Nonlinear optics with cold Rb atoms using tapered optical nanofibres

Optical nanofibres (ONFs) are very thin optical waveguides with sub-wavelength diameters. ONFs have very high evanescent fields and the guided light is confined strongly in the transverse direction. These fibres can be used to achieve strong light-matter interactions. Atoms around the waist of an ONF can be probed by collecting the atomic fluorescence coupling or by measuring the transmission (or the polarisation) of the probe beam sent through it. This thesis presents experiments using ONFs for probing and manipulating laser-cooled 87Rb atoms. As an initial experiment, a single mode ONF was integrated into a magneto-optical trap (MOT) and used for measuring the characteristics of the MOT, such as the loading time and the average temperature of the atom cloud. The effect of a near-resonant probe beam on the local temperature of the cold atoms has been studied. Next, the ONF was used for manipulating the atoms in the evanescent fields region in order to generate nonlinear optical effects. Four-wave mixing, ac Stark effect (Autler-Townes splitting) and electromagnetically induced transparency have been observed at unprecedented ultralow power levels. In another experiment, a few-mode ONF, supporting only the fundamental mode and the first higher order mode group, has been used for studying cold atoms. A higher pumping rate of the atomic fluorescence into the higher order fibreguided modes and more interactions with the surrounding atoms for higher order mode evanescent light, when compared to signals for the fundamental mode, have been identified. The results obtained in the thesis are particularly for a fundamental understanding of light-atom interactions when atoms are near a dielectric surface and also for the development of fibre-based quantum information technologies. Atoms coupled to ONFs could be used for preparing intrinsically fibre-coupled quantum nodes for quantum computing and the studies presented here are significant for a detailed understanding of such a system.

NONLINEAR EFFECTS IN MAGNETIC GARNET FILMS AND NONRECIPROCAL OPTICAL BLOCH OSCILLATIONS IN WAVEGUIDE ARRAYS

This dissertation presents detailed experimental and theoretical investigations of nonlinear and nonreciprocal effects in magnetic garnet films. The dissertation thus comprises two major sections. The first section concentrates on the study of a new class of nonlinear magneto-optic thin film materials possessing strong higher order magnetic susceptibility for nonlinear optical applications. The focus was on enlarging the nonlinear performance of ferrite garnet films by strain generation and compositional gradients in the sputter-deposition growth of these films. Under this project several bismuth-substituted yttrium iron garnet (Bi,Y) 3 (Fe,Ga)5 O12(acronym as Bi:YIG) films have been sputter-deposited over gadolinium gallium garnet (Gd 3 Ga5 O12 ) substrates and characterized for their nonlinear optical response. One of the important findings of this work is that lattice mismatch strain drives the second harmonic (SH) signal in the Bi:YIG films, in agreement with theoretical predictions; whereas micro-strain was found not to correlate significantly with SH signal at the micro-strain levels present in these films. This study also elaborates on the role of the film's constitutive elements and their concentration gradients in nonlinear response of the films. Ultrahigh sensitivity delivered by second harmonic generation provides a new exciting tool for studying magnetized surfaces and buried interfaces, making this work important from both a fundamental and application point of view. The second part of the dissertation addresses an important technological need; namely the development of an on-chip optical isolator for use in photonic integrated circuits. It is based on two related novel effects, nonreciprocal and unidirectional optical Bloch oscillations (BOs), recently proposed and developed by Professor Miguel Levy and myself. This dissertation work has established a comprehensive theoretical background for the implementation of these effects in magneto-optic waveguide arrays. The model systems we developed consist of photonic lattices in the form of one-dimensional waveguide arrays where an optical force is introduced into the array through geometrical design turning the beam sideways. Laterally displaced photons are periodically returned to a central guide by photonic crystal action. The effect leads to a novel oscillatory optical phenomenon that can be magnetically controlled and rendered unidirectional. An on-chip optical isolator was designed based on the unidirectionality of the magneto-opticBloch oscillatory motion. The proposed device delivers an isolation ratio as high as 36 dB that remains above 30 dB in a 0.7 nm wavelength bandwidth, at the telecommunication wavelength 1.55 μm. Slight modifications in isolator design allow one to achieve an even more impressive isolation ratio ~ 55 dB, but at the expense of smaller bandwidth. Moreover, the device allows multifunctionality, such as optical switching with a simultaneous isolation function, well suited for photonic integrated circuits.

Optical second harmonic generation in the centrosymmetric magnetic semiconductors EuTe and EuSe

The magnetic europium chalcogenide semiconductors EuTe and EuSe are investigated by the spectroscopy of second harmonic generation (SHG) in the vicinity of the optical band gap formed by transitions involving the 4f and 5d electronic orbitals of the magnetic Eu(2+) ions. In these materials with centrosymmetric crystal lattice the electric-dipole SHG process is symmetry forbidden so that no signal is observed in zero magnetic field. Signal appears, however, in applied magnetic field with the SHG intensity being proportional to the square of magnetization. The magnetic field and temperature dependencies of the induced SHG allow us to introduce a type of nonlinear optical susceptibility determined by the magnetic-dipole contribution in combination with a spontaneous or induced magnetization. The experimental results can be described qualitatively by a phenomenological model based on a symmetry analysis and are in good quantitative agreement with microscopic model calculations accounting for details of the electronic energy and spin structure.

Spin-Induced Optical Second Harmonic Generation in the Centrosymmetric Magnetic Semiconductors EuTe and EuSe

Spectroscopy of the centrosymmetric magnetic semiconductors EuTe and EuSe reveals spin-induced optical second harmonic generation (SHG) in the band gap vicinity at 2.1-2.4 eV. The magnetic field and temperature dependence demonstrates that the SHG arises from the bulk of the materials due to a novel type of nonlinear optical susceptibility caused by the magnetic dipole contribution combined with spontaneous or induced magnetization. This spin-induced susceptibility opens access to a wide class of centrosymmetric systems by harmonics generation spectroscopy.

Porous silicon optical cavity structure applied to high sensitivity organic solvent sensor

The present work reports the thermal annealing process, the number of layer and electrochemical process effect in the optical response quality of Bragg and microcavity devices that were applied as organic solvent sensors. These devices have been obtained by using porous silicon (PS) technology. The optical characterization of the Bragg reflector, before annealing, showed a broad photonic band-gap structure with blue shifted and narrowed after annealing process. The electrochemical process used to obtain the PS-based device imposes the limit in the number of layers because of the chemical dissolution effect. The interface roughness minimizations in the devices have been achieved by using the double electrochemical cell setup. The microcavity devices showed to have a good sensibility for organic solvent detection. The thermal annealed device showed better sensibility feature and this result was attributed to passivation of the surface devices. (c) 2007 Elsevier Ltd. All rights reserved.

Theoretical Analysis of Multimodal Four-Wave Mixing in Optical Microwires

Optical fiber microwires (OFMs) are nonlinear optical waveguides that support several spatial modes. The multimodal generalized nonlinear Schrodinger equation (MM-GNLSE) is deduced taking into account the linear and nonlinear modal coupling. A detailed theoretical description of four-wave mixing (FWM) considering the modal coupling is developed. Both, the intramode and the intermode phase-matching conditions is calculated for an optical microwire in a strong guiding regime. Finally, the FWM dynamics is studied and the amplitude evolution of the pump beams, the signal and the idler are analyzed.

Mono(Eta(5)-cyclopentadienyl)metal(II) complexes with thienyl acetylide chromophores: synthesis, electrochemical studies, and first hyperpolarizabilities

A series of mono(eta(5)-cyclopentadienyl)metal-(II) complexes with nitro-substituted thienyl acetylide ligands of general formula [M(eta(5)-C5H5)(L)(C C{C4H2S}(n)NO2)] (M = Fe, L = kappa(2)-DPPE, n = 1,2; M = Ru, L = kappa(2)-DPPE, 2 PPh3, n = 1, 2; M = Ni, L = PPh3, n = 1, 2) has been synthesized and fully characterized by NMR, FT-IR, and UV-Vis spectroscopy. The electrochemical behavior of the complexes was explored by cyclic voltammetry. Quadratic hyperpolarizabilities (beta) of the complexes have been determined by hyper-Rayleigh scattering (HRS) measurements at 1500 nm. The effect of donor abilities of different organometallic fragments on the quadratic hyperpolarizabilities was studied and correlated with spectroscopic and electrochemical data. Density functional theory (DFT) and time-dependent DFT (TDDFT) calculations were employed to get a better understanding of the second-order nonlinear optical properties in these complexes. In this series, the complexity of the push pull systems is revealed; even so, several trends in the second-order hyperpolarizability can still be recognized. In particular, the overall data seem to indicate that the existence of other electronic transitions in addition to the main MLCT clearly controls the effectiveness of the organometallic donor ability on the second-order NLO properties of these push pull systems.

Harmonic Nanocrystals for Biolabeling: A Survey of Optical Properties and Biocompatibility.

Nonlinear optical nanocrystals have been recently introduced as a promising alternative to fluorescent probes for multiphoton microscopy. We present for the first time a complete survey of the properties of five nanomaterials (KNbO(3), LiNbO(3), BaTiO(3), KTP, and ZnO), describing their preparation and stabilization and providing quantitative estimations of their nonlinear optical response. In the light of their prospective use as biological and clinical markers, we assess their biocompatibility on human healthy and cancerous cell lines. Finally, we demonstrate the great potential for cell imaging of these inherently nonlinear probes in terms of optical contrast, wavelength flexibility, and signal photostability.

Structural and optical properties of dilute InAsN grown by molecular beam epitaxy

We perform a structural and optical characterization of InAs1¿xNx epilayers grown by molecular beam epitaxy on InAs substrates x 2.2% . High-resolution x-ray diffraction HRXRD is used to obtain information about the crystal quality and the strain state of the samples and to determine the N content of the films. The composition of two of the samples investigated is also obtained with time-of-flight secondary ion mass spectroscopy ToF-SIMS measurements. The combined analysis of the HRXRD and ToF-SIMS data suggests that the lattice parameter of InAsN might significantly deviate from Vegard"s law. Raman scattering and far-infrared reflectivity measurements have been carried out to investigate the incorporation of N into the InAsN alloy. N-related local vibrational modes are detected in the samples with higher N content. The origin of the observed features is discussed. We study the compositional dependence of the room-temperature band gap energy of the InAsN alloy. For this purpose, photoluminescence and optical absorption measurements are presented. The results are analyzed in terms of the band-anticrossing BAC model. We find that the room-temperature coupling parameter for InAsN within the BAC model is CNM=2.0 0.1 eV.

Conventional and nonconventional Kramers-Kronig analysis in optical spectroscopy

This Master’s Thesis is dedicated to the investigation and testing conventional and nonconventional Kramers-Kronig relations on simulated and experimentally measured spectra. It is done for both linear and nonlinear optical spectral data. Big part of attention is paid to the new method of obtaining complex refractive index from a transmittance spectrum without direct information of the sample thickness. The latter method is coupled with terahertz tome-domain spectroscopy and Kramers-Kronig analysis applied for testing the validity of complex refractive index. In this research precision of data inversion is evaluated by root-mean square error. Testing of methods is made over different spectral range and implementation of this methods in future is considered.

Optical absorption studies in ion implanted and amorphous semiconductors - Investigations in some tetrahedrally co-ordinated and chalcogenide materials

The thesis provides an overall review and introduction to amorphous semiconductors, followed by a brief discussion on the important structural models proposed for chalcogenide glasses and their electrical, optional and thermal properties. It also gives a brief description of the Physics of thin films, ion implantation and Photothermal Deflection Spectroscopy. A brief description of the experimental setup of a photothermal deflection spectrometer and the details of the preparation and optical characterization of the thin film samples. It deals with the employment of the subgap optional absorption measurement by PDS to characterize the defects, amorphization and annealing behavior in silicon implanted with B+ ions and the profiles of ion range and vacancy distribution obtained by the TRIM simulation. It reports the results of all absorption measurements by PDS in nitrogen implanted thin film samples of Ge-Se and As-Se systems

Possibility of waveguide formation on organic nonlinear crystal methyl para-hydroxy benzoate using high energy ion irradiation

Organic nonlinear optical single crystals of Methyl para-Hydroxy Benzoate (MHB) have been grown using gel-solution technique. These crystals are cut along z-axis and are bombarded with Ag14+ ions of energy 100 MeV. The results show an increase in refractive index at the ion irradiated region. The dielectric constant of the irradiated crystal is increased more than 15 times compared to that of a nonirradiated crystal. The result of these changes and comparative study of second harmonic generation (SHG) efficiency before and after irradiation is discussed.

Fabrication and Characterization of Chalcogenide nano composite based materials for Photonic device applications

In this context,in search of new materials based on chalcogenide glasses,we have developed a novel technique for fabrication of chalcogenide nano composites which are presented in this theis.The techniques includes the dissolution of bulk chalcogenide glasses in amine solvent.This solution casting method allows to retain the attractive optical properties of chalcogenide glasses enabling new fabrication routes for realization of large area thick-thin films with less cost. Chalcogenide glass fiber geometry opens new possibilities for a large number of applications in optics,like remote temperature measurements ,CO2 laser power delivery, and optical sensing and single mode propagation of IR light.We have fabricated new optical polymer fibers doped with chalcogenide glasses which can be used for many optical applications.The present thesis also describes the structural,thermal and optical characterization of certain chalocogenide based materials prepared for different methods and its applications.

Cadmium Selenide Based Core-Shell Quantum Dots for Biosensing and Imaging Applications

The overall focus of the thesis involves the synthesis and characterization of CdSe QDs overcoated with shell materials for various biological and chemical sensing applications. Second chapter deals with the synthesis and characterization of CdSe and CdSe/ZnS core shell QDs. The primary attention of this work is to develop a simple method based on photoinduced charge transfer to optimize the shell thickness. Synthesis of water soluble CdSe QDs, their cytotoxicity analysis and investigation of nonlinear optical properties form the subject of third chapter. Final chapter deals with development of QD based sensor systems for the selective detection of biologically and environmentally important analytes from aqueous media.

Investigations on the structural, optical and Magnetic properties of nanostructured cerium oxide in pure and doped forms and its polymer nanocomposiets

This thesis Entitled INVESTIGATIONS ON THE STRUCTURAL, OPTICAL AND MAGNETIC PROPERTIES OF NANOSTRUCTURED CERIUM OXIDE IN PURE AND DOPED FORMS AND ITS POLYMER NANOCOMPOSITES.Synthesis and processing of nanomatelials and nanostmctures are the essential aspects of nanotechnology. Studies on new physical properties and applications of nanomaterials and nanostructures are possible only when nanostructured materials are made available with desired size, morphology,crystal structure and chemical composition.Recently, several methods have been developed to prepare pure and doped CeO2 powder, including wet chemical synthesis, thermal hydrolysis, flux method, hydrothermal synthesis, gas condensation method, microwave technique etc. In all these, some special reaction conditions, such as high temperature, high pressure, capping agents, expensive or toxic solvents etc. have been involved.Another hi gh-li ght of the present work is room temperature ferromagnetism in cerium oxdie thin films deposited by spray pyrolysis technique.The observation of self trapped exciton mediated PL in ceria nanocrystals is another important outcome of the present study. STE mediated mechanism has been proposed for CeO2 nanocrystals based on the dependence of PL intensity on the annealing temperature. It would be interesting to extent these investigations to the doped forms of cerium oxide and cerium oxide thin films to get deeper Insight into STE mechanism.Due to time constraints detailed investigations could not be canied out on the preparation and properties of free standing films of polymer/ceria nanocomposites. It has been observed that good quality free standing films of PVDF/ceria, PS/C61‘l8, PMMA/ceria can be obtained using solution casting technique. These polymer nanocomposite films show high dielectric constant around 20 and offer prospects of applications as gate electrodes in metal-oxide semiconductor devices.