A fully quantized analysis is presented of induced magneto-electric rectification in individual diatomic molecules in the steady-state regime. Good agreement is obtained between this quantum theory and a classical model that includes the same key kinematic elements but predicts temporal dynamics as well. At the molecular level, an enhanced magneto-electric optical interaction driven by dual optical fields E and H is shown to give rise to a static electric dipole (ED) moment oriented along the propagation direction of linearly-polarized light in dielectric materials. This longitudinal Hall effect or "charge separation" interaction is quadratic with respect to the incident field strength and exhibits an induced moment that is limited by the ED transition moment of the molecular resonance. Overall, the two-photon dynamics can be described as first establishing an electric polarization and imparting orbital angular momentum on which the magnetic field exerts torque in the excited state of the molecule. Magnetic torque mediates an exchange of orbital and rotational angular momenta that de-excites the molecule and simultaneously enhances magneto-electric rectification. Material properties that affect magneto-electric response at the molecular level are identified.
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.
A fully quantized analysis is presented on the origin of induced magnetic dipole (MD) scattering in two-level diatomic molecules. The interaction is driven by dual optical fields, E and H*, and is universally allowed in dielectric optical materials, including centrosymmetric media. Leading terms of the interaction are shown to be quadratic and cubic with respect to the intensity, predicting an upper limit for the induced magnetic dipole scattering intensity (IMD∝m2) that is equal to the electric dipole scattering (IED∝p2). The optical dynamics proceed by first establishing an electric polarization in the system. Then the magnetic field exerts torque on the orbital angular momentum of the excited state, mediating an exchange of orbital and rotational angular momenta that enhances the magnetic moment. The magneto-electric interaction also accounts for second-order, unpolarized scattering from high-frequency librations previously ascribed to third-order, all-electric processes.
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