Nonlinear optical phenomena associated with high-order soliton breakup in photonic crystal fibres and squeezed state generation in three dimensional photonic crystal microcavities are investigated. In both cases, the properties of periodically patterned, high-index contrast dielectric structures are engineered to control the dispersion and local field enhancements of the electromagnetic field. Ultra-short pulse propagation in a polarization-maintaining microstructured fibre (with 1 um core diameter and 1.1 m length) is investigated experimentally and theoretically. For an 80 MHz train of 130 fs pulses with average propagating powers in the fibre up to 13.8 mW, the output spectra consist of multiple discrete solitons that shift continuously to lower energies as they propagate in the lowest transverse mode of the fibre. The number of solitons and the amount that they shift both increase with the launched power. All of the data is quantitatively consistent with solutions of the nonlinear Schrodinger equation, but only when the Raman nonlinearity is treated without approximation, and self-steepening is included. The feasibility of using a parametric down-conversion process to generate squeezed electromagnetic states in 3D photonic crystal microcavity structures is investigated for the first time. The spectrum of the squeezed light is theoretically calculated by using an open cavity quantum mechanical formalism. The cavity communicates with two main channels, which model vertical radiation losses and coupling into a single-mode waveguide respectively. The amount of squeezing is determined by the correlation functions relating the field quadratures of light coupled into the waveguide. All of the relevant model parameters are realistically estimated using 3D finite-difference time-domain (FDTD) simulations. Squeezing up to ~20% below the shot noise level is predicted for reasonable optical excitation levels. To preserve the squeezed nature of the light generated in the microcavity, a unidirectional coupling geometry from the microcavity to a ridge waveguide in a slab photonic crystal structure is studied. The structure was successfully fabricated in a silicon membrane, and experimental measurements of the efficiency for the signal coupled out of the structure are in good agreement with the result of FDTD simulations. The coupling efficiency of the cavity mode to the output channel is ~60%.

Resonant or near resonant optical nonlinearities in semiconductor coupled quantum-well systems are discussed. Quantum engineered coupled or cascade quantumwell structures can provide giant nonlinear susceptibilities for various optical nonlinear processes. Nonlinearities integrated within quantum cascade lasers (QCL) showed great potential in various applications in the infrared range. Several schemes of nonlinearities are proposed and discussed in this work. Integrating difference frequency generation (DFG) with QCL can yield long wavelength radiation, such as terahertz light. The DFG process does not require population inversion at a transition associated with low photon energy; however, this requirement is necessary to lasers, such as QCL, and is hard to meet, because of the thermal backfilling and inefficient injection or pumping at room temperature. Therefore terahertz radiation due to DFG QCL for room temperature is proposed. On the other hand, the second harmonic generation can double laser frequency, and then push radiation frequency of AlInAs/GaInAs/InP based QCL to short wavelengths such as 3 μm and shorter. Optical nonlinearities can extend working frequencies of light sources, and also can help to improve light detection. For example, a sum frequency generation can upconvert mid/far-IR signal into near-IR signal with strong near-IR pump light, namely high efficient near-IR photon detector could be employed to detect mid/far-IR light. A specific designed quantum well structure of this frequency up-conversion scheme is discussed. A scheme of monolithic in-plane integration of the optical nonlinearities with QCL is also proposed. In this scheme, an optical nonlinear section is made from the same quantum well structure of a QCL, and is under an independent applied bias. Due to the independence of the applied bias, the nonlinearities can be tuned flexibly. In particular, a widely tunable Raman laser based on this scheme could be achieved. A frequency up-conversion based on sum frequency generation process in coupled quantum-well structure is also proposed for mid-infrared detection. By converting mid-IR signal to near-IR, superior near-IR detector such as silicon avalanche photo diode (APD) can be employed. The scheme can provide lower noise equivalent power (NEP) or higher detectivity compared with regular semiconductor photo detectors. A scheme of lasing without inversion (LWI) based on QCL for THz radiation is proposed. A ladder type three-level system for LWI process is integrated into a boundto- continue high power QCL at 10 μm. The proposed LWI generates THz signal at 69 μm. An optical gain about 80 cm-1 is achieved, against a waveguide loss about 30 cm-1 in a semi insulator (SI) surface plasmon waveguide.

The first hyperpolarizability £], which is an important factor in the second-order nonlinear optical effect, of the 5-6-5 heterocyclic rigid-rod chromophores-based derivatives has been systematically investigated in this work, applying the first principle based software CASTEP and the semi-empirical software MOPAC There are four factors chosen for this computational analysis, including the effects of (i) various rigid-rod molecules, (ii) auxiliary ability of various five-member rings, (iii) donor ability, and (iv) conjugation length. Results indicate that the benzobisimidazole (BBI)-based derivatives have larger £] values than those of benzobisthiazole (BBT) and benzobisoxazole (BBO)-based derivatives. The auxiliary donor ability of the pyrrole is larger than that of the thiophene and furan. In general, the £] value of various derivatives studied is parallel to the original donor strength and the trend in the donor is -N(CH3)2 > -NH2 > -OH > -CH3. In addition, the greater the conjugation length in the derivatives is, the higher the £] value. Further, from the analyses on the band-resolved £] values and the orbital density figures, it is found that the major contribution to the enhanced £] comes primarily from an efficient charge transfer from the donor side via the intermediate heterocyclic bridge to the acceptor side. Finally, a comparison between CASTEP and MOPAC reveals that CASTEP is more appropriate and accurate in predicting the optical properties of the heterocyclic-ring-based derivatives.

Nonlinear optical phenomena associated with high-order soliton breakup in photonic crystal fibres and squeezed state generation in three dimensional photonic crystal microcavities are investigated. In both cases, the properties of periodically patterned, high-index contrast dielectric structures are engineered to control the dispersion and local field enhancements of the electromagnetic field. Ultra-short pulse propagation in a polarization-maintaining microstructured fibre (with 1 um core diameter and 1.1 m length) is investigated experimentally and theoretically. For an 80 MHz train of 130 fs pulses with average propagating powers in the fibre up to 13.8 mW, the output spectra consist of multiple discrete solitons that shift continuously to lower energies as they propagate in the lowest transverse mode of the fibre. The number of solitons and the amount that they shift both increase with the launched power. All of the data is quantitatively consistent with solutions of the nonlinear Schrodinger equation, but only when the Raman nonlinearity is treated without approximation, and self-steepening is included. The feasibility of using a parametric down-conversion process to generate squeezed electromagnetic states in 3D photonic crystal microcavity structures is investigated for the first time. The spectrum of the squeezed light is theoretically calculated by using an open cavity quantum mechanical formalism. The cavity communicates with two main channels, which model vertical radiation losses and coupling into a single-mode waveguide respectively. The amount of squeezing is determined by the correlation functions relating the field quadratures of light coupled into the waveguide. All of the relevant model parameters are realistically estimated using 3D finite-difference time-domain (FDTD) simulations. Squeezing up to ~20% below the shot noise level is predicted for reasonable optical excitation levels. To preserve the squeezed nature of the light generated in the microcavity, a unidirectional coupling geometry from the microcavity to a ridge waveguide in a slab photonic crystal structure is studied. The structure was successfully fabricated in a silicon membrane, and experimental measurements of the efficiency for the signal coupled out of the structure are in good agreement with the result of FDTD simulations. The coupling efficiency of the cavity mode to the output channel is ~60%.

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Coherent anti-Stokes Raman scattering (CARS) microscopy has developed rapidly and is opening the door to new types of experiments. This work describes the development of new laser sources for CARS microscopy and their use for different applications. It is specifically focused on multimodal nonlinear optical microscopy—the simultaneous combination of different imaging techniques. This allows us to address a diverse range of applications, such as the study of biomaterials, fluid inclusions, atherosclerosis, hepatitis C infection in cells, and ice formation in cells. For these applications new laser sources are developed that allow for practical multimodal imaging. For example, it is shown that using a single Ti:sapphire oscillator with a photonic crystal fiber, it is possible to develop a versatile multimodal imaging system using optimally chirped laser pulses. This system can perform simultaneous two photon excited fluorescence, second harmonic generation, and CARS microscopy. The versatility of the system is further demonstrated by showing that it is possible to probe different Raman modes using CARS microscopy simply by changing a time delay between the excitation beams. Using optimally chirped pulses also enables further simplification of the laser system required by using a single fiber laser combined with nonlinear optical fibers to perform effective multimodal imaging. While these sources are useful for practical multimodal imaging, it is believed that for further improvements in CARS microscopy sensitivity, new excitation schemes are necessary. This has led to the design of a new, high power, extended cavity oscillator that should be capable of implementing new excitation schemes for CARS microscopy as well as other techniques. Our interest in multimodal imaging has led us to other areas of research as well. For example, a fiber-coupling scheme for signal collection in the forward direction is demonstrated that allows for fluorescence lifetime imaging without significant temporal distortion. Also highlighted is an imaging artifact that is unique to CARS microscopy that can alter image interpretation, especially when using multimodal imaging. By combining expertise in nonlinear optics, laser development, fiber optics, and microscopy, we have developed systems and techniques that will be of benefit for multimodal CARS microscopy. / Thesis (Ph.D, Physics, Engineering Physics and Astronomy) -- Queen's University, 2011-08-11 13:46:26.065

Thesis (M. Phil.)--University of Hong Kong, 2008. / Also available in print.

Thesis (PhD) - Swinburne University of Technology, Faculty of Engineering and Industrial Sciences, Centre for Micro-Photonics, 2007. / A thesis submitted for the degree of Doctor of Philosophy, Centre for Micro-Photonics, Faculty of Engineering and Industrial Sciences, Swinburne University of Technology, 2007. Typescript. Bibliography: p. 146-162.

Thesis (M. Sc.)--Carleton University, 2003. / Includes bibliographical references. Also available in electronic format on the Internet.

Thesis (Ph. D.)--University of Washington, 2004. / Vita. Includes bibliographical references (p. 92-95).