Results of research on surface emission from a waveguide due to second-harmonic generation are presented. This concept has been applied and demonstrated here in the InP-InGaAsP material system for the first time, using a fundamental wavelength of 1.32 |im and a harmonic surface emission at 660 nm. The surface emission is the result of the nonlinear mixing of two counterpropagating modes in a waveguide. The theory of nonlinear optics that produces this effect is explained, leading up to a model that describes the behaviour of the surface emitting waveguide (SEWG). This model is then used to design a pseudo-optimized structure that was subsequently grown, characterized and tested. Device performance and behaviour are compared with theoretical predictions. / Thesis / Master of Engineering (ME)

published_or_final_version / Chemistry / Doctoral / Doctor of Philosophy

Charge trapping dynamics in Si/SiO2/Hf(1-x)SixO2 and III-V film stack systems are characterized using spectroscopic ellipsometry (SE) and second harmonic generation (SHG). For the first time, discrete absorption features within the bandgap of the SiO2 interfacial layer are identified using SE, and their relation to both intrinsic and process-induced defects is proposed. Sensitivity of the absorption features to process conditions is demonstrated and evidence that these defects contribute to Vfb roll-off is presented. Defects in the Hf(1-x)SixO2 films are probed with fs laser-induced internal multi-photon photo-excitation (IMPE) and time dependent electrostatic field induced second harmonic (TD-EFISH) generation. For the as deposited HfO2 films, a unique TD-EFISH response is identified and explained by resonant two photon ionization of a specific point defect and subsequent tunneling of the photoelectrons to the Si substrate. Charge trapping kinetics for all Hf(1-x)SixO2 films are investigated. Two characteristic trap cross sections are identified and found to be insensitive to dielectric film and process conditions, and associated with a surface “harpooning” mechanism. EFISH from non-centrosymmetric III-V media, including GaAs and In0.53Ga0.47As, is also studied. The anisotropic and time dependent SHG response from different chemically treated In0.53Ga0.47As surfaces is clearly distinguishable and associated with a process-induced change in the surface depletion field. / text

Second harmonic generation (SHG) is a nonlinear optical effect sensitive to interfaces between materials with inversion symmetry. It is used as an effective tool for detection of the adsorption of a substance to microscopic particles, cells, liposomes, emulsions and similar structures, surface analysis and characterization of microparticles. The scattered second harmonic (SH) intensity from surfaces of suspended microparticles is characterized by its complex angular distribution dependence on the shape, size, and physical and chemical properties of the molecules making up the outer layer of the particles. In particular, the overall scattered SH intensity has been predicted to have a dramatic and nontrivial dependence on the particle size. Results are reported for aqueous suspensions of polystyrene microspheres with different dye molecules adsorbed on their surfaces. They indicate that the scattered SH power has an oscillatory dependence on the particle size. It is also shown that adsorption of one of the dyes (malachite green) on polystyrene particles is strongly affected when SDS surfactants are added to the solution. For this system a rapid increase of the SH signal with increasing concentration of SDS was observed in the range of low SDS concentration. Three different theoretical models are used to analyze the observed particle size dependence of SHG. The calculated angular and particle size dependences of the SH scattered power show that the models do not agree very well between each other when the size of the particles is of the order of the fundamental light wavelength, as here. One of the models - nonlinear Mie scattering - predicts oscillatory behaviour of the scattered SH power with the particle size, but fails to reproduce the position of the maxima and minima of the experimentally observed oscillations. The obtained results on the size dependence of the SH can be used in all applications to increase the count rate by choosing particles of the size for which the SH efficiency was found to the highest. A new effect of cooperative malachite green and SDS interaction at the polystyrene surface can be employed, for example, in the areas of microbiology or biotechnology, where adsorption macromolecules, surfactants and dyes to polystyrene microparticles is widely used.

Chiral molecules, which exist under enantiomers with non-mirror-symmetrical structures, have been the subject of intense research for their linear and nonlinear optical activities. Cysteine is such a chiral amino acid found as a building block of proteins throughout human bodies. Second harmonic generation (SHG) has been considered to investigate chiral molecules. SHG from metallic nanoparticles is promising for nanoplasmonics and photonic nanodevice applications. Therefore, it’s desirable to combine and study nonlinear properties due to both chirality and metallic nanoparticles, and help developing an alternatively optical diagnostic of chiral molecules. Our experiments are carried out with the FemtoFiber Scientific FFS laser system. SHG of silver nanoparticles (Ag NPs) modified by either L-Cysteine (L-C) or D-Cysteine (D-C) is observed, where L-Cysteine and D-Cysteine are a pair of enantiomers. Ag NPs are deposited through Vacuum Thermal Evaporation, controlled under different deposition thicknesses. UV-Vis/IR spectra and AFM are used to characterize Ag NPs under different conditions. Transmitted SHG measurements dependent on incidence are recorded with standard lock-in techniques. Deposition thickness of vacuum thermal evaporation plays an important role in forming diverse Ag NPs, which strongly imparts the intensity of SHG. Second harmonic intensity as a function of the incident angle presents similar results for Ag NPs with or without L-Cysteine or D-Cysteine modification, in the output of p- and s-polarization. However, we monitor reversed rotation difference in second harmonic intensities at linearly +45° and -45° polarization for L-C/Ag NPs and D-C/Ag NPs, while there’s no difference at linearly +45° and -45° polarization for Ag NPs alone. This optical rotation difference in SHG is termed as SHG-ORD. Also, for second harmonic light fixed at p-polarization, L-C/Ag NPs and D-C/Ag NPs exhibit a reversely net difference for SHG excited by right and left circular polarization, which is termed as SHG-CD. Experiments on SHG-ORD of chiral-modified Ag NPs by a mixture of L-Cysteine and D-Cysteine further help verifying the existence of chirality in chiral-modified Ag NPs. As a conclusion, SHG efficiently probed and distinguished L-Cysteine from D-Cysteine in chiral-modified Ag NPs. / Thesis (Master, Physics, Engineering Physics and Astronomy) -- Queen's University, 2013-09-29 21:27:23.112

To Chi Wing = 具非線性光學性質客體-主體聚合物系統的極化動力學研究 / 杜志榮. / Thesis (M.Phil.)--Chinese University of Hong Kong, 2006. / Includes bibliographical references (leaves 102-104). / Text in English; abstracts in English and Chinese. / by To Chi Wing = Ju fei xian xing guang xue xing zhi ke ti-zhu ti ju he wu xi tong de ji hua dong li xue yan jiu / Du Zhirong. / Table of contents / Acknowledgements --- p.ii / Abstract --- p.iii / Chinese Abstract --- p.iv / Table of Contents --- p.v / List of Figures --- p.viii / Chapter Chapter 1 --- Introduction --- p.1 / Chapter 1.1 --- Fundamental of nonlinear optics --- p.2 / Chapter 1.2 --- Centrosymmetry and even-order nonlinear susceptibilities --- p.4 / Chapter 1.3 --- Generation of second harmonic radiation --- p.5 / Chapter 1.4 --- Tensor properties of the nonlinear susceptibilities --- p.7 / Chapter 1.5 --- Relationship between macroscopic and microscopic nonlinear susceptibility for a poled polymer --- p.8 / Chapter 1.6 --- Outline of the thesis --- p.12 / Figures --- p.13 / Chapter Chapter 2 --- Poling and Relaxation of Guest-host Polymeric System --- p.15 / Chapter 2.1 --- Guest-host nonlinear optical polymeric systems --- p.15 / Chapter 2.1.1 --- Photoisomerization of Azobenzene --- p.16 / Chapter 2.1.2 --- Disperse Red-1 --- p.17 / Chapter 2.1.3 --- Poly (methyl methacrylate) --- p.18 / Chapter 2.2 --- Poling techniques --- p.19 / Chapter 2.2.1 --- Thermal Assisted Electric-field Poling --- p.19 / Chapter 2.2.2 --- Photo-assisted Electric-field poling --- p.22 / Chapter 2.2.3 --- All-Optical Poling --- p.25 / Chapter 2.3 --- Relaxation of poled nonlinear optical polymers --- p.27 / Figures --- p.31 / Chapter Chapter 3 --- Experimental Methods --- p.36 / Chapter 3.1 --- Sample Preparation --- p.36 / Chapter 3.2 --- Experimental Setup --- p.38 / Chapter 3.2.1 --- Laser system --- p.38 / Chapter 3.2.2 --- The reference arm --- p.39 / Chapter 3.2.3 --- The sample arm --- p.40 / Chapter 3.2.4 --- Data acquisition (DAQ) system --- p.41 / Chapter 3.2.5 --- Temperature control --- p.42 / Chapter 3.3 --- Poling and the erasing of thermal history --- p.43 / Chapter 3.3.1 --- All Optical Poling --- p.43 / Chapter 3.3.2 --- Eecteic Poling --- p.44 / Chapter 3.3.3 --- Erasure of thermal history --- p.45 / Figures --- p.46 / Chapter Chapter 4 --- Experimental results and discussions --- p.51 / Chapter 4.1 --- Reliability and reproducibility --- p.51 / Chapter 4.2 --- Features of different poling techniques --- p.52 / Chapter 4.2.1 --- Sub-Tg electric Poling --- p.53 / Chapter 4.2.2 --- Thermal assisted electric Poling --- p.54 / Chapter 4.2.3 --- Photo assisted electric Poling --- p.55 / Chapter 4.3 --- Relaxation of poling induced x(2) --- p.56 / Chapter 4.4 --- Effect of physical aging on the relaxation of PAP induced x{2) --- p.58 / Chapter 4.4.1 --- Origin of physical aging and its effect on relaxation --- p.58 / Chapter 4.4.2 --- Effect of aging on the relaxation of a PAP sample --- p.59 / Chapter 4.5 --- Onset studies of photo-induced free volume --- p.61 / Chapter 4.6 --- Comparative studies of TAP and PAP induced x{2) --- p.62 / Chapter 4.6.1 --- Secondary Poling --- p.63 / Chapter 4.6.1.1 --- Model for describing the temporal behavior of secondary poling --- p.65 / Chapter 4.6.1.2 --- Experimental details of the secondary poling measurement --- p.68 / Chapter 4.6.1.3 --- Results and Discussion on secondary poling of sample poled by TAP or PAP --- p.69 / Chapter 4.6.2 --- Onset of second harmonic signal during electric poling --- p.71 / Chapter 4.7 --- Charge injection studies --- p.73 / Figures --- p.77 / Chapter Chapter 5 --- Conclusion --- p.98 / References --- p.101

<p>Second harmonic generation (SHG) is a nonlinear optical effect sensitive to interfaces between materials with inversion symmetry. It is used as an effective tool for detection of the adsorption of a substance to microscopic particles, cells, liposomes, emulsions and similar structures, surface analysis and characterization of microparticles. The scattered second harmonic (SH) intensity from surfaces of suspended microparticles is characterized by its complex angular distribution dependence on the shape, size, and physical and chemical properties of the molecules making up the outer layer of the particles. In particular, the overall scattered SH intensity has been predicted to have a dramatic and nontrivial dependence on the particle size.</p><p>Results are reported for aqueous suspensions of polystyrene microspheres with different dye molecules adsorbed on their surfaces. They indicate that the scattered SH power has an oscillatory dependence on the particle size. It is also shown that adsorption of one of the dyes (malachite green) on polystyrene particles is strongly affected when SDS surfactants are added to the solution. For this system a rapid increase of the SH signal with increasing concentration of SDS was observed in the range of low SDS concentration.</p><p>Three different theoretical models are used to analyze the observed particle size dependence of SHG. The calculated angular and particle size dependences of the SH scattered power show that the models do not agree very well between each other when the size of the particles is of the order of the fundamental light wavelength, as here. One of the models - nonlinear Mie scattering - predicts oscillatory behaviour of the scattered SH power with the particle size, but fails to reproduce the position of the maxima and minima of the experimentally observed oscillations.</p><p>The obtained results on the size dependence of the SH can be used in all applications to increase the count rate by choosing particles of the size for which the SH efficiency was found to the highest. A new effect of cooperative malachite green and SDS interaction at the polystyrene surface can be employed, for example, in the areas of microbiology or biotechnology, where adsorption macromolecules, surfactants and dyes to polystyrene microparticles is widely used.</p>

Diamond-like semiconductors are interesting materials to study due to the wide variety of technologically useful properties that these materials possess. These normal valence compounds have structures that are based on that of diamond, either the cubic or hexagonal polymorph. Though there are a finite number of possible compounds, due to isovalent and isoelectronic principles, the total number of potential compounds is quite extensive. Quaternary diamond-like semiconductors provide a unique opportunity, because much of the previous research has focused on binary and ternary systems leaving quaternary systems, relatively unexplored. Additionally, quaternary diamond-like semiconductors possess a greater degree of compositional flexibility compared to binary and ternary materials, which could result in the ability to more carefully tune desired physical properties. &lt;br&gt;In order to prepare the new materials, Li2ZnGeS4, Li2ZnSnS4, Li2CdGeS4, Li2CdSnS4 and Ag2MnSnS4, several synthetic methods have been employed, including high-temperature solid-state synthesis, polychalcogenide flux synthesis and solid-state microwave synthesis. The solid-state microwave synthetic method was itself studied using a number of target systems such as the ternary diamond-like semiconductor, AgInSe2. Additionally, several intermetallic compounds, such as Ag3In, AuIn2 and Bi2Pd were prepared using this procedure. Solid-state microwave synthesis is not as well known as some of the other synthetic methods that were employed in this work possibly due to a lack of understanding of the method, training and equipment. Despite these problems, the method has the potential to save time, energy and cost due to the unique nature of microwave heating. In an attempt to gain a better understanding of this synthetic method and its capabilities, the solid-state microwave synthetic method was used to prepare diamond-like semiconductors and intermetallic compounds. / Bayer School of Natural and Environmental Sciences / Chemistry and Biochemistry / PhD / Dissertation

Conventional step-index silica fibers do not possess a second-order optical nonlinearity due to symmetry concerns. However, through the process of poling, the generation of a frozen-in DC field $E^{DC}$, and in turn, a non-zero second-order nonlinearity $\chi^{(2)} = 3\chi^{(3)}E^{DC}$, can be created in optical fibers. In this thesis, I measure the individual $\chi^{(2)}$ tensor elements of birefringent periodically poled fiber via second-harmonic generation and sum-frequency generation experiments. The symmetry of the $\chi^{(2)}$ tensor is consistent with that of the $\chi^{(3)}$ for isotropic media. This is the first study that characterizes all the $\chi^{(2)}$ tensor elements in birefringent poled fiber. Furthermore, I investigate the intermix of the $\chi^{(2)}$ tensor elements by twisting the fiber, which results in the generation of new second-harmonic signals not observed in untwisted fiber. The conversion efficiencies and spectral positions of these new signals can be varied by twisting the fiber.

The three wave mixing process was modeled in GaAs:AlGaAs superlattices using two new modeling tools that were developed in the course of this work: A 2D beam propagation tool for optimizing quasi-phase matching gratings, and a 1D iterative beam propagation tool for determining the output powers and threshold of optical parametric oscillators of arbitrary geometries. The 2D tool predicts close to 80% enhancement of conversion e ciency by phase matching near 800 nm compared to 775 nm, which was the originally designed operation wavelength. The model also predicts resonant behaviour for an abrupt grating pro le. The 1D tool was used to determine the threshold conditions for para- metric oscillation for di erent geometries. The performances of di erent phase matching approaches in AlGaAs were quantitatively compared. The model also indicated the need for pulsed operation to achieve reasonably low threshold powers in AlGaAs waveguides.