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Title: Non-Reciprocal Wave Transmission in Integrated Waveguide Array Isolators.
Creator: Ho, Yat, Likamwa, Patrick, Christodoulides, Demetrios, Vanstryland, Eric, Kaup, David, University of Central Florida
Abstract / Description: Non-reciprocal wave transmission is a phenomenon witnessed in certain photonic devices when the wave propagation dynamics through the device along one direction differs greatly from the dynamics along the counter-propagating direction. Specifically, it refers to significant power transfer occurring in one direction, and greatly reduced power transfer in the opposite direction. The resulting effect is to isolate the directionality of wave propagation, allowing transmission to occur along one...
Show moreNon-reciprocal wave transmission is a phenomenon witnessed in certain photonic devices when the wave propagation dynamics through the device along one direction differs greatly from the dynamics along the counter-propagating direction. Specifically, it refers to significant power transfer occurring in one direction, and greatly reduced power transfer in the opposite direction. The resulting effect is to isolate the directionality of wave propagation, allowing transmission to occur along one direction only.Given the popularity of photonic integrated circuits (PIC), in which all the optical components are fabricated on the same chip so that the entire optical system can be made more compact, it is desirable to have an easily integrated optical isolator. Common free-space optical isolator designs, which rely on the Faraday effect, are limited by the availability of suitable magnetic materials. This research proposes a novel integrated optical isolator based on an array of closely spaced, identical waveguides. Because of the nonlinear optical properties of the material, this device exploits the differing behaviors of such an array when illuminated with either a high power or a low power beam to achieve non-reciprocal wave transmission in the forwards and backwards directions, respectively. The switching can be controlled electro-optically via an integrated gain section which provides optical amplification before the input to the array. The design, fabrication, characterization and testing of this optical isolator are covered in this dissertation. We study the switching dynamics of this device and present its optimum operating conditions. ?
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Date Issued: 2012
Identifier: CFE0004305, ucf:49495
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0004305

Title: NONLINEAR FEMTOSECOND NEAR INFRARED LASER STRUCTURING IN OXIDE GLASSES.
Creator: Royon, Arnaud, Richardson, Martin, University of Central Florida
Abstract / Description: Three-dimensional femtosecond laser structuring has a growing interest because of its ease of implementation and the numerous possible applications in the domain of photonic components. Structures such as waveguides, diffraction gratings, optical memories or photonic crystals can be fabricated thanks to this technique. Its use with oxide glasses is promising because of several advantages; they are resistant to flux and ageing, their chemical composition can easily be changed to fit the well...
Show moreThree-dimensional femtosecond laser structuring has a growing interest because of its ease of implementation and the numerous possible applications in the domain of photonic components. Structures such as waveguides, diffraction gratings, optical memories or photonic crystals can be fabricated thanks to this technique. Its use with oxide glasses is promising because of several advantages; they are resistant to flux and ageing, their chemical composition can easily be changed to fit the well-defined requirements of an application. They can already be found in Raman amplifiers, optical fibers, fiber lasers, and other devices. This thesis is based on two axes. The first axis consists in characterizing the linear and nonlinear optical properties of bulk vitreous materials in order to optimize their composition with a particular application in view. Within this context, the nonlinear optical properties, their physical origins (electronic and nuclear) as well as their characteristic response times (from a few femtoseconds to a few hundreds of picoseconds) are described within the Born-Oppenheimer approximation. Fused silica and several sodium-borophosphate glasses containing different concentrations in niobium oxide have been studied. Results show that the nonlinear optical properties of fused silica are mainly from electronic origin, whereas in the sodium-borophosphate glasses, the contribution from nuclear origin becomes predominant when the concentration of niobium oxide exceeds 30%. The second axis is based on the structuring of materials. Three commercially available fused silica samples presenting different fabrication conditions (therefore distinct impurity levels) and irradiated with a near infrared femtosecond laser have been studied. The laser induced defects have been identified by means of several spectroscopic techniques. They show the formation of color centers as well as a densification inside the irradiated area. Their linear refractive index and nonlinear third-order susceptibility properties have been measured. Moreover, the structuring of fused silica at the subwavelength scale into "nanogratings" is observed and the form of birefringence induced by these structures is discussed. In addition to the fused silica samples, several oxide glasses presenting very distinct chemical compositions have been studied. A sodium-borophosphate glass containing niobium oxide exhibits micro-cracks and nano-crystallites following irradiation. A silicate glass with or without a silver component reveals fluorescent rings or "nanograting" structures. A zinc phosphate glass containing silver also presents fluorescent ring structures, with a size of the order of 80 nm, well below the diffraction limit. Pump-probe microscope techniques have been performed on this glass to investigate the laser-glass interaction. The absorption mechanism is determined to be four-photon absorption. The generated free electron density is ~ 1017 cm-3, which suggests the conclusion that an electron gas rather than a plasma is formed during the laser irradiation.
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Date Issued: 2009
Identifier: CFE0002666, ucf:48200
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0002666

Title: Nano and nanostructured materials for optical applications.
Creator: Chantharasupawong, Panit, Thomas, Jayan, Hagan, David, Kik, Pieter, Gaume, Romain, Chanda, Debashis, University of Central Florida
Abstract / Description: Nano and nanostructured materials offer unique physical and chemical properties that differ considerably from their bulk counterparts. For decades, due to their fascinating properties, they have been extensively explored and found to be beneficial in numerous applications. These materials are key components in many cutting-edge optic and photonic technologies, including photovoltaics, waveguides and sensors. In this dissertation, the uses of nano and nanostructured materials for optical...
Show moreNano and nanostructured materials offer unique physical and chemical properties that differ considerably from their bulk counterparts. For decades, due to their fascinating properties, they have been extensively explored and found to be beneficial in numerous applications. These materials are key components in many cutting-edge optic and photonic technologies, including photovoltaics, waveguides and sensors. In this dissertation, the uses of nano and nanostructured materials for optical applications are investigated in the context of optical limiting, three dimensional displays, and optical sensing. Nanomaterials with nonlinear optical responses are promising candidates for self-activating optical limiters. In the first part of this study, optical limiting properties of unexplored nanomaterials are investigated. A photoacoustic detection technique is developed as an alternative characterization method for studying optical nonlinearities. This was done with an indigenously developed setup for measuring the photoacoustic signals generated from samples excited with a pulse laser. A theoretical model for understanding the experimental observations is presented. In addition, the advantages of this newly developed technique over the existing methods are demonstrated. Blending optical sensitizers with photoconducting polymers and chromophores results in a polymer composite that is able to record a light grating. This composite can be used as recording media in 3D holographic display technology. Here, 2D nano materials, like graphenes, are used as optical sensitizers to improve the response time of a photorefractive polymer. The addition of graphenes to a PATPD/ECZ/7-DCST composite results in a three-fold enhancement in response time and therefore faster recording speed of the medium. The faster build-up time is attributed to better charge generation and mobility due to the presence of graphenes in the composite. Lastly, a facile nanofabrication technique is developed to produce metallic nanostructures with a tunable plasmonic response. The enhancement of the light-matter interactions due to these nanostructures in sensing an analyte is demonstrated.
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Date Issued: 2015
Identifier: CFE0006029, ucf:51016
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0006029

Title: Two-photon absorption in bulk semiconductors and quantum well structures and its applications.
Creator: Pattanaik, Himansu, Vanstryland, Eric, Hagan, David, Delfyett, Peter, Schoenfeld, Winston, Peale, Robert, University of Central Florida
Abstract / Description: The purpose of this dissertation is to provide a study and possible applications of two-photon absorption (2PA), in direct-gap semiconductors and quantum-well (QW) semiconductor structures. One application uses extremely nondegenerate (END) 2PA, for mid-infrared (mid-IR) detection in uncooled semiconductors. The use of END, where the two photons have very different energies gives strong enhancement comapared to degenerate 2PA. This END-2PA enhanced detection is also applied to mid-IR imaging...
Show moreThe purpose of this dissertation is to provide a study and possible applications of two-photon absorption (2PA), in direct-gap semiconductors and quantum-well (QW) semiconductor structures. One application uses extremely nondegenerate (END) 2PA, for mid-infrared (mid-IR) detection in uncooled semiconductors. The use of END, where the two photons have very different energies gives strong enhancement comapared to degenerate 2PA. This END-2PA enhanced detection is also applied to mid-IR imaging and light detection and ranging (LIDAR) in uncooled direct-gap photodiodes. A theoretical study of degenerate 2PA (D-2PA) in quantum wells, QWs, is presented, along with a new theory of ND 2PA in QWs is developed. Pulsed mid-IR detection of femtosecond pulses is investigated in two different semiconductor p-i-n photodiodes (GaAs and GaN). With the smaller gap materials having larger ND-2PA, it is observed that they have better sensitivity to mid-IR detection, but unwanted background from D-2PA outweighs this advantage. A comparison of responsivity and signal-to-background ratio for GaAs and GaN in END-2PA based detection is presented. END-2PA enhancement is utilized for CW IR detection in uncooled GaAs and GaN p-i-n photodiodes. The pulsed mid-IR detection experiments are further extended to perform mid-IR imaging in uncooled GaN p-i-n photodetectors. A 3-D automated scanning gated imaging system is developed to obtain 3-D mid-IR images of various objects. The gated imaging system allows simultaneous 3-D and 2-D imaging of objects. The 3-D gated imaging system described in the dissertation could be used for examination of buried structures (microchannels, defects etc.) or laser written volumetric structures and could also be suitable for in-vivo imaging applications in biology in the mid-IR spectral region. As an example, 3-D imaging of buried semiconductor structures is presented.A theoretical study of D-2PA of QWs for transverse electric (TE) and transverse magnetic (TM) fields is carried out and an analytical expression for the D-2PA coefficient in QWs using second-order perturbation theory is derived. A theory for ND-2PA in QW semiconductor using second-order perturbation theory is developed for the first time and an analytical expression for the ND-2PA coefficient for TE, TM, and the mixed case of TE and TM is derived. The shape of the 2PA curve for the D-2PA and ND-2PA for QWs in the TE case is similar to that of bulk semiconductors. As governed by the selection rules both the D-2PA and ND-2PA curves for the TE case does not show a step-like signature for the density of states of the QWs whereas 2PA curve for the TM case shows such step like sharp features. The ND-2PA coefficient for TE, TM, and the mixed case is compared with that obtained for bulk semiconductors. Large enhancement in ND-2PA of QW semiconductors for the TM case over bulk semiconductors is predicted.
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Date Issued: 2015
Identifier: CFE0005684, ucf:50164
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0005684

Title: CHEMICAL STRUCTURE - NONLINEAR OPTICAL PROPERTY RELATIONSHIPS FOR A SERIES OF TWO-PHOTON ABSORBING FLUORENE MOLECULES.
Creator: Hales, Joel McCajah, Van Stryland, Eric W., University of Central Florida
Abstract / Description: This dissertation reports on the investigation of two-photon absorption (2PA) in a series of fluorenyl molecules. Several current and emerging technologies exploit this optical nonlinearity including two-photon fluorescence imaging, three-dimensional microfabrication, site-specific photodynamic cancer therapy and biological caging studies. The two key features of this nonlinearity which make it an ideal candidate for the above applications are its quadratic dependence on the incident...
Show moreThis dissertation reports on the investigation of two-photon absorption (2PA) in a series of fluorenyl molecules. Several current and emerging technologies exploit this optical nonlinearity including two-photon fluorescence imaging, three-dimensional microfabrication, site-specific photodynamic cancer therapy and biological caging studies. The two key features of this nonlinearity which make it an ideal candidate for the above applications are its quadratic dependence on the incident irradiance and the improved penetration into absorbing media that it affords. As a consequence of the burgeoning field which exploits 2PA, it is a goal to find materials that exhibit strong two-photon absorbing capabilities. Organic materials are promising candidates for 2PA applications because their material properties can be tailored through molecular engineering thereby facilitating optimization of their nonlinear optical properties. Fluorene derivatives are particularly interesting since they possess high photochemical stability for organic molecules and are generally strongly fluorescent. By systematically altering the structural properties in a series of fluorenyl molecules, we have determined how these changes affect their two-photon absorbing capabilities. This was accomplished through characterization of both the strength and location of their 2PA spectra. In order to ensure the validity of these results, three separate nonlinear characterization techniques were employed: two-photon fluorescence spectroscopy, white-light continuum pump-probe spectroscopy, and the Z-scan technique. In addition, full linear spectroscopic characterization was performed on these molecules along with supplementary quantum chemical calculations to obtain certain molecular properties that might impact the nonlinearity. Different designs in chemical architecture allowed investigation of the effects of symmetry, solvism, donor-acceptor strengths, conjugation length, and multi-branched geometries on the two-photon absorbing properties of these molecules. In addition, the means to enhance 2PA via intermediate state resonances was investigated. To provide plausible explanations for the experimentally observed trends, a conceptually simple three level model was employed. The subsequent correlations found between chemical structure and the linear and nonlinear optical properties of these molecules provided definitive conclusions on how to properly optimize their two-photon absorbing capabilities. The resulting large nonlinearities found in these molecules have already shown promise in a variety of the aforementioned applications.
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Date Issued: 2004
Identifier: CFE0000005, ucf:46103
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0000005

Title: 2 micron fiber lasers: power scaling concepts and limitations.
Creator: Sincore, Alex, Richardson, Martin, Amezcua Correa, Rodrigo, Schulzgen, Axel, Shah, Lawrence, University of Central Florida
Abstract / Description: Thulium- and holmium-doped fiber lasers (TDF and HDF) emitting at 2 micron offer unique benefits and applications compared to common ytterbium-doped 1 micron lasers. This dissertation details the concepts, limitations, design, and performance of four 2 micron fiber laser systems. While these lasers were developed for various end-uses, they also provide further insight into two major power scaling limitations. The first limitation is optical nonlinearities: specifically stimulated Brillouin...
Show moreThulium- and holmium-doped fiber lasers (TDF and HDF) emitting at 2 micron offer unique benefits and applications compared to common ytterbium-doped 1 micron lasers. This dissertation details the concepts, limitations, design, and performance of four 2 micron fiber laser systems. While these lasers were developed for various end-uses, they also provide further insight into two major power scaling limitations. The first limitation is optical nonlinearities: specifically stimulated Brillouin scattering (SBS) and modulation instability (MI). The second limitation is thermal failure due to inefficient pump conversion. First, a 21.5 W single-frequency, single-mode laser with adjustable output from continuous-wave to nanosecond pulses is developed. Measuring the SBS threshold versus pulse duration enables the Brillouin gain coefficient and gain bandwidth to be determined at 2 micron. Second, a 23 W spectrally-broadband, nanosecond pulsed laser is constructed for materials processing applications. The temporally incoherent multi-kW peak power pulses can also efficiently produce MI and supercontinuum generation by adjusting the input spectral linewidth. Third, the measured performance of in-band pumped TDF and HDF lasers are compared with simulations. HDF displays low efficiencies, which is explained by including ion clustering in the simulations. The TDF operates with impressive (>)90% slope efficiencies. Based on this result, a system design for (>)1 kW average power TDF amplifier is described. The designed final amplifier will be in-band pumped to enable high efficiency and low thermal load. The amplifier efficiency, operating bandwidth, thermal load, and nonlinear limits are modeled and analyzed to provide a framework for execution. Overall, this dissertation provides further insight and understanding on the various processes that limit power scaling of 2 micron fiber lasers.
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Date Issued: 2018
Identifier: CFE0007374, ucf:52105
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0007374

Title: Particle Manipulation Via Optical Forces and Engineering Soft-Matter Systems With Tunable Nonlinearities.
Creator: Fardad, Shima, Christodoulides, Demetrios, Hagan, David, Amezcua Correa, Rodrigo, Likamwa, Patrick, Chen, Zhigang, University of Central Florida
Abstract / Description: One of the most intriguing properties of light-matter interaction is the ability of an electromagnetic field to exert mechanical forces on polarizable objects. This phenomenon is a direct consequence of the fact that light carries momentum, which in turn can be transferred to matter. Mediated by scattering, this interaction usually manifests itself as a (")pushing force(") in the direction of beam propagation. However, it is possible to judiciously engineer these optical forces, either by...
Show moreOne of the most intriguing properties of light-matter interaction is the ability of an electromagnetic field to exert mechanical forces on polarizable objects. This phenomenon is a direct consequence of the fact that light carries momentum, which in turn can be transferred to matter. Mediated by scattering, this interaction usually manifests itself as a (")pushing force(") in the direction of beam propagation. However, it is possible to judiciously engineer these optical forces, either by tailoring particle polarizability, and/or by structuring the incident light field. As a simple example, a tightly focused laser beam demonstrates strong gradient forces, which may attract and even trap particles with positive polarizability in the focal volume. The opposite occurs in the regime of negative polarizability, where particles are expelled from the regions of highest intensity. Based on this fundamental principle, one can actively shape the beam using spatial light modulators to manipulate individual objects as well as ensembles of particles suspended in a liquid. In the latter case, a modulation of the local particle concentration is associated with changes of the effective refractive index. The result is an artificial nonlinear medium, whose Kerr-type response can be readily tuned by the parameters of its constituent particles.In the course of this work, we introduce a new class of synthetic colloidal suspensions exhibiting negative polarizabilities, and observe for the first time robust propagation and enhanced transmission of self-trapped light over long distances. Such light penetration in strongly scattering environments is enabled by the interplay between optical forces and self-activated transparency effects. We explore various approaches to the design of negative-polarizability arrangements, including purely dielectric as well as metallic and hybrid nanoparticles. In particular, we find that plasmonic resonances allow for extremely high and spectrally tunable polarizabilities, leading to unique nonlinear light-matter interactions. Here, for the first time we were able to observe plasmonic resonant solitons over more than 25 diffraction lengths, in colloidal nanosuspensions.
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Date Issued: 2014
Identifier: CFE0005610, ucf:50239
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0005610

Title: EXPERIMENTAL AND THEORETICAL APPROACHES TO CHARACTERIZATION OF ELECTRONIC NONLINEARITIES IN DIRECT-GAP SEMICONDUCTORS.
Creator: Cirloganu, Claudiu, Van Stryland, Eric, University of Central Florida
Abstract / Description: The general goal of this dissertation is to provide a comprehensive description of the limitations of established theories on bound electronic nonlinearities in direct-gap semiconductors by performing various experiments on wide and narrow bandgap semiconductors along with developing theoretical models. Nondegenerate two-photon absorption (2PA) is studied in several semiconductors showing orders of magnitude enhancement over the degenerate counterpart. In addition, three-photon absorption ...
Show moreThe general goal of this dissertation is to provide a comprehensive description of the limitations of established theories on bound electronic nonlinearities in direct-gap semiconductors by performing various experiments on wide and narrow bandgap semiconductors along with developing theoretical models. Nondegenerate two-photon absorption (2PA) is studied in several semiconductors showing orders of magnitude enhancement over the degenerate counterpart. In addition, three-photon absorption (3PA) is studied in ZnSe and other semiconductors and a new theory using a Kane 4-band model is developed which fits new data well. Finally, the narrow gap semiconductor InSb is studied with regard to multiphoton absorption, free-carrier nonlinearities and decay mechanisms. The non-degenerate two-photon absorption was investigated in several direct-gap semiconductors with picosecond and femtosecond pulses. Large enhancements in 2PA were demonstrated when employing highly non-degenerate photon pairs and the results were shown to be consistent to a simple 2-parabolic band theory based on a Ã‚Â"dressedÃ‚Â" state approach. The nonlinear refractive index induced in such configurations was also calculated and possible implications of such extreme behavior are discussed. A large number of measurements of 3PA were taken at multiple wavelengths and in several semiconductors. The subsequent analysis has shown that simple 2-band model calculations (based on either perturbative or tunneling approaches) do not adequately describe the experimental trends. A more comprehensive model, based on KaneÃ‚Â's 4-band theory was developed and we calculate three-photon spectra for zincblende structures within the perturbative framework. We have confirmed the results of our calculations performing a series of Z-scans in semiconductors ZnSe and ZnS, yielding complete experimental three-photon spectra. A systematic approach based on using a large variety of pulse durations was needed to quantify the wealth of nonlinear optical processes in InSb, accessible in the mid-infrared range. Femtosecond pulses provided a lower limit to measurements of the instantaneous effects (absorptive and refractive), while picosecond pulses allowed further characterization of the free-carrier effects, including population dynamics in the high density regime (Auger effects). The model developed permitted us to verify the temperature dependence of free-carrier absorption recently predicted, and to successfully model optical limiting data with longer, nanosecond pulses.
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Date Issued: 2010
Identifier: CFE0003401, ucf:48417
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0003401

Title: White Light Continuum for Broadband Nonlinear Spectroscopy.
Creator: Ensley, Trenton, Hagan, David, Vanstryland, Eric, Zeldovich, Boris, Christodoulides, Demetrios, Schulte, Alfons, University of Central Florida
Abstract / Description: Supercontinuum (SC) generation, oftentimes referred to as white-light continuum (WLC), has been a subject of interest for more than 40 years. From the first observation of WLC in condensed media in the early 1970s to the first observation of WLC in gases in the mid-1980s, much work has been devoted to developing a framework for understanding the complex nature of this phenomenon as well as discovering its utility in various applications. The main effort of this dissertation is to develop a...
Show moreSupercontinuum (SC) generation, oftentimes referred to as white-light continuum (WLC), has been a subject of interest for more than 40 years. From the first observation of WLC in condensed media in the early 1970s to the first observation of WLC in gases in the mid-1980s, much work has been devoted to developing a framework for understanding the complex nature of this phenomenon as well as discovering its utility in various applications. The main effort of this dissertation is to develop a WLC for the purpose of broadband nonlinear spectroscopy and use it in spectroscopic measurements. The ability to generate a high-quality, high-spectral-irradiance source of radiation confined in a single beam that spans the visible and near-infrared spectral regimes has great utility for nonlinear measurement methods such as the Z-scan technique. Using a broadband WLC instead of conventional tunable sources of radiation such as optical parametric generators/amplifiers has been shown to increase the efficiency of such measurements by nearly an order of magnitude. Although WLC generation has many complex processes involved, and complete models of the process involve highly complex numerical modeling, simple models can still guide us in the optimization of systems for WLC generation. In this dissertation the effects of two key mechanisms behind WLC generation in gaseous media are explored: self-phase modulation (SPM) and ionization leading to plasma production. The effects of SPM are largely dependent upon the third-order nonlinear refractive index, n2, of the gaseous medium whereas the effects of plasma production are dependent upon many parameters including the initial number density, ionization potential/energy, and the rate of ionization production. It is found that in order to generate a stable WLC suitable for nonlinear spectroscopy, the phase contributions from SPM and plasma production should be nearly equal. This guided our experiments in inert gases using mJ level, 150 fs-FWHM (full-width at half-maximum) pulses at 780 nm as well as 40 fs-FWHM pulses primarily at 1800 nm to create a stable, high-spectral-irradiance WLC. The generated WLC is shown to have sufficient spectral energy and spatial quality suitable for nonlinear spectroscopic measurements. In addition to extending the WLC bandwidth by using a long wavelength (1800 nm) pump source, it is found that by using a secondary weak seed pulse with a peak irradiance three orders of magnitude less than the main pulse, the spectral energy density is enhanced by more than a factor of 3 in Krypton gas for a WLC spectrum that spans over 2 octaves. Numerical simulations are presented which qualitatively describe the experimental results. The spectral enhancement of the WLC by seeding is also demonstrated for other inert gases and condensed media. Other efforts described in this dissertation include the development of the Dual-Arm Z-scan technique and its extension to measuring thin film nonlinearities in the presence of large substrate signals as well as predicting the n2 spectra of organic molecules (where we can approximate their behavior as if they were centrosymmetric) from knowledge of the one-photon and two-photon absorption spectra using a simplified sum-over-states quantum perturbative model by utilizing a quasi 3-level and quasi 4-level system.
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Date Issued: 2015
Identifier: CFE0005608, ucf:50264
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0005608

Title: Third-order optical nonlinearities for integrated microwave photonics applications.
Creator: Malinowski, Marcin, Fathpour, Sasan, Delfyett, Peter, Christodoulides, Demetrios, Lyakh, Arkadiy, University of Central Florida
Abstract / Description: The field of integrated photonics aims at compressing large and environmentally-sensitive opticalsystems to micron-sized circuits that can be mass-produced through existing semiconductor fabri-cation facilities. The integration of optical components on single chips is pivotal to the realizationof miniature systems with high degree of complexity. Such novel photonic chips find abundant ap-plications in optical communication, spectroscopy and signal processing. This work concentrateson...
Show moreThe field of integrated photonics aims at compressing large and environmentally-sensitive opticalsystems to micron-sized circuits that can be mass-produced through existing semiconductor fabri-cation facilities. The integration of optical components on single chips is pivotal to the realizationof miniature systems with high degree of complexity. Such novel photonic chips find abundant ap-plications in optical communication, spectroscopy and signal processing. This work concentrateson harnessing nonlinear phenomena to this avail.The first part of this dissertation discusses, both from component and system level, the developmentof a frequency comb source with a semiconductor mode-locked laser at its heart. New nonlinear de-vices for supercontinuum and second-harmonic generations are developed and their performance isassessed inside the system. Theoretical analysis of a hybrid approach with synchronously-pumpedKerr cavity is also provided. The second part of the dissertation investigates stimulated Brillouinscattering (SBS) in integrated photonics. A fully-tensorial open-source numerical tool is developedto study SBS in optical waveguides composed of crystalline materials, particularly silicon. SBS isdemonstrated in an all-silicon optical platform.
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Date Issued: 2019
Identifier: CFE0007674, ucf:52497
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0007674

Title: Hybrid integration of second- and third-order highly nonlinear waveguides on silicon substrates.
Creator: Camacho Gonzalez, Guillermo Fernando, Fathpour, Sasan, Likamwa, Patrick, Amezcua Correa, Rodrigo, Peale, Robert, University of Central Florida
Abstract / Description: In order to extend the capabilities and applications of silicon photonics, other materials and compatible technologies have been developed and integrated on silicon substrates. A particular class of integrable materials are those with high second- and third-order nonlinear optical properties. This work presents contributions made to nonlinear integrated photonics on silicon substrates, including chalcogenide waveguides for over an octave supercontinuum generation, and rib-loaded thin-film...
Show moreIn order to extend the capabilities and applications of silicon photonics, other materials and compatible technologies have been developed and integrated on silicon substrates. A particular class of integrable materials are those with high second- and third-order nonlinear optical properties. This work presents contributions made to nonlinear integrated photonics on silicon substrates, including chalcogenide waveguides for over an octave supercontinuum generation, and rib-loaded thin-film lithium niobate waveguides for highly efficient second-harmonic generation. Through the pursuit of hybrid integration of the two types of waveguides for applications such as on-chip self-referenced optical frequency combs, we have experimentally demonstrated fabrication integrability of chalcogenide and thin-film lithium niobate waveguides in a single chip and a pathway for both second- and third-order nonlinearities occurring therein. Accordingly, design specifications for an efficient nonlinear integrated waveguide are reported, showing over an octave supercontinuum generation and frequency selectivity for second-harmonic generation, enabling potentials of on-chip interferometry techniques for carrier-envelope offset detection, and hence stabilized optical combs.
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Date Issued: 2019
Identifier: CFE0007607, ucf:52560
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0007607

Title: NONLINEAR OPTICAL PROPERTIES OF ORGANIC CHROMOPHORES CALCULATED WITHIN TIME DEPENDENT DENSITY FUNCTIONAL THEORY.
Creator: Tafur, Sergio, Kokoouline, Viatcheslav, University of Central Florida
Abstract / Description: Time Dependent Density Functional Theory offers a good accuracy/computational cost ratio among different methods used to predict the electronic structure for molecules of practical interest. The Coupled Electronic Oscillator (CEO) formalism was recently shown to accurately predict Nonlinear Optical (NLO) properties of organic chromophores when combined with Time Dependent Density Functional Theory. Unfortunately, CEO does not lend itself easily to interpretation of the structure activity...
Show moreTime Dependent Density Functional Theory offers a good accuracy/computational cost ratio among different methods used to predict the electronic structure for molecules of practical interest. The Coupled Electronic Oscillator (CEO) formalism was recently shown to accurately predict Nonlinear Optical (NLO) properties of organic chromophores when combined with Time Dependent Density Functional Theory. Unfortunately, CEO does not lend itself easily to interpretation of the structure activity relationships of chromophores. On the other hand, the Sum Over States formalism in combination with semiempirical wavefunction methods has been used in the past for the design of simplified essential states models. These models can be applied to optimization of NLO properties of interest for applications. Unfortunately, TD-DFT can not be combined directly with SOS because state-to-state transition dipoles are not defined in the linear response TD approach. In this work, a second order CEO approach to TD-DFT is simplified so that properties of double excited states and state-to-state transition dipoles may be expressed through the combination of linear response properties. This approach is termed the a posteriori Tamm-Dancoff approximation (ATDA), and validated against high-level wavefunction theory methods. Sum over States (SOS) and related Two-Photon Transition Matrix formalism are then used to predict Two-Photon Absorption (2PA) profiles and anisotropy, as well as Second Harmonic Generation (SHG) properties. Numerical results for several conjugated molecules are in excellent agreement with CEO and finite field calculations, and reproduce experimental measurements well.
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Date Issued: 2007
Identifier: CFE0001853, ucf:47372
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0001853

Title: Quantum Chemical Studies for the Engineering of Metal Organic Materials.
Creator: Rivera Jacquez, Hector, Masunov, Artem, Balaeff, Alexander, Harper, James, Heider, Emily, Zou, Shengli, Kaden, William, University of Central Florida
Abstract / Description: Metal Organic Materials (MOM) are composed of transition metal ions as connectors and organic ligands as linkers. MOMs have been found to have high porosity, catalytic, and optical properties. Here we study the gas adsorption, color change, and non-linear optical properties of MOMs. These properties can be predicted using theoretical methods, and the results may provide experimentalists with guidance for rational design and engineering of novel MOMs. The theory levels used include semi...
Show moreMetal Organic Materials (MOM) are composed of transition metal ions as connectors and organic ligands as linkers. MOMs have been found to have high porosity, catalytic, and optical properties. Here we study the gas adsorption, color change, and non-linear optical properties of MOMs. These properties can be predicted using theoretical methods, and the results may provide experimentalists with guidance for rational design and engineering of novel MOMs. The theory levels used include semi-empirical quantum mechanical calculations with the PM7 Hamiltonian and, Density Functional Theory (DFT) to predict the geometry and electronic structure of the ground state, and Time Dependent DFT (TD-DFT) to predict the excited states and the optical properties.The molecular absorption capacity of aldoxime coordinated Zn(II) based MOMs (previously measured experimentally) is predicted by using PM7 Theory level. The 3D structures were optimized with and without host molecules inside the pores. The absorption capacity of these crystals was predicted to be 8H2 or 3N2 per unit cell. When going beyond this limit, the structural integrity of the bulk material becomes fractured and microcrystals are observed both experimentally and theoretically.The linear absorption properties of Co(II) based complexes are known to change color when the coordination number is altered. In order to understand the mechanism of this color change TD-DFT methods are employed. The chromic behavior of the Co(II) based complexes studied was confirmed to be due to a chain in coordination number that resulted in lower metal to ligand distances. These distances destabilize the occupied metal d orbitals, and as a consequence of this, the metal to ligand transition energy is lowered enough to allow the crystals to absorb light at longer wavelengths.Covalent organic frameworks (COFs) present an extension of MOM principles to the main group elements. The synthesis of ordered COFs is possible by using predesigned structures andcarefully selecting the building blocks and their conditions for assembly. The crystals formed by these systems often possess non-linear optical (NLO) properties. Second Harmonic Generation (SHG) is one of the most used optical processes. Currently, there is a great demand for materials with NLO optical properties to be used for optoelectronic, imaging, sensing, among other applications. DFT calculations can predict the second order hyperpolarizability ?2 and tensor components necessary to estimate NLO. These calculations for the ?2 were done with the use of the Berry's finite field approach. An efficient material with high ?2 was designed and the resulting material was predicted to be nearly fivefold higher than the urea standard.Two-photon absorption (2PA) is another NLO effect. Unlike SHG, it is not limited to acentric material and can be used development of in vivo bio-imaging agents for the brain. Pt(II) complexes with porphyrin derivatives are theoretically studied for that purpose. The mechanism of 2PA enhancement was identified. For the most efficient porphyrin, the large 2PA cross-section was found to be caused by a HOMO-LUMO+2 transition. This transition is strongly coupled to 1PA allowed Q-band HOMO-LUMO states by large transition dipoles. Alkyl carboxyl substituents delocalize the LUMO+2 orbital due to their strong ?-acceptor effect, enhancing transition dipoles and lowering the 2PA transition to the desirable wavelengths range.The mechanism 2PA cross-section enhancement of aminoxime and aldoxime ligands upon metal addition of is studied with TD-DFT methods. This mechanism of enhancement is found to be caused by the polarization of the ligand orbitals by the metal cation. After polarization an increase in ligand to ligand transition dipole moment. This enhancement of dipole moment is related to the increase in 2PA cross-sections.
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Date Issued: 2015
Identifier: CFE0005990, ucf:50777
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0005990

Title: Prediction of Optical Properties of Pi-Conjugated Organic Materials for Technological Innovations.
Creator: Nayyar, Iffat, Masunov, Artem, Saha, Haripada, Stolbov, Sergey, Gesquiere, Andre, University of Central Florida
Abstract / Description: Organic ?-conjugated solids are promising candidates for new optoelectronic materials. The large body of evidence points at their advantageous properties such as high charge-carrier mobility, large nonlinear polarizability, mechanical flexibility, simple and low cost fabrication and superior luminescence. They can be used as nonlinear optical (NLO) materials with large two-photon absorption (2PA) and as electronic components capable of generating nonlinear neutral (excitonic) and charged ...
Show moreOrganic ?-conjugated solids are promising candidates for new optoelectronic materials. The large body of evidence points at their advantageous properties such as high charge-carrier mobility, large nonlinear polarizability, mechanical flexibility, simple and low cost fabrication and superior luminescence. They can be used as nonlinear optical (NLO) materials with large two-photon absorption (2PA) and as electronic components capable of generating nonlinear neutral (excitonic) and charged (polaronic) excitations. In this work, we investigate the appropriate theoretical methods used for the (a) prediction of 2PA properties for rational design of organic materials with improved NLO properties, and (b) understanding of the essential electronic excitations controlling the energy-transfer and charge-transport properties in organic optoelectronics. Accurate prediction of these electro-optical properties is helpful for structure-activity relationships useful for technological innovations.In Chapter 1 we emphasize on the potential use of the organic materials for these two applications. The 2PA process is advantageous over one-photon absorption for deep-tissue fluorescence microscopy, photodynamic therapy, microfabrication and optical data storage owing to the three-dimensional spatial selectivity and improved penetration depth in the absorbing or scattering media. The design of the NLO materials with large 2PA cross-sections may reduce the optical damage due to the use of the high intensity laser beams for excitation. The organic molecules also possess self-localized excited states which can decay radiatively or nonradiatively to form excitonic states. This suggests the use of these materials in the electroluminescent devices such as light-emitting diodes and photovoltaic cells through the processes of exciton formation or dissociation, respectively. It is therefore necessary to understand ultrafast relaxation processes required in understanding the interplay between the efficient radiative transfer between the excited states and exciton dissociation into polarons for improving the efficiency of these devices. In Chapter 2, we provide the detailed description of the various theoretical methods applied for the prediction as well as the interpretation of the optical properties of a special class of substituted PPV [poly (p-phenylene vinylene)] oligomers. In Chapter 3, we report the accuracy of different second and third order time dependent density functional theory (TD-DFT) formalisms in prediction of the 2PA spectra compared to the experimental measurements for donor-acceptor PPV derivatives. We recommend a posteriori Tamm-Dancoff approximation method for both qualitative and quantitative analysis of 2PA properties. Whereas, Agren's quadratic response methods lack the double excitations and are not suitable for the qualitative analysis of the state-specific contributions distorting the overall quality of the 2PA predictions. We trace the reasons to the artifactual excited states above the ionization threshold. We also study the effect of the basis set, geometrical constraints and the orbital exchange fraction on the 2PA excitation energies and cross-sections. Higher exchange (BMK and M05-2X) and range-separated (CAM-B3LYP) hybrid functionals are found to yield inaccurate predictions both quantitatively and qualitatively. The failure of the exchange-correlation (XC) functionals with correct asymptotic is traced to the inaccurate transition dipoles between the valence states, where functionals with low HF exchange succeed. In Chapter 4, we test the performance of different semiempirical wavefunction theory methods for the prediction of 2PA properties compared to the DFT results for the same set of molecules. The spectroscopic parameterized (ZINDO/S) method is relatively better than the general purpose parameterized (PM6) method but the accuracy is trailing behind the DFT methods. The poor performances of PM6 and ZINDO/S methods are attributed to the incorrect description of excited-to-excited state transition and 2PA energies, respectively. The different semiempirical parameterizations can at best be used for quantitative analysis of the 2PA properties. The ZINDO/S method combined with different orders of multi-reference configuration interactions provide an improved description of 2PA properties. However, the results are observed to be highly dependent on the specific choice for the active space, order of excitation and reference configurations.In Chapter 5, we present a linear response TD-DFT study to benchmark the ability of existing functional models to describe the extent of self-trapped neutral and charged excitations in PPV and its derivative MEH-PPV considered in their trans-isomeric forms. The electronic excitations in question include the lowest singlet (S1) and triplet (T1†) excitons, positive (P+) and negative (P-) polarons and the lowest triplet (T1) states. Use of the long-range-corrected DFT functional, such as LC-wPBE, is found to be crucial in order to predict the physically correct spatial localization of all the electronic excitations in agreement with experiment. The inclusion of polarizable dielectric environment play an important role for the charged states. The particle-hole symmetry is preserved for both the polymers in trans geometries. These studies indicate two distinct origins leading to self-localization of electronic excitations. Firstly, distortion of molecular geometry may create a spatially localized potential energy well where the state wavefunction self-traps. Secondly, even in the absence of geometric and vibrational dynamics, the excitation may become spatially confined due to energy stabilization caused by polarization effects from surrounding dielectric medium.In Chapter 6, we aim to separate these two fundamental sources of spatial localization. We observe the electronic localization of P+ and P- is determined by the polarization effects of the surrounding media and the character of the DFT functional. In contrast, the self-trapping of the electronic wavefunctions of S1 and T1(T1†) mostly follows their lattice distortions. Geometry relaxation plays an important role in the localization of the S1 and T1† excitons owing to the non-variational construction of the excited state wavefunction. While, mean-field calculated P+, P- and T1 states are always spatially localized even in ground state S0 geometry. Polaron P+ and P- formation is signified by the presence of the localized states for the hole or the electron deep inside the HOMO-LUMO gap of the oligomer as a result of the orbital stabilization at the LC-wPBE level. The broadening of the HOMO-LUMO band gap for the T1 exciton compared to the charged states is associated with the inverted bond length alternation observed at this level. The molecular orbital energetics are investigated to identify the relationships between state localization and the corresponding orbital structure.In Chapter 7, we investigate the effect of various conformational defects of trans and cis nature on the energetics and localization of the charged P+ and P- excitations in PPV and MEH-PPV. We observe that the extent of self-trapping for P+ and P- polarons is highly sensitive on molecular and structural conformations, and distribution of atomic charges within the polymers. The particle-hole symmetry is broken with the introduction of trans defects and inclusion of the polarizable environment in consistent with experiment. The differences in the behavior of PPV and MEH-PPV is rationalized based on their orbital energetics and atomic charge distributions. We show these isomeric defects influence the behavior and drift mobilities of the charge carriers in substituted PPVs.
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Date Issued: 2013
Identifier: CFE0005110, ucf:50722
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0005110

Title: Engineering and Application of Ultrafast Laser Pulses and Filamentation in Air.
Creator: Barbieri, Nicholas, Richardson, Martin, University of Central Florida
Abstract / Description: Continuing advances in laser and photonic technology has seen the development of lasers with increasing power and increasingly short pulsewidths, which have become available over an increasing range of wavelengths. As the availability of laser sources grow, so do their applications. To make better use of this improving technology, understanding and controlling laser propagation in free space is critical, as is understanding the interaction between laser light and matter.The need to better...
Show moreContinuing advances in laser and photonic technology has seen the development of lasers with increasing power and increasingly short pulsewidths, which have become available over an increasing range of wavelengths. As the availability of laser sources grow, so do their applications. To make better use of this improving technology, understanding and controlling laser propagation in free space is critical, as is understanding the interaction between laser light and matter.The need to better control the light obtained from increasingly advanced laser sources leads to the emergence of beam engineering, the systematic understanding and control of light through refractive media and free space. Beam engineering enables control over the beam shape, energy and spectral composition during propagation, which can be achieved through a variety of means. In this dissertation, several methods of beam engineering are investigated. These methods enable improved control over the shape and propagation of laser light. Laser-matter interaction is also investigated, as it provides both a means to control the propagation of pulsed laser light through the atmosphere, and provides a means to generation remote sources of radiation.
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Date Issued: 2013
Identifier: CFE0004650, ucf:49881
Format: Document (PDF)
PURL: http://purl.flvc.org/ucf/fd/CFE0004650

nonlinear optics (13)	+ -
Nonlinear Optics (8)	+ -
Nonlinear optics (4)	+ -
integrated photonics (4)	+ -
Two-Photon Absorption (3)	+ -

Filamentation (2)	+ -
Solitons (2)	+ -
nonlinear guided waves (2)	+ -
second harmonic generation (2)	+ -
silicon photonics (2)	+ -
solitons (2)	+ -
1PA (1)	+ -
2PA (1)	+ -
Anisotropy (1)	+ -
Axicon (1)	+ -
Bessel Beams (1)	+ -
Cascaded Field Enhancement (1)	+ -
Chrage Transport (1)	+ -
Coherent transients (1)	+ -
Computational Chemistry (1)	+ -
Conjugated Chromophore (1)	+ -
DFT (1)	+ -
Diffraction (1)	+ -
Discrete Optics (1)	+ -
Energy Projection (1)	+ -
Exchange-Correlation Functionals. (1)	+ -
Excited State Dynamics (1)	+ -
Excitons (1)	+ -
FEM and Nonlinear Optics (1)	+ -
Femtosecond (1)	+ -

University of Central Florida (35)	+ -
Christodoulides, Demetrios (12)	+ -
Hagan, David (10)	+ -
Vanstryland, Eric (9)	+ -
Richardson, Martin (7)	+ -

Likamwa, Patrick (5)	+ -
Delfyett, Peter (4)	+ -
Fathpour, Sasan (4)	+ -
Peale, Robert (4)	+ -
Amezcua Correa, Rodrigo (3)	+ -
Hernandez, Florencio (3)	+ -
Baudelet, Matthieu (2)	+ -
Kik, Pieter (2)	+ -
Li, Guifang (2)	+ -
Masunov, Artem (2)	+ -
Thomas, Jayan (2)	+ -
Van Stryland, Eric (2)	+ -
Van Stryland, Eric W. (2)	+ -
Zeldovich, Boris (2)	+ -
Aleahmad, Parinaz (1)	+ -
Balaeff, Alexander (1)	+ -
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Belfield, Kevin (1)	+ -
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Chantharasupawong, Panit (1)	+ -
Chen, Zhigang (1)	+ -
Choi, Jiyeon (1)	+ -
Cirloganu, Claudiu (1)	+ -

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