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The molecular origins of optical nonlinearity: beyond charge-transfer effects

A remarkably simple methodology is described for quantitatively relating virtually all nonlinear optical phenomena directly back to intuitive molecular processes, including absorption, Raman polarizability, and two-photon absorption. The dramatic reduction in complexity resulting from this approach provides new routes for predicting and optimizing the molecular nonlinearities in emerging materials and spectroscopic applications without sacrificing mathematical rigor. In combination with experimental measurements, this general approach is shown to be particularly useful in interpreting the unique polarization-dependent nonlinear optical properties of chiral materials and surfaces.