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The nonlinear optical response of a system of molecules often containscontributions whereby the products of lower-order processes in two separatemolecules give signals that appear on top of a genuine direct higher-orderprocess with a single molecule. These many-body contributions are known ascascading and complicate the interpretation of multidimensional stimulatedRaman and other nonlinear signals. In a quantum electrodynamic (QED) treatment,these cascading processes arise from second-order expansion in the molecularcoupling to vacuum modes of the radiation field, i.e., single-photon exchangebetween molecules, which also gives rise to other collective effects. Wepredict the relative phase of the direct and cascading nonlinear signals andits dependence on the microscopic dynamics as well as the sample geometry. Thisphase may be used to identify experimental conditions for distinguishing thedirect and cascading signals by their phase. Higher-order cascading processesinvolving the exchange of several photons between more than two molecules arediscussed as well.

Discriminating Cascading Processes in Nonlinear Optics; A QED Analysis Based on Their Molecular and Geometric Origin