Abstract
Novel, high-sensitivity and high-resolution spectroscopic methods can provide site-specific nuclear information by exploiting nuclear magneto-optic properties. We present a first-principles electronic structure formulation of the recently proposed nuclear-spin-induced Cotton-Mouton effect in a strong external magnetic field (NSCM-B). In NSCM-B, ellipticity is induced in a linearly polarized light beam, which can be attributed to both the dependence of the symmetric dynamic polarizability on the external magnetic field and the nuclear magnetic moment, as well as the temperature-dependent partial alignment of the molecules due to the magnetic fields. Quantum-chemical calculations of NSCM-B were conducted for a series of molecular liquids. The overall order of magnitude of the induced ellipticities is predicted to be 10(-11) -10(-6) rad T(-1) M(-1) cm(-1) for fully spin-polarized nuclei. In particular, liquid-state heavy-atom systems should be promising for experiments in the Voigt setup.
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