High-order (N = 4–6) multiphoton absorption and mid-infrared Kerr nonlinearity in GaP, ZnSe, GaSe, and ZGP crystals

Abstract

We report a study of high-order multiphoton absorption, nonlinear refraction, and their anisotropy in four notable mid-infrared χ(2) crystals: GaP, ZnSe, GaSe, and ZGP using femtosecond pulses at 2.35  μm with peak intensity in excess of 200 GW/cm2. We found that the nonlinear absorption obeys a perturbation model with multiphoton absorption (MPA) orders from N = 4–6, in agreement with the bandgaps of the crystals. A study of the role of free carrier absorption, performed by changing the pulse duration from 30 to 70 fs while maintaining a constant peak intensity, showed that, at our intensity levels, free carriers generated during the MPA process absorb much more strongly than would be expected from their known linear absorption cross section. Possible mechanisms for this anomalous behavior are high-field effects, such as intravalley scattering in the conduction band and absorption to higher lying bands. Nonlinear refractive indices were measured using (i) closed aperture Z-scan and (ii) spectral broadening due to self-phase modulation, both methods agreeing with each other.