Higher polarization of organic molecules used in nonlinear optics: Influence of the Coulomb interaction

Matrix formulation of TDHF theory of HP is given, (2i+l)-rule for dynamic HP and compatibility of TDHF with finite field approach are proven. The definition of tensor invariants of HP is given for the general case. The above results are illustrated by calculations of HP in organic molecules with expressed nonlinear optical properties. A method of inclusion of intermolecular Madelung potential into HP calculation in crystals and crystal layers is described and illustrated by estimation of its influence on HP of some Langmuir-Blodgett films. Similar technique is developed for calculation of Lorentz factors in crystals and crystal layers, which have been used for transformation of molecular HP into higher susceptibilities of crystals and films.