Spectral features of hyper-Rayleigh scattering in chloroform-d

Measurements of hyper-Rayleigh scattering (HRS) in chloroform-d indicate that interaction induced contributions account for more than half of the scattered intensity from the liquid phase. The effective hyperpolarizability obtained from the entire liquid HRS spectrum in the VV polarization geometry is [beta(VV)(2)](1/2) = 15.7 +/- 0.6 au. The unimolecular hyperpolarizabilities obtained from the Lorentzian components of the HRS spectrum are [beta(VV)(2)](1/2) = 10.2 +/- 0.7 au and beta(parallel to) = 10.8 +/- 0.5 au. This value for beta(parallel to) differs substantially from that previously inferred from electric field induced second harmonic generation (EFISH) measurements, calling into question previous HRS results calibrated using chloroform as a standard. (C) 1998 Elsevier Science B.V. All rights reserved.