Nonlinear optics with full three-dimensional illumination

We investigate the nonlinear optical process of third-harmonic generation in argon gas in a thus-far-unexplored regime of focusing the pump light from a full solid angle. We reason that the observed generation of frequency-tripled photons is due to six-wave mixing, in agreement with observations in the paraxial regime. Furthermore, we provide numerical simulations that reproduce the amount of frequency-tripled light as a function of the solid angle used for focusing and that yield a fifth-order susceptibility of $\chi^{(5)}=1.53^{+0.21}_{-0.18}\times10^{-48}\,(\text{m/V})^4/\text{bar}$ for this particular six-wave mixing process.