The third-order nonlinearities of the GaP sample in the 600- to 1000-nm wavelength range were estimated with the single-beam Z-scan technique, using the same setup as described elsewhere (23). The laser beam from the tunable laser system mentioned above was focused onto the sample with a 150-mm plano-convex lens (Rayleigh range of 2.2 ± 0.3 mm), and the transmitted light was recorded with a Thorlabs DCC1545M CMOS (complementary metal-oxide semiconductor) camera. In the long-wavelength end (900 to 1000 nm), the nonlinear absorption coefficient was determined using a 125-mm lens to improve the signal-to-noise ratio. The sample was moved through the lens focus using a Thorlabs PT1/M-Z8 motorized stage. For each position of the sample, the transmitted intensity distribution was registered, and the open and closed Z-scan traces were obtained by summing over all camera pixels and over a reduced circular region in the center containing 2% of the total intensity, respectively. The normalized Z-scan data were fitted using standard formulae from the literature (24, 25). Z-scan results can be found in the Supplementary Materials.

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