Hyper-Rayleigh scattering is frequently used to determine all of the rotational invariants of the first hyperpolarizability tensor. It requires numerous polarization states of both incident and scattered light and thus justifies the use of a dual-rotating-retarder polarimeter. We optimized our experimental setup by reducing the condition number of the polarization processing matrix. Our numerical study showed that, on condition to make six measurements, the choice of the detector angle and of the angular steps of both retarders was paramount. Overspecifying the calculation through a much higher number of measurements allowed us to make broad optimal detector angles and retarder angular steps available. Numerical simulations are presented to optimize our experimental setup.
© 2007 Optical Society of AmericaFull Article | PDF Article