Studies on Domain Dynamics in Nonlinear Optical Ferroelectric Oxide Crystals

Nonlinear optical frequency conversion is the key technology for modifying laser output radiation, in order to target specific applications. The most powerful technique to obtain tailored second-order nonlinear interactions is the quasi-phasematching (QPM) approach. QPM is based on periodic modulation of the medium’s nonlinearity and allows versatile and efficient frequency conversion in the whole transparency region of the material. QPM is commonly implemented in ferroelectric oxide crystals by periodically inverting the spontaneous polarization, so-called, periodic poling. However, in order to achieve QPM structures of practical relevance, both the optical properties of the material and the domain engineering techniques have to be suitable for the targeted nonlinear interaction. Rb-doped KTiOPO4 (RKTP) and vapor-transport-equilibrated stoichiometric LiTaO3 (VTE-SLT) are two of the most promising ferroelectric oxides used for nonlinear optics. The former is suitable for high peak-power applications and for engineering of QPM devices with sub-µm periodicity. The latter shows a short cut-off wavelength with low linear absorption, which makes it very attractive for UV-light generation. However, in order to fully exploit the potential of these two materials, it is of utmost importance to understand the domain dynamics and stability from a fundamental point of view, as well as to investigate ways to overcome their limitations. This thesis presents studies on domain dynamics and stability in these two materials. A novel method for periodic poling of RKTP has been investigated. The method, based on using a micro-structured silicon chip as the contact electrode, has been used to fabricate periodically poled RKTP crystals with 9.01 µm period. The samples became well-poled and showed high conversion efficiency for second harmonic generation. The domain dynamics, when the silicon stamp was used as an electrode were studied, showing potential for short-pitch poling and complex patterning. Furthermore, the domain stability in RKTP during thermal annealing at high temperatures was investigated. The results show anisotropic domain wall motion, with severe domain contraction along the crystallographic b-axis when the periodicity was reduced. A technique to suppress this domain contraction was developed based on dicing away the edges of the QPM grating so that the domain b-faces terminate in air. This gave excellent results for a broad range of periodicities. Studies of the domain stability of periodically poled VTE-SLT during chemical etching were performed by on-line second harmonic generation, and optical microscopy. The results show that wet etching directly after poling leads to domain-wall motion, resulting in back-switching or domain merging. Furthermore, the domain wall motion induced by electron beam irradiation was investigated using a scanning electron microscope. It was found that domain switching strongly depends on the ratio of secondary electrons to incident electrons. These results are discussed in terms of electron beam and screening charges interaction.QC 20190412