Optical nonlinearity in Ar and N$_2$ near the ionization threshold

We directly measure the nonlinear optical response in argon and nitrogen in a thin gas target to laser intensities near the ionization threshold. No instantaneous negative nonlinear refractive index is observed, nor is saturation, in contrast with a previous measurement [Loriot et al., Opt. Express v. 17, 13429 (2009)] and calculations [Brée et al., Phys. Rev. Lett. v. 106, 183902 (2011)]. In addition, we are able to cleanly separate the instantaneous and rotational components of the nonlinear response in nitrogen. In both Ar and N$_2$, we observe the peak instantaneous index response scale linearly with the laser intensity until the point of ionization, whereupon it turns abruptly negative and ~constant, consistent with plasma generation.

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