Surface behaviour of nco species on Rh(111) and polycrystalline Rh surfaces

Quasi-phase-matching (QPM) is a method to get tailored efficient second order nonlinear interactions [1]. Several techniques exist for fabrication of periodic domain structures in ferroelectric crystals for QPM frequency conversion. By far, electric field poling using lithographically patterned electrodes on the z-face of the crystal is the most common one [2]. High-quality periodically inverted ferroelectric domain structures in flux grown KTiOP 4 (KTP) crystals were fabricated already in the late 90's using this technique [3], and recently periodic domain sizes of few hundred nanometers were fabricated in 1 mm thick samples thanks to the quasi-one dimensional structure of KTP. It has recently also been shown that a slight Rb doping of the KTP crystal (RKTP) facilitates the periodic poling [4]. However, fabrication of two-dimensional (2D) domain structures in RKTP has not yet been investigated. A disadvantage with the lithographic patterning is that each sample needs to be patterned individually, which is tedious and time consuming. Moreover, when it comes to the small domain features, which are required by the next generation of nonlinear optical devices, a more versatile poling technique has to be developed due to the limitations of conventional photolithography. Structured silicon has been investigated as an alternative electrode for formation of 1D domains by contact poling in LiNb3 [5]. However, these electrodes were fabricated by wet etching and the sample thickness was limited to ∼200 μm.QC 20140619</p

Electron-beam-induced ferroelectric domain behavior in the transmission electron microscope: Toward deterministic domain patterning

We report on transmission electron microscope beam-induced ferroelectric domain nucleation and motion. While previous observations of this phenomenon have been reported, a consistent theory explaining induced domain response is lacking, and little control over domain behavior has been demonstrated. We identify positive sample charging, a result of Auger and secondary electron emission, as the underlying mechanism driving domain behavior. By converging the electron beam to a focused probe, we demonstrate controlled nucleation of nanoscale domains. Molecular dynamics simulations performed are consistent with experimental results, confirming positive sample charging and reproducing the result of controlled domain nucleation. Furthermore, we discuss the effects of sample geometry and electron irradiation conditions on induced domain response. These findings elucidate past reports of electron beam-induced domain behavior in the transmission electron microscope and provide a path towards more predictive, deterministic domain patterning through electron irradiation.</p

QPM Devices in KTA and RKTP

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 5th order non-collinear QPM backward second harmonic generation.QC 20140114</p

QPM Devices in KTA and RKTP

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 5th order non-collinear QPM backward second harmonic generation.QC 20140114</p

Short Period, Large Aperture PPRKTP via Coercive Field Engineering : Key Parameters

We demonstrate large aperture PPRKTP with a period as short as 3.43 m fabricated via coercive-field engineering through ion-exchange. The key parameters to achieve high-aspect ratio domain structures are discussed.</p

Second-harmonic generation in periodically poled bulk Rb-doped KTiOPO_4 below 400 nm at high peak-intensities

We demonstrate that bulk Rb-doped KTiOPO4 (RKTP) shows improved susceptibility to gray-tracking compared to flux-grown KTiOPO4. We show high-fidelity periodic poling of 1 mm thick RKTP with a period of 3.18 mu m for second harmonic generation at 398 nm with a normalized conversion efficiency of 1.79%/Wcm. The crystal is used to frequency-double 138 fs-long pulses with an efficiency of 20% and a peak intensity of 560 MW/cm(2) without visible gray-tracking signs. We demonstrate that two-photon absorption is the predominant mechanism limiting the SHG efficiency in this spectral range at high peak powers and high repetition rates.</p

Quasi-periodic self-assembled sub-micrometer ferroelectric bulk domain gratings in Rb-doped KTiOPO₄

We present a simple technique for fabricating quasi-periodic bulk sub-μm ferroelectric domain gratings in Rb-doped KTiOPO4 (RKTP) based on self-organized ferroelectric domain formation. One-dimensional ferroelectric domain structures, with an average periodicity of 650 ± 200 nm and extending throughout 1 mm thick crystals, are obtained by etching and subsequent electric field poling using planar electrodes. The sub-μm structures in RKTP were used to demonstrate 5th order non-collinear quasi-phase matched backward second harmonic generation.</p