot.

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Fig. 5
Fig. 5 An energy level diagram depicting the second-order magneto-electric dynamics driven by E and B fields of (i) equal frequency (solid arrows), and (ii) frequencies differing by rotational frequency ω φ (dashed arrow).

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