ABSTRACT
As reviewed recently [1], the calculation of the properties of individual molecules as found in an infinitely dilute gas has for long been of great interest to quantum chemists. This curiosity has been spurred in recent decades by the increasing importance of the communications industry in the world and the parallel need for materials having specific properties for electronic, optical and other devices. In particular, the nonlinear-optical quantities, defined at the microscopic level as hyperpolarizabilities and at the macroscopic level as nonlinear susceptibilities, have played a key role in determining the suitability of substances for practical use, for example, in electro-optical switching and frequency mixing.
