Second-harmonic scattering by domains in RbH2PO4 ferroelectrics

Second-harmonic scattering (SHS) of light by laminar ferroelectric domains of the orthorhombic phase of RbH₂PO₄ below T_c=147 K is studied in detail. CCD images of the far-field SHS pattern reveal up to six off-axis distinct intensity maxima in a plane normal to the ferroelectric axis c. These scattering maxima are interpreted on the basis of the quasi-phase matching (QPM) conditions for the three sets of polarizations allowed by the nonvanishing elements of the second-order nonlinear susceptibility tensor. On this assumption scattering angles of the three SHS modes calculated from crystal optics are shown to fit well the experimental data for any incidence of the pump beam normal to c. Scattering intensities of the two most intense modes are also measured versus the component of the wave vector perpendicular to the modulated structure. A stochastic model giving the intensity as a function of the density probability of domain widths is developed and is shown to give a good fit of the scattered intensity. Moreover, it permits the evaluation of the mean and dispersion of the ferroelectric domain widths, which are found to be, respectively, 2.6 and 0.7 μm in the crystal under study. This is consistent with the domain size of the ferroelastic counterpart revealed by polarization microscopy.