Optical nonlinearity in Ar and N2 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 [Opt. Express 17, 13429 (2009)] and calculations [Phys. Rev. Lett. 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 N2, the peak instantaneous index response scales linearly with the laser intensity until the point of ionization, whereupon the response turns abruptly negative and ∼constant, consistent with plasma generation.