A nonlinear-optical investigation technique for the domain structuring in ferroelectric crystals is reported. Noncollinear optical frequency doubling in a quasiphase-matched scheme allows for conclusions on the k-space representation of the domain morphology or-putting it in other terms-on the k-space representation of the correlation lengths ͑k-space spectroscopy͒. As an example, the ferroelectric-to-paraelectric phase transition of the relaxor ferroelectric strontium-barium niobate ͑SBN͒ is studied. One important result is that homogeneously poled crystals of SBN do not uniquely go through the phase transition as commonly assumed. Instead, the correlation length shows a characteristic anisotropic behavior in the phase-transition region.
The optical properties of single crystals of strontium barium niobate, grown from the congruently melting composition and doped with different amounts of europium, are investigated. Absorption and emission spectra are measured in the visible and infrared spectral regions at different temperatures. From the spectra, conclusions on the structural sites can be drawn, revealing the major occupations of the B1 and B2 sites, and a minor one of the A2 site. The data are used to calculate crystal-field parameters for the mainly occupied site. A Judd-Ofelt analysis shows that the radiative quantum efficiency is approximately 70%. Furthermore, the influence of europium doping on the phase-transition temperature is determined.
We present investigations of the domain dynamics and of the evolution of the critical exponent β in a ferroelectric relaxor system, exemplarily in the up-to-date controversial strontium barium niobate (SBN). k-space spectroscopy at the phase-transition and when applying an electric field reveals a size-dependent response of the domains. This is supported by pyroelectric measurements that show, by analysis in terms of criticality, the critical exponent β is not only dependent on the level of poling but also on the manner in which the poling was achieved. It must be concluded that the crystals undergo a phase transition not—as commonly assumed—in a uniform way with homogeneous polarization throughout the crystal. Instead they behave as a set of more or less independent domains with size-dependent stability. Therefore, one should be very careful with critical exponents—especially those derived from experiments that explicitly or implicitly—assume a uniform polarization behavior.
The product of the linear electro-optic coefficient with the electron-hole competition factor r33ζ is determined as a function of the wavelength together with the photorefractive trap density Neff in cerium-doped strontium barium niobate. The photorefractive method of photoinduced light scattering is applied. A pronounced increase of r33 by more than a factor of 2 is self-evident in the blue-green spectral range, which is described by a theoretical approach based on the combination of the Sellmeier formulation and the polarization tensor concept. By this further important material parameters are estimated, such as the strength and frequency of the average dipole oscillator characterizing the optical interband transfer.
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