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We show that a combination of linear absorption spectroscopy, hyper-Rayleighscattering, and a theoretical analysis using sum rules to reduce the size ofthe parameter space leads to a prediction of the two-photon absorptioncross-section of the dye AF455 that agrees with two-photon absorptionspectroscopy. Our procedure, which demands self-consistency between severalmeasurement techniques and does not use adjustable parameters, provides a meansfor determining transition moments between the dominant excited states basedstrictly on experimental characterization. This is made possible by our newapproach that uses sum rules and molecular symmetry to rigorously reduce thenumber of required physical quantities.

Experimental verification of a self-consistent theory of the first-, second-, and third-order (non)linear optical response