Abstract

The techniques of group-theoretical statistical mechanics (GTSM) are applied to various aspects of the interaction of electromagnetic radiation with molecular ensembles. Six nonlinear optical effects are examined in terms of the three principles of GTSM, using a classical series expansion of the induced electric dipole moment in terms of the electric and magnetic components of the electromagnetic field. Classical-quantum equivalence relations are derived at each stage. Symmetry arguments are applied to the chiral properties of some of the new nonlinear optical effects using the third principle of GTSM. A careful distinction is made between natural and magnetic optical activity, and our analysis attempts to resolve some recent disagreements in the literature.

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