Non-linear optical processes such as coherent anti-Stokes Raman scattering and sum frequency generation offer a view into the chemical and biological interactions of molecules that is distinctly different from linear techniques like near infra-red and fluorescence. This insight comes at a cost: non-linear techniques are more sensitive to external perturbations of the system, increasing the noise and decreasing the repeatability of the data. We work here on both aspects of these non-linear techniques, taking advantage of their power to offer new imaging techniques as well as working to quantify and reduce the non-resonant noise inherent to the system. In pursuit of the first part, we look at formalin fixed paraffin embedded tissue samples. This is the most common form of tissue storage in the world. However, the paraffin renders them unavailable for spectroscopic study. We introduce a new technique, combination coherent anti-Stokes Raman scattering microscopy and sum frequency generation microscopy, to avoid the issue of paraffin signal contamination. This high resolution, widefield technique allows for the separate identification of paraffin and the tissue embedded within it. We show in this work the capability of this technique to enable high throughput automated detection of osteoporosis in mice. In pursuit of the second part, we demonstrate experimentally for the first time, deferred build up in coherent anti-Stokes Raman scattering. We show that coherent anti-Stokes Raman scattering signal is maximized when the probe pulse is delayed by an amount dependent on the probe width and the material itself. Non-resonant contamination, however, is maximized when the probe delay is zero, meaning that it is possible to decrease the non-resonant noise while increasing the desired signal. We also show that the dephasing time is inversely dependent on the probe width, so narrower probe pulses allow for further delayed probe pulses, which in turn decrease non-resonant noise more. We demonstrate this technique by looking at the effects of hydrogen bonding in pyridine-water complexes.

Wavefront sensors for measurements on human eyes are usually large, expensive and difficult to move. A compact wavefront sensor would be more cost-effective and versatile as is could be used in multiple systems. The aim of this thesis was to produce a more compact and portable wavefront sensor. A shorter telescope design for the wavefront sensor was proposed and checked theoretically and with computer simulations. An experimental arrangement comparing the proposed telescope design with a conventional telescope design was constructed. A compact wavefront sensor was built using off-the-shelf components and a few modified components. Tests with the compact wavefront sensor were made both on eye models and on human eyes. The compact wavefront sensor correctly measured the refractive errors of two eye models. It was also possible to perform measurements on human eyes, both in the central and peripheral visual fields, and higher order aberrations were confirmed. For positioning human eyes at the correct distance from the wavefront sensor an additional pupil camera was needed, which was not included in the system. Future improvements for the compact wavefront sensor are discussed. / Vågfrontssensorer för mätningar på ögon är ofta mycket stora, dyra och svåra att transportera. En kompakt vågfrontssensor skulle vara kostnadseffektiv och flexibel eftersom den skulle kunna användas i flera olika system. Målet med detta examensarbete var att producera en mer kompakt och transportabel vågfrontssensor. En kortare teleskopvariant föreslogs och analyserades både teoretiskt och med datorsimuleringar. En experimentell uppsättning gjordes också för att jämföra den kortare teleskopdesignen med ett sedvanligt vågfrontssensorteleskop. En kompakt vågfrontssensor byggdes med standardkomponenter samt med några modifierade standardkomponenter. Tester med den kompakta vågfrontssensorn gjordes både på ögonmodeller och mänskliga ögon. Den kompakta vågfrontssensorn gav korrekta mätvärden på brytningsfelen på ögonmodellerna. Det gick bra att genomföra mätningar på mänskliga ögon, både i centrala och perifera synfältet, och högre ordningens aberrationer bekräftades. För att placera mänskliga ögon på korrekt avstånd från vågfrontssensorn krävdes en extra pupillkamera, som inte var inkluderad i den kompakta vågfrontssensorn. Framtida förbättringar för den kompakta vågfrontssensorn diskuteras.

A variant of RABBITT pump-probe spectroscopy in which the attosecond pulse train comprises both even and odd harmonics of the fundamental IR probe frequency is explored to measure time-resolved photoelectron emission in systems that exhibit autoionizing states. It is shown that the group delay of both one-photon and two-photon resonant transitions is directly encoded in the energy-resolved photoelectron anisotropy as a function of the pump-probe time-delay. This principle is illustrated for a 1D model with symmetric zero-range potentials that supports both bound states and shape-resonances. The model is studied using both perturbation theory and solving the time-dependent Schodinger equation on a grid. Moreover, we study the case of a realistic atomic system, helium. In both cases, we demonstrate faithful reconstruction of the phase information for resonant photoemission.

No description available.

<p>Optical beams that travel through a material without undergoing divergence are known as self-trapped beams. Self-trapping occurs when a beam induces a suitable index gradient in the medium that is capable of guiding the original beam. An incoherent light consists of femtosecond scale speckles, due to random phase fluctuations and were not thought to self-trap until recently. In 1997, Mitchell et al., showed that white light can self-trap, provided the medium cannot respond fast enough to form index gradients to these speckles individually. However, detailed studies have been hampered by a lack of suitable materials and strategies for enabling such a response. In 2006, our group showed that a photopolymer is suitable for incoherent self-trapping, since the index change is governed by an inherently slow rate of polymerization (of the order of milliseconds). This has enabled further studies of various phenomena with white light self-trapping.</p> <p>The studies here show (i) the first direct experimental evidence of interactions of two incoherent white light self-trapped beams, as well as fission, fusion and repulsion. Existence of dark self-trapping beams with incoherent white light was also shown, counter intuitively in a positive nonlinear medium. (iii) Lattices were formed with multiple ordered bright as well as dark self-trapping filaments using optochemical self-organization. (iv) Woodpile-like 3D lattices with bright and dark beams were also demonstrated and simulations showed theoretical band gaps. (v) Self-trapping of a co-axial beam of incoherent white light was also shown experimentally and through simulations.</p> / Doctor of Philosophy (PhD)

This dissertation is focused on theoretical and experimental studies of optical properties of materials and multilayer structures composing liquid crystal displays (LCDs) and electrochromic (EC) devices. By applying spectroscopic ellipsometry, we have determined the optical constants of thin films of electrochromic tungsten oxide (WOx) and nickel oxide (NiOy), the films’ thickness and roughness. These films, which were obtained at spattering conditions possess high transmittance that is important for achieving good visibility and high contrast in an EC device. Another application of the general spectroscopic ellipsometry relates to the study of a photo-alignment layer of a mixture of azo-dyes SD-1 and SDA-2. We have found the optical constants of this mixture before and after illuminating it by polarized UV light. The results obtained confirm the diffusion model to explain the formation of the photo-induced order in azo-dye films. We have developed new techniques for fast characterization of twisted nematic LC cells in transmissive and reflective modes. Our techniques are based on the characteristics functions that we have introduced for determination of parameters of non-uniform birefringent media. These characteristic functions are found by simple procedures and can be utilised for simultaneous determination of retardation, its wavelength dispersion, and twist angle, as well as for solving associated optimization problems. Cholesteric LCD that possesses some unique properties, such as bistability and good selective scattering, however, has a disadvantage – relatively high driving voltage (tens of volts). The way we propose to reduce the driving voltage consists of applying a stack of thin (~1µm) LC layers. We have studied the ability of a layer of a surface stabilized ferroelectric liquid crystal coupled with several retardation plates for birefringent color generation. We have demonstrated that in order to accomplish good color characteristics and high brightness of the display, one or two retardation plates are sufficient.

No description available.

Theoretical work in quantum information has demonstrated that a classical hidden-variable model of an entangled singlet state can explain nonclassical correlations observed in tests of Bell’s inequality if while measuring the Bell correlation, the underlying probability distribution of the hidden-variable changes depending on the measurement basis. To rule out this possibility, distant quasars can be utilized as random number generators to set measurement bases in an experimental test of Bell’s inequality. Here we report on the design and characterization of a device that uses the color of incoming quasar photons to output a random bit with nanosecond latency. Through the 1-meter telescope at JPL Table Mountain Observatory, we observe and generate random bits from quasars with redshifts z = 0.1−3.9. In addition, we formulate a mathematical model that quantifies the fidelity of the bits generated.

Quantum confinement in small metal clusters leads to a bunching of states into electronic shells reminiscent of shells in atoms. The addition of ligands can tune the valence electron count and electron distribution in metal clusters. A combined experimental and theoretical study of the reactivity of methanol with AlnIm− clusters reveals that ligands can enhance the stability of clusters. In some cases the electronegative ligand may perturb the charge density of the metallic core generating active sites that can lead to the etching of the cluster. Also, an investigation is conducted to understand how the bonding scheme of a magnetic dopant evolves as the electronic structure of the host material is varied. By considering VCun+, VAgn+, and VAun+ clusters, we find that the electronic and atomic structure of the cluster plays a major role in determining how an impurity will couple to its surroundings.

Doctor of Philosophy / Department of Physics / Itzik Ben-Itzhak / One ultimate goal of ultrafast, strong- field laser science is to coherently control chemical reactions. Present laser technology allows for the production of intense (>10[superscript]13 W/cm[superscript]2), ultrashort ( 5 fs), carrier-envelope phase-stabilized pulses. By knowing the electric field waveform, sub-cycle resolution on the order of 100's of attoseconds (1 as=10[superscript]-18 s) can be reached -- the timescale for electron motion. Meanwhile, the laser field strengths are comparable to that which binds electrons to atoms or molecules. In this intense-field ultrashort-pulse regime one can both measure and manipulate dynamics of strong-field, quantum-mechanical processes in atoms and molecules. Despite much progress in the technology, typical durations for which lasers can be reliably locked to a specific carrier-envelope phase ranges from a few minutes to a few hours. Experiments investigating carrier-envelope phase effects that have necessarily long data acquisition times, such as those requiring coincidence between fragments originating from the same atom or molecule, are thus challenging and uncommon. Therefore, we combined the new technology for measuring the carrier-envelope phase of each and every laser shot with other single-shot coincidence three-dimensional momentum imaging techniques to alleviate the need for carrier-envelope phase stabilized laser pulses. Using phase-tagged coincidence techniques, several targets and laser-induced processes were studied. One particular highlight uses this method to study the recollision process of non-sequential double ionization of argon. By measuring the momentum of the two electrons emitted in the process, we could study their energy sharing. Furthermore, by selecting certain carrier-envelope phase values, and therefore laser pulses with a particular waveform, events with single recollision could be isolated and further analyzed. Another highlight is our studies of carrier-envelope phase effects in the dissociation of the benchmark H[subscript]2[superscript[+] ion beam. Aided by near-exact quantum mechanical calculations, we could identify interfering pathways which lead to the observed spatial asymmetry. These and other similar experiments are described in this thesis as significant steps toward their ultimate control.