Andrius Zukauskas

Abstract:

Even though KTiOPO₄ (KTP) is considered to be one of the best nonlinear materials for quasi-phase matched (QPM) frequency conversion in the visible and the near-infrared spectral regions, its use is often limited by poor material homogeneity, high ionic conductivity, a considerable linear absorption and photochromatic damage. On the other hand, the improved material homogeneity and the lower ionic conductivity of bulk Rb-doped KTP (RKTP) make this material an ideal alternative for fabrication of fine-pitch QPM gratings, while the arsenate isomorph KTiOAsO₄ (KTA) promises a better performance in the green spectral region and adds the advantage of a wider transparency window in the infrared. Unfortunately, the available studies on these materials are limited and unable to answer the question whether RKTP and KTA are feasible alternatives to KTP in terms of periodic poling and optical performance. 

The optical performance of the QPM devices depends on the periodic poling quality, therefore, a detailed comprehension of domain-grating formation in the KTP isomorphs is highly desired. The goals of this thesis were to gain a better understanding of the periodic poling process in the KTP isomorphs, in order to study the specifics of ferroelectric domain engineering in KTA and RKTP, and to evaluate the optical performance of these isomorphs. Fine-pitch periodically-poled structures were engineered both in KTA and RKTP crystals. It was demonstrated that QPM gratings with excellent quality and with periods as short as 8.49 μm can be fabricated in KTA crystals. Comparative transmission studies have shown that periodically poled KTA (PPKTA) crystals can be superior to KTP for QPM second harmonic generation in the visible spectral region due to lower linear absorption.

It was also demonstrated that RKTP is a superior alternative to KTP for high-quality QPM grating fabrication. A consistent room-temperature periodic poling of 5 mm thick RKTP crystals with a period of 38.86 μm has been achieved. The obtained large aperture periodically poled RKTP (PPRKTP) crystals showed an outstanding QPM grating uniformity and excellent optical performance in optical parametric oscillator (OPO) applications. Moreover, it was shown that RKTP is less susceptible to blue-induced infrared absorption than KTP.

Finally, a novel and a relatively simple method for self-assembling quasi-periodic sub-μm scale ferroelectric domain structure in RKTP crystals has been presented. It was shown that, after treatment in aqueous KOH/KNO₃ solution, periodic poling of RKTP with planar electrodes resulted in one-dimensional ferroelectric domain structure with an average periodicity of 650±200 nm, extending over the whole 1 mm thick crystal. Such self-assembled structures in RKTP were used to demonstrate 5^thorder non-collinear QPM backward second harmonic generation.