Nonlinearity measurements of thin films by third-harmonic-generation microscopy.

We show that the electronic part of the nonlinear susceptibility chi(3) of thin films can be easily measured by third harmonic microscopy. The phenomenon of third harmonic generation (THG) is excited by a femtosecond laser beam focused at the interface between the thin film and a reference layer. The value of chi(3) is deduced from the THG intensity measurements with the help of a classical model. The validity of this simple and alternative method is established by testing reference liquid films.