Hyper-Rayleigh scattering, originally based on low repetition rate nanosecond pulse lasers and gated detection, has provided a wealth of hyperpolarizability data from organic and organometallic species in isotropic solution. We here present experimental advances in hyper-Rayleigh scattering recently developed in our laboratory. These advances have improved both accuracy and resolution, and have also imparted new possibilities. The addition of angular resolution, originally intended for better accuracy when phase relations between the chromophores exist, has proven useful for the attribution of photonic crystal properties based on these phase relations. The use of high repetition rate femtosecond pulses has allowed frequency resolution, initially used for better accuracy with fluorescent chromophores. The use of the complete Fourier domain (i.e., phase and demodulation data) additionally allows better precision. Finally, this frequency resolution also allows the study of photonic bandgap (PBG) properties.