High-order nonlinear phase shift caused by cascaded third-order processes

We show, for the first time to our knowledge, that the fundamental beam that participates in the process of third-harmonic generation experiences an additional high-order nonlinear phase shift. The magnitude of the shift is proportional to the square of the pump intensity and the length of the sample and depends on the deviation from the exact phase-matched condition. This phase shift arises from cascaded third-order processes. Its value can exceed the value of the phase shift that originates from inherent fifth-order susceptibility of the nonlinear medium. Its sign is controllable by the sign of the phase mismatch of the third-harmonic generation process