A classical model of the upper bounds of the cascading contribution to the second hyperpolarizability

Abstract

We investigate whether microscopic cascading of second-order nonlinearities of two molecules in the side-by-side configuration can lead to a third-order molecular nonlinear-optical response that exceeds the fundamental limit. We find that for large values of the second hyperpolarizability, the side-by-side configuration has a cascading contribution that lowers the direct contribution. However, we do find that there is a cascading contribution to the second hyperpolarizability when there is no direct contribution. Thus, while cascading can never lead to a larger nonlinear-optical response than for a single molecule with the same number of electrons, it may provide design flexibility in making large third-order susceptibility materials when the molecular second hyperpolarizability vanishes

10 pages, 7 Figures, 1 table

References in corpus (6)

• Studies on optimizing potential energy functions for maximal intrinsic hyperpolarizability
• A new dipole-free sum-over-states expression for the second hyperpolarizability
• The Effects of Geometry on the Hyperpolarizability
• The critical role of the energy spectrum in determining the nonlinear-optical response of a quantum system
• Monte Carlo Studies of the Intrinsic Second Hyperpolarizability
• A quantum mechanical model of the upper bounds of the cascading contribution to the second hyperpolarizability

Cited by in corpus (6)

• Generalizing the correlated chromophore domain model of reversible photodegradation to include the effects of an applied electric field
• Charge delocalization and hyperpolarizability in ionic liquids
• A quantum mechanical model of the upper bounds of the cascading contribution to the second hyperpolarizability
• Lowest-order relativistic corrections to the fundamental limits of nonlinear-optical coefficients
• The Local Field Factor and Microscopic Cascading: A Self-Consistent Method Applied to Confined Systems of Molecules
• Modeling off-resonant nonlinear-optical cascading in mesoscopic thin films and guest-host molecular systems