The creation of optical states of light that are quantum mechanical in nature in optical fibers is discussed and demonstrated experimentally. Specifically, two- photon states created by spontaneous four-wave-mixing in commercially available single-mode, birefringent fibers are studied. When creating photon states of light, it is important to verify the created states are of the proper photon number distribution and free of noise. We detail a method for combining thresholding, non-number resolving detectors to characterize the photon number distribution created via SFWM and a procedure to quantify the noise sources present in the process. Frequency translation in optical fibers with two-photon states is discussed and experimental considerations are presented.

M.Ing. / The aim of this project is to research the feasibility of an all-fibre laser distance measurement device that utilises a figure-eight fibre laser (F8L), in the nonlinear amplifying loop mirror (NALM) configuration, as a light source and implements pulse compression to improve the accuracy and signal-to-noise ratio of the system. A figure-eight fibre laser in the NALM configuration for use in a laser distance measurement device is described. The theory of fibre lasers is discussed, including mode-locking and Qswitching, and the characteristics of a NALM loop are analysed. By varying the length of the NALM loop from 500 m to 2000 m or inserting highly nonlinear dispersion shifted fibre, a variety of pulses in the picosecond to nanosecond range can be produced. The lengths of the pulses depend on the length of the NALM loop, the pump power and the setting of the polarisation controllers. The figure-eight fibre laser is pumped with a 980 nm laser diode up to 550 mA, which corresponds to 320 mW. Distance measurements are done with short unmodulated and long modulated pulses. Distance measurement with short unmodulated pulses is discussed only briefly and tested with a simple experiment. The focus of this project is distance measurement with long modulated pulses. A low autocorrelated binary sequence is modulated onto one of the long pulses produced by the figure-eight fibre laser by an electro-optic amplitude modulator. The long pulse gives the proposed system a good signal-to-noise ratio (SNR), while the modulation improves the accuracy. A Barker code of length 13 is proposed as modulation code because of its good autocorrelation properties. The Barker code will improve the accuracy 13-fold, with a corresponding increase in SNR. An electro-optic amplitude modulator is used to implement the modulation. The modulated long pulse is then sent to a target. After reflection, the signal is detected and cross-correlated to obtain the time-of-flight for the pulse. The code generation and cross-correlation are implemented with an FPGA via VHDL programming. The distance to a target can be calculated by knowing the time-of-flight and the speed of light in the propagation medium. In this project the resolution, single-shot precision, accuracy, linearity, repeatability and maximum unambiguous distance of the proposed all-fibre laser distance measurement device are examined.

CdTe QDs capped with mercaptopropionic acid (MPA) and thioglycolic acid (TGA) were covalently linked to zinc and indium tetraaminophthalocyanines (TAPcs) using N-ethyl-N(3-dimethylaminopropyl) carbodiimide (EDC) and N-hydroxy succinimide (NHS) as the coupling agents. The results presented give evidence in favour of formation of an amide bond between the MTAPc and CdTe QDs. Both the linked ZnTAPc–QD complexes and the mixture of QDs and ZnTAPc (without chemical linking) showed Förster resonance energy transfer (FRET), though the linked showed less FRET, whereas the QD interactions with InTAPc yielded no evidence of FRET. Both MTAPcs quenched the QDs emission, with quenching constants of the order of 103–104M−1, binding constants of the order of 108-1010M-1 and the number of binding sites for the MTAPc upon the QD being 2. High energy transfer efficiencies were obtained (in some cases as high as 93%), due to the low donor to acceptor distances. Lastly, both MTAPc were shown to be poor optical limiters because their imaginary third-order susceptibility (Im[χ(3)]) was of the order of 10-17-10-16 (optimal range is 10-9-10-11), the hyperpolarizability (γ) of the order of 10-37-10-36 (optimal range is 10-29-10-34) and the k values were above one but below ten.

Please read the abstract in the section front of this document. / Dissertation (MSc (Chemistry))--University of Pretoria, 2006. / Chemistry / unrestricted

No description available.

In this thesis we ran a series of 2D simulations of femtosecond laser pulses filamenting in air using the FDTD method, a saturable Lorentz oscillator model of air [1], and two separate models of plasma: a Drude model where the plasma density is static in space, and a particle-in-cell model where plasma is free to migrate throughout the simulation space. By comparing matched pairs of simulations, which varied in pulse size, duration, and intensity, we can gauge the impact plasma dynamics has upon the evolution of a filamenting laser pulse. From these tests we determine that, while there are some visible differences between dynamic and static plasmas, plasma dynamics do not significantly alter the evolution of the pulse.

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.

Thesis: M.S., Massachusetts Institute of Technology, Department of Physics, 1976 / Includes bibliographical references. / M.S. / M.S. Massachusetts Institute of Technology, Department of Physics

The molecular structure and charge on solid surfaces in aqueous environments is of fundamental importance to various scientific research and applications, yet remain not sufficiently understood. The research herein uses sum frequency generation spectroscopy to reveal the molecular structure of the mineral and polymer surfaces, and also probes the water molecules near the charged aqueous interfaces to get information about the surface charge. The application of visible-infrared sum-frequency generation spectroscopy to polymer thin-films requires a careful interpretation of the results, as the electric field magnitude and phase at each interface must be determined in a manner that takes thin film interference effects into account. A straightforward method that has a concise analytic solution in the case of a single thin film that exhibits interference effects was proposed. This method enabled selective probing of transparent thin-films using sum frequency generation spectroscopy, hence eliminated the ambiguity of the contribution of signal from two interfaces. The method was then extended to multiple polarization schemes, enabling easier and more comprehensive study of the molecular orientation on thin-films. Nonlinear vibrational spectroscopy has also been used to study the temperature-dependent surface structure of polydimethylsiloxane when exposed to water and a perfluorinated hydrophobic liquid. Quantitative analysis of the methyl plane orientation was performed using a combination of vibrational peak ratios and peak amplitudes that enable proposed structures to be identified. For both environments, the tilt and twist of the methyl plane was found to increase with temperature in a reversible manner. This has been attributed to be a consequence of the backbone reorganization due to temperature-dependent density changes. At charged aqueous interfaces, the structure of water adjacent to solid interface is sensitive to the surface potential. As a result, close inspection of signals originating from these water molecules can be used to reveal the surface charge density. Nonlinear vibrational spectroscopy was used to monitor the water O-H stretching band over a temperature range of 10-75°C to account for the increase in surface potential from deprotonation. It has been demonstrated that the behavior at the silica surface is a balance between increasing surface charge, and a decreasing contribution of water molecules aligned by the surface charge. Together with a model that accounts for two different types of silanol sites, the change in enthalpy and entropy for deprotonation at each site were reported. The surface charge density of untreated polydimethylsiloxane surface in water with various ionic strengths was also determined. It was found that the surface charge could be explained with an ion adsorption model. A relationship between the surface potential and measured nonlinear optics response that is valid at high potentials and low ionic strength was proposed. Finally, a universal method was demonstrated to derive the surface potential with nonlinear optics by modulating the coherence length. / Graduate / 2022-09-07

Stimulated Raman scattering (SRS) imaging is a chemical imaging scheme that can visualize cellular content based on intrinsic chemical bond vibrations. To resolve chemicals with overlapping Raman bands, spectroscopic SRS platforms have been developed. To date, endeavors on high-speed instrumentation have achieved spectral acquisition at the microsecond level, enabling in vivo imaging of cells and tissues. Nevertheless, due to the extremely small Raman cross-sections, the current performance of SRS is bounded by a design space that trades off speed, signal fidelity, and spectral bandwidth. The lack of tailored data mining algorithms further limits the chemical information one can extract from the spectroscopic images. My thesis work focuses on developing computational SRS imaging approaches to break the physical tradeoffs and novel data analytical tools to decipher essential chemical information from stimulated Raman spectroscopic images. Utilizing data redundancy of spectroscopic images, we developed two compressive sensing schemes to improve the imaging speed by one order of magnitude without information loss. To break the sensitivity limit, we proposed an ultrafast spectroscopic SRS system and further integrated it with a deep neural network to synergistically achieve microsecond level imaging in the fingerprint region. To improve the chemical specificity and content levels, we implemented a sparsity-regularized spectral unmixing algorithm, realizing multiplexed imaging of up to six major metabolites in a cell. Finally, enabled by advances in low-exposure imaging and spectral unmixing, longitudinal imaging of biofuel synthesis in live cells with sophisticated chemical information is demonstrated. / 2022-09-24T00:00:00Z