Since the discovery of optical bistability a considerable amount of research activity has been aimed toward the realization of general-purpose all-optical computers. The basic premise for most of this work is the widely held notion that a reliable optical switch can be fabricated from a piece of optically bistable material. To date only a very small number of published articles have addressed the subject of the engineering issues (that is, the optimization and tolerancing) of these optical switches. This dissertation is a systematic treatment of these issues. From the starting point of Maxwell's equations a simple model of optically bistable Fabry-Perot etalons is outlined, in which the material is assumed to be a pure Kerr medium having linear absorption. This model allows for a relatively straightforward optical switch optimization procedure. The procedure is applicable for optimizing any number of switch parameters. The emphasis in this dissertation is on the optimization of the contrast of the switch's output signals, with the other parameters (switching energy, tolerance sensitivity) assuming a secondary yet critical role. Following the optimization of the optical switch is a tolerance analysis which addresses the manufacturability and noise immunity of the optimized switch. In the first part of this analysis equations describing the propagation of errors through a large scale system of like devices are derived from the truth tables of the switches themselves. From these equations worst case tolerances are established on the optical switch's transfer function parameters. In the second part of the tolerance analysis the bistability model is used to arrive at tolerances on the physical parameters of the switch. These tolerances are what determine the manufacturability of the optical switches. The major conclusion of the dissertation is that, within the range of validity of the model and the other simplifying assumptions, optically bistable Fabry-Perot etalons cannot be used reliably as logic gates in large-scale computing systems.

This dissertation describes the study of excitonic optical nonlinearities in semiconductors and semiconductor microstructures. The main emphasis is placed on the evolution of optical nonlinearities as one goes from bulk to quantum-confined structures. Included are experimental studies of molecular-beam-epitaxially-grown bulk GaAs and ZnSe, GaAs/AlGaAs multiple-Quantum-Wells (MQW's), and finally, quantum-confined CdSe-doped glasses. The microscopic origins and magnitudes of the optical nonlinearities of bulk GaAs and ZnSe were investigated and the exciton recovery time in ZnSe was measured. A comparison with a plasma theory indicates that in GaAs, band filling and screening of the continuum-state Coulomb enhancement are the most efficient mechanisms, while in ZnSe, exciton screening and broadening are the dominating mechanism for the nonlinearity. The maximum nonlinear index per excited electron-hole pair of ZnSe at room temperature is comparable to that of bulk GaAs and the exciton recovery times are of the order of 100 ps or less. A systematic study of the dependence of the optical nonlinearities on quantum well thickness for GaAs/AlGaAs MQWs and the results of nonlinear optical switching and gain in a 58 A GaAs/AlGaAs MQW are reported and discussed. The maximum change in the refractive index is greatest for the MQWs with the smallest well size and decreases with increasing well size, reaching a minimum for bulk GaAs. The maximum index change per photoexcited carrier increases by a factor of 3 as the well size decreases from bulk to 76 A MQW. A differential energy gain of 0.2 and the contrast of 4 are measured for a 58 MQW using 3 ns laser pulses. The linear and nonlinear optical properties of CdSe semiconductor microcrystallites grown under different heat treatments in borosilicate glasses are investigated. Pump-probe spectroscopic techniques and interferometric techniques were employed to study size quantization effects in these microcrystallites (quantum dots). Nonlinear optical properties due to the transitions between quantum confined electron and hole states are reported for low temperature and room temperature. A relatively large homogeneous linewidth is observed. Single beam saturation experiments for quantum confined samples were performed to study the optical nonlinearities as a function of microcrystallite size. Results indicate that the saturation intensity is larger for smaller size quantum dots.

This dissertation describes the study of various nonlinear optical effects in both bulk and quantum-confined semiconductors. Transverse effects in increasing absorption optical bistability are considered in bulk CdS for both single beam and wave mixing geometries. Measurement of the temporal response of BiI₃ quantum dots is described using degenerate four-wave mixing and explained theoretically. Finally, the experimental techniques developed to measure the one- and two-photon absorption coefficients of CdS quantum dots in glass are described along with the latest theoretical description and interpretation of the experimental spectra. The basic theory of increasing absorption optical bistability is presented along with experimental observation of this effect in CdS at low temperature. Transverse effects in increasing absorption optical bistability were observed in single beam experiments with CdS at low temperatures. The ring structures observed experimentally are explained theoretically. Degenerate four-wave mixing performed with this nonlinearity is theoretically shown to produce new scattering orders compared with a standard Kerr analysis. Experimental observation of these new scattering orders is presented. The temporal response of the nonlinearity in a solution of BiI₃ quantum dots in acetonitrile is determined using degenerate four-wave mixing. The independent contributions to the phase-conjugate signal are determined for both of the spatial gratings induced in the solution. The observed temporal responses indicated that a thermal mechanism was responsible for the nonlinearity. A theoretical analysis based on a thermal nonlinearity is presented which provides good agreement with the observed responses. The experimental techniques necessary to measure the one- and two-photon absorption coefficients of CdS quantum dots are described. The resultant measurements of quantum dot samples with microcrystallites ranging from 3.6 to 10.8 nm in diameter indicate no splitting of the energy levels associated with the hole. Theoretical spectra indicate this can be partially explained by the inclusion of Coulombic effects of the charged electron-hole pair.

This dissertation combines aspects of lasers, nonlinear optics and interferometry to measure the linear optical properties involved in phase matched second harmonic generation, (SHG). A new measuring technique has been developed to rapidly analyze the phase matching performance of potential SHGs. The data taken is in the form of interferograms produced by the self referencing nonlinear Fizeau interferometer (NLF), and correctly predicts when phase matched SHG will occur in the sample wedge. Data extracted from the interferograms produced by the NLF, allows us to predict both phase matching temperatures for noncritically phase matchable crystals and crystal orientation for angle tuned crystals. Phase matching measurements can be made for both Type I and Type II configurations. Phase mismatch measurements were made at the fundamental wavelength of 1.32 (mu)m, for: calcite, lithium niobate, and gadolinium molybdate (GMO). Similar measurements were made at 1.06 (mu)m. for calcite. Phase matched SHG was demonstrated in calcite, lithium niobate and KTP, while phase matching by temperature tuning is ruled out for GMO.

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

QC 351 A7 no. 66 / This volume is intended to be used as a text for two courses at the Optical Sciences Center. A major part of the volume consists of lecture notes on the theory of laser operation, written by M. O. Scully and M. Sargent III. These notes, developed under NSF sponsorship for a new quantum optics curriculum at the University of Arizona, were the basis of a new course "Quantum Optics," which was first offered during the 1969-70 academic year. After considerable editing they were again used during "The Physics of Quantum Electronics" summer course in Prescott, June 22 - July 3, 1970. The remainder of the volume consists of unpublished work presented at Prescott, most of which will be utilized in a new course on nonlinear optics. References are given to material presented that has already appeared in print.

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by Cheung Ka Wing = 由有機物質發放的超瑞利散射的光譜性硏究 / 張家榮. / Thesis (M.Phil.)--Chinese University of Hong Kong, 2000. / Includes bibliographical references (leaves 94-95). / Text in English; abstracts in English and Chinese. / by Cheung Ka Wing = You you ji wu zhi fa fang de chao rui li san she de guang pu xing yan jiu / Zhang Jiarong. / Title Page --- p.i / Acknowledgments --- p.ii / Abstract --- p.iii / Chinese Abstract --- p.iv / Table of Contents --- p.v / Chapter Chapter 1 --- Introduction --- p.1 / Chapter 1.1 --- Nonlinear Optics --- p.1 / Chapter 1.2 --- Tensor Properties of the Polarizability --- p.4 / Chapter 1.3 --- Inversion Symmetry --- p.5 / Chapter 1.4 --- Second Harmonic Generation --- p.6 / Chapter 1.5 --- Outline --- p.10 / Chapter Chapter 2 --- Measurement of the First Hyperpolarizability β --- p.11 / Chapter 2.1 --- Scattering by a Single Small Particle --- p.11 / Chapter 2.2 --- Rayleigh Scattering --- p.13 / Chapter 2.3 --- Fluctuation --- p.15 / Chapter 2.4 --- Hyper-Rayleigh Scattering --- p.16 / Chapter 2.5 --- Coherent and Incoherent Optical Processes --- p.16 / Chapter 2.6 --- Difference between Second Harmonic Generation (SHG) and Hyper Rayleigh Scattering (HRS) --- p.17 / Chapter 2.7 --- Measurement of the First Hyperpolarizability β by Electric Field Induced Second harmonic Generation (EFISHG) --- p.20 / Chapter 2.8 --- Measurement of the First Hyperpolarizability β by Hyper-Rayleigh Scattering (HRS) --- p.22 / Chapter 2.9 --- Two-Component System ´ؤ´ؤInternal Reference Method (IRM) and External Reference Method (ERM) --- p.23 / Chapter 2.10 --- Orientation Average of β --- p.25 / Chapter Chapter 3 --- Experimental Setup --- p.29 / Chapter 3.1 --- Detail Description of the Main Components --- p.29 / Chapter A). --- Laser System --- p.29 / Chapter B). --- Monochromator --- p.33 / Chapter C). --- Photomultiplier Tubes (PMT) --- p.36 / Chapter D). --- Photon Counter --- p.37 / Chapter 3.2 --- Layout of the Optical Design and Alignment Procedures --- p.39 / Chapter 3.3 --- Difficulties in the Experiment --- p.42 / Chapter A). --- Alignment --- p.42 / Chapter B). --- Temporal Stability of the Apparatus --- p.43 / Chapter C). --- The Effects of Using Different Sample Cells --- p.47 / Chapter 3.4 --- Sample Preparation --- p.48 / Chapter 3.5 --- Special Interest on the Organic Compounds --- p.49 / Chapter Chapter 4 --- Measurement on p-nitroaniline --- p.52 / Chapter 4.1 --- The Spectrum of Light Signal from pNA --- p.52 / Chapter 4.2 --- Concentration Dependence Measurement --- p.54 / Chapter Chapter 5 --- Measurement of the Hyperpolarizability of a Fluorescence Dye --- p.58 / Chapter 5.1 --- The Spectrum of Light Signal from DANS --- p.58 / Chapter 5.2 --- Design of an Experimental Technique to Measure β of Fluorescence Dyes that is Absorptive at the Second Harmonic --- p.61 / Chapter 5.3 --- Result of the Measurement on DANS --- p.64 / Chapter Chapter 6 --- Studies of the First Hyperpolarizability β of Two New Compounds --- p.74 / Chapter 6.1 --- The New Compounds --- p.74 / Chapter 6.2 --- Measurement on NC1 --- p.75 / Chapter 6.3 --- Measurement on NC2 --- p.79 / Chapter Chapter 7 --- Probing the Molecular Interaction in a Liquid Using HRS --- p.84 / Chapter 7.1 --- The Spectrum of Light Signal from Nitrobenzene --- p.85 / Chapter 7.2 --- The Signal Depolarization Ratio --- p.86 / Chapter 7.3 --- Results of the Depolarization Ratio Measurement on pNA --- p.87 / Chapter 7.4 --- Results of the Depolarization Ratio Measurement on Nitrobenzene --- p.88 / Chapter Chapter 8 --- Conclusions --- p.91 / References --- p.94

Wong, Chi Yan. / Thesis (Ph.D.)--Chinese University of Hong Kong, 2013. / Includes bibliographical references (leaves 134-149). / Electronic reproduction. Hong Kong : Chinese University of Hong Kong, [2012] System requirements: Adobe Acrobat Reader. Available via World Wide Web. / Abstract also in Chinese.

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