Nonlinear optical activity in chiral molecules: surface second harmonic generation and nonlinear circular dichroism

Nonlinear optical activity in chiral molecules is investigated. We first examine the importance of the nonlocality of the light–matter interaction in optical activity and extend this concept to second-order (surface second harmonic generation) and third-order (nonlinear circular dichroism) nonlinear optical phenomena. Microscopic models are also discussed. Various phenomena derived from these considerations are demonstrated experimentally with specially-synthesized chiral molecules. To cite this article: F. Hache et al., C. R. Physique 3 (2002) 429–437.