Observation of a Microscopic Cascaded Contribution to the Fifth-Order Nonlinear Susceptibility

Typically, low-order nonlinearities are much stronger than high-order nonlinearities. In this Letter, we demonstrate a procedure by which strong high-order nonlinearities can be synthesized out of low-order nonlinearities. Our procedure involves the use of the previously largely overlooked process of microscopic cascading, which results from local-field effects. We have performed an experiment that allows us to distinguish the influence of microscopic cascading from the more-well-known process of macroscopic cascading, and we find conditions under which microscopic cascading can be the dominant effect. The ability to create a large high-order nonlinear response could prove useful for applications in quantum-information science that require the detection of the simultaneous presence of N entangled photons.