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

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

2011-04-11

arxiv.org/abs/1104.1844v2

Phys. Rev. A 84, 043406 (2011)

Physics

Optics

10 pages, 7 Figures, 1 table

Scientific paper

10.1103/PhysRevA.84.043406

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

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