Thesis (Ph. D.)--University of Hong Kong, 2000. / Includes bibliographical references (leaves 280-300).

Thesis (Ph. D. in Physics)--Vanderbilt University, Dec. 2006. / Title from title screen. Includes bibliographical references.

We present the results of a numerical simulation tool for modeling the second-harmonic generation (SHG) interaction experienced by a diffracting beam. This code is used to study the simultaneous frequency and spatial profile conversion of a truncated Bessel beam that closely resembles a higher-order mode (HOM) of an optical fiber. SHG with Bessel beams has been investigated in the past and was determined have limited value because it is less efficient than SHG with a Gaussian beam in the undepleted pump regime. This thesis considers, for the first time to the best of our knowledge, whether most of the power from a Bessel-like beam could be converted into a second-harmonic beam (full depletion), as is the case with a Gaussian beam. We study this problem because using HOMs for fiber lasers and amplifiers allows reduced optical intensities, which mitigates nonlinearities, and is one possible way to increase the available output powers of fiber laser systems. The chief disadvantage of using HOM fiber amplifiers is the spatial profile of the output, but this can be transformed as part of the SHG interaction, most notably to a quasi-Gaussian profile when the phase mismatch meets the noncollinear criteria. We predict, based on numerical simulation, that noncollinear SHG (NC-SHG) can simultaneously perform highly efficient (90%) wavelength conversion from 1064 nm to 532 nm, as well as concurrent mode transformation from a truncated Bessel beam to a Gaussian-like beam (94% overlap with a Gaussian) at modest input powers (250 W, peak power or continuous-wave operation). These simulated results reveal two attractive features – the feasibility of efficiently converting HOMs of fibers into Gaussian-like beams, and the ability to simultaneously perform frequency conversion. Combining the high powers that are possible with HOM fiber amplifiers with access to non-traditional wavelengths may offer significant advantages over the state of the art for many important applications, including underwater communications, laser guide stars, and theater projectors.

We study the behavior of electric fields in and around dielectric and metal nanoparticles, and prepare the ground for their applications to a variety of systems viz. photovoltaics, imaging and detection techniques, and molecular spectroscopy. We exploit the property of nanoparticles being able to focus the radiation field into small regions and study some of the interesting nonlinear, and quantum coherence and interference phenomena near them. The traditional approach to study the nonlinear light-matter interactions involves the use of the slowly varying amplitude approximation (SVAA) as it simplifies the theoretical analysis. However, SVVA cannot be used for systems which are of the order of the wavelength of the light. We use the exact solutions of the Maxwell's equations to obtain the fields created due to metal and dielectric nanoparticles, and study nonlinear and quantum optical phenomena near these nanoparticles. We begin with the theoretical description of the electromagnetic fields created due to the nonlinear wavemixing process, namely, second-order nonlinearity in an nonlinear sphere. The phase-matching condition has been revisited in such particles and we found that it is not satisfied in the sphere. We have suggested a way to obtain optimal conditions for any type and size of material medium. We have also studied the modifications of the electromagnetic fields in a collection of nanoparticles due to strong near field nonlinear interactions using the generalized Mie theory for the case of many particles applicable in photovoltaics (PV). We also consider quantum coherence phenomena such as modification of dark states, stimulated Raman adiabatic passage (STIRAP), optical pumping in $4$-level atoms near nanoparticles by using rotating wave approximation to describe the Hamiltonian of the atomic system. We also considered the behavior of atomic and the averaged atomic polarization in $7$-level atoms near nanoparticles. This could be used as a prototype to study any $n-$level atomic system experimentally in the presence of ensembles of quantum emitters. In the last chapter, we suggested a variant of a pulse-shaping technique applicable in stimulated Raman spectroscopy (SRS) for detection of atoms and molecules in multiscattering media. We used discrete-dipole approximation to obtain the fields created by the nanoparticles.

No description available.

No description available.

Quadratic spatial soliton interactions were investigated in this Dissertation. The first part deals with characterizing the principal features of multi-soliton generation and soliton self-reflection. The second deals with two beam processes leading to soliton interactions and collisions. These subjects were investigated both theoretically and experimentally. The experiments were performed by using potassium niobate (KNBO3) and periodically poled potassium titanyl phosphate (KTP) crystals. These particular crystals were desirable for these experiments because of their large nonlinear coefficients and, more importantly, because the experiments could be performed under non-critical-phase-matching (NCPM) conditions. The single soliton generation measurements, performed on KNBO3 by launching the fundamental component only, showed a broad angular acceptance bandwidth which was important for the soliton collisions performed later. Furthermore, at high input intensities multi-soliton generation was observed for the first time. The influence on the multi-soliton patterns generated of the input intensity and beam symmetry was investigated. The combined experimental and theoretical efforts indicated that spatial and temporal noise on the input laser beam induced multi-soliton patterns. Another research direction pursued was intensity dependent soliton routing by using of a specially engineered quadratically nonlinear interface within a periodically poled KTP sample. This was the first time demonstration of the self-reflection phenomenon in a system with a quadratic nonlinearity. The feature investigated is believed to have a great potential for soliton routing and manipulation by engineered structures. A detailed investigation was conducted on two soliton interaction and collision processes. Birth of an additional soliton resulting from a two soliton collision was observed and characterized for the special case of a non-planar geometry. A small amount of spiraling, up to 30 degrees rotation, was measured in the experiments performed. The parameters relevant for characterizing soliton collision processes were also studied in detail. Measurements were performed for various collision angles (from 0.2 to 4 degrees), phase mismatch, relative phase between the solitons and the distance to the collision point within the sample (which affects soliton formation). Both the individual and combined effects of these collision variables were investigated. Based on the research conducted, several all-optical switching scenarios were proposed.

Single-pass frequency conversion by a nonlinear optical crystal is an attractive method to generate coherent radiation in various spectral domains from ultraviolet to mid-infrared. Wavelength converters based on quasi-phase matched (QPM) periodically poled lithium niobate (PPLN) have proved to be important wavelength conversion devices for many useful applications. This thesis develops a novel integration design for temperature controlling and temperature wavelength tuning of a QPM-PPLN waveguide wavelength converter. A Cr/Pt/Au thin film alloy layer is deposited on a PPLN device with a polymer buffer layer to work as a micro-heater and a temperature sensor at the same time. The temperature of the device can be tailored by applying current to the micro-heater layer, which changes the effective period of the QPM grating and thus the QPM wavelength through the thermal optical effect (TOE). The device's temperature can be monitored by measuring the resistance change of the alloy layer. Micro-heater design and mode profile simulation are involved in the thesis. The entire device fabrication process is introduced. Both electrical and optical features of the device are characterized and discussed. In contrast to the conventional temperature tuning method based on a bulky oven, the proposed design has some excellent characteristics such as compact package size and low power consumption. / Thesis / Master of Applied Science (MASc)

In this thesis, detailed studies are presented into self-assembled, noncentrosymmetric, optically active films. Second harmonic generation (SHG) is used to measure the second order nonlinear optical susceptibility (?(2)) of ionically self-assembled monolayer (ISAM) thin films. Conventional ISAM films are fabricated by alternately immersing a substrate into oppositely-charged polyelectrolyte solutions. The polyelectrolytes bind electrostatically to the oppositely-charged substrate, and thus reverse the charge of the substrate. The charge reversal limits the amount of adsorbed material and primes the substrate for the next layer. During the deposition of the nonlinear optical (NLO) active layer, the chromophores are attracted to the oppositely-charged surface, which results in net orientation of the chromophores. Some of the net orientation is lost during the deposition of the next NLO-inactive layer as this layer orients some of the chromophores away from the substrate. A disadvantage of the polymer ISAM deposition method is that although there is a net orientation toward the substrate, a large number of chromophores are randomly or oppositely oriented. This reduces the nonlinear optical response. To overcome this problem, two alternative methods with a better net orientation are discussed: hybrid covalent / ionic deposition and multivalent monomer deposition. In both deposition methods, the NLO-active material is a monomer instead of a polymer. In hybrid covalent / ionic deposition, the NLO-inactive polymer is deposited using electrostatic attraction while the NLO-active monomer is deposited covalently. This forces alignment of the chromophores. The multivalent method uses chromophores with multiple charges on one side of the molecule and one charge (same sign) on the other. The difference in electrostatic attraction causes a preferential orientation of the chromophores during deposition. Attempts have been made to further improve the net orientation by complexation of the monomers with cyclodextrins (cone shaped organic molecules), so far with only limited success. The SHG response of NLO-active layers near the glass and air interfaces is much stronger than the SHG response of layers in the bulk of the film for all deposition methods and NLO-active materials investigated in this thesis. For larger number of bilayers (the bulk regime), the square root of the SHG signal increases linearly with the number of bilayers as expected for a uniform chromophore orientation. We isolated the interface effects through use of buffer layers of NLO-inactive polymers. The glass interface effect extends roughly one bilayer deep for all investigated materials. The air interface effect is different for polymers and monomers. For monomers, this effect extends only one bilayer deep, while it extends multiple layers deep for polymers. Using glass cells to contain the polyelectrolyte solutions, we were able to measure the SHG signal in situ, which proved to be a powerful tool to monitor the deposition rate as a function of chosen parameters. All depositions were rapid, on the order of one minute or less. Provided that a minimum concentration is met, the deposition rate and final SHG values are independent of concentration. Bulk layers deposit at the same rate as layers near the interface. For polymer NLO-active layers a secondary, slower growth of SHG is observed that is presumably due to reorganization of the adsorbed polymer layer. This secondary growth is not observed in the deposition of NLO-active monomers. / Ph. D.

Detailed studies are presented of thin films that self-assemble into the noncentrosymmetric structure required for second order nonlinear optical responses. Second harmonic generation is used as a probe of the second-order nonlinear optical susceptibility (c(2)) of ionic self-assembled monolayer (ISAM) films. Films produced from the ISAM technique are shown to possess significant c(2), with values presently comparable to quartz (c(2)=1.53*10⁹ esu). These films show exceptional stability over time, with negligible decrease in c(2) after 26 months. ISAM films self-assemble from polyelectrolyte solutions due to coulombic interactions between a charged substrate and the charged polymer in solution. This process is self-limiting since charge overcompensation at the surface restricts further deposition as like charges accumulate at the surface. We have found that this 'kinetically hindered equilibrium' occurs quickly for the samples studied, after approximately 45 seconds immersion. Non-centrosymmetry is obtained during deposition as chromophores orient towards the substrate as a strong, localized collection of opposite charge. This net orientation is partially diminished as some amount of chromophore extends in the opposite direction at the film/solution interface. Second harmonic measurements suggest that chromophores at the outermost interface collapse against the film surface when dried, resulting in a larger c(2) than other 'capped' layers. Any polymer which is not located at the interfaces is thought to possess random orientation, and therefore does not contribute to c(2). We have investigated how ionic strength and solution pH affect the structure of ISAM films. These parameters serve to control the electrostatic screening in solution. Low salt concentrations result in low or no electrostatic screening. As a result, charges on a polymer strongly feel one another's presence, and decrease the net electrostatic energy by maximizing their distance from each other. This results in a rod-like conformation, which when adsorbed onto the film surface produces thin layers. Large salt concentrations serve to screen the electrostatic interaction. Because charges do not experience the strong repulsion from their neighbors, the polymer backbone is more likely to loop and coil. If the polymer is weakly soluble (pH near the solubility edge), the polymer will loop about itself and other polymer chains in order to reduce the number of polymer/water contacts. Increased screening results in adsorption of thicker films. We show that this also results in a marginal increase in film density, likely due to an increase in polymer interpenetration of adjacent layers. We can associate an increase in chromophore population at the interface with this increase in density. The reduction in screening also is shown to decrease the chromophore orientation angle, presumably by decreasing the repulsion between charges located on the chromophore ends. The improved orientation leads to an increased non-centrosymmetry in the layer. c(2) is decreased, however, as film thickness (and therefore the population of randomly oriented chromophore between interfaces) increases faster than the improvements to non-centrosymmetry at the interface. We have investigated the thermal stability of ISAM films at elevated temperatures, and have found that these films do not exhibit a permanent decay of c(2) with increased temperature as do poled guest-host polymers. A temperature-dependent decrease is observed for temperatures up to 250°C. This decrease is completely reversible (for films heated to 150C), with c(2) recovering its initial value upon cooling in spite of a glass transition temperature measured as Tg=140°C The decrease in c(2) is thought to be due to a combination of effects. Predominant decrease is thought to be due to disassociation of ionic bonds, which serve to provide noncentrosymmetry in films. A slower, smaller decay due to decrease in moisture content of the films at high temperature is also thought to be present. / Ph. D.