Abstract

A molecular theory of circular and axial birefringence and dichroism induced by circularly polarized, linearly polarized and unpolarized pump light in isotropic systems of chiral molecules is presented. General analytical expressions for molecular contributions arising from electric dipole, magnetic dipole and electric quadrupole interactions with radiation are given in terms of linear and nonlinear polarizabilities and some specific cases are discussed. It is shown that in general the contributions due to electric quadrupole and magnetic dipole interactions of molecules with probe light to birefringence and dichroism differ from those brought by the same kind interactions with a pump light beam. To obtain information about the nonlinear optical properties of chiral molecules measurements of axial birefringence may present an advantage over circular birefringence experiments.

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