Quadratic hyperpolarizabilities of fluorinated sulfonyl and carbonyl aromatics: optimization of nonlinearity and transparency trade-off

Abstract

We present electric-field induced second-harmonic generation measurement results on the hyperpolarizabilities of donor-acceptor substituted aromatics. Those with strongly inductive accepting groups, such as the fluoromethyl carbonyl, perfluoroalkyl sulfonyl, and perfluoroalkyl sulfonylsulfimide groups, afford favorable trade-off between quadratic optical nonlinearity and optical transparency. Their relatively large molecular dipole moment and hyperpolarizability products (4) as well as high transparency in the visible region suggest promising applications in the frequency conversion of short wavelength diode lasers. The inductive contribution is found to be short ranged, being most effective in the relatively compact benzene derivatives but less so in the extended stilbene structures. Dispersive enhancements of hyperpolarizabiities at 1064 and 810 nm are also reported.