Effect of concentration gradient on the first-, second- and third-order polarizabilities

The effect of concentration gradients on the polarizabilities of chemical systems of mixed composition is examined theoretically. It is found that the first-, second- and third-order polarizabilities all exhibit linear dependences on concentration gradient but nonlinear dependences on dielectric gradient. Furthermore, sample calculations imply that under selected conditions, concentration and/or dielectric gradient effects should be readily observable experimentally and indeed, under some conditions could dominate the experimental response. Examples of systems that might display the predicted effects include compositionally graded polymer, semiconductor, composite films, as well as thermally graded liquid mixtures and colloidal suspensions.