Charge transfer complexes and hyperpolarizabilities

Abstract
We have measured the second order β and third order γ hyperpolarizabilities of the three charge transfer complexes pyridine+I2, pyridine+ICl, and 4‐aminopyridine+I2. Using Mulliken’s charge transfer theory we have been able to understand theoretically the large magnitude and absolute sign of these hyperpolarizabilities as well as their interesting and surprising dependence on the strength of the charge transfer interaction.