The phenomenon of polarization interaction in certain nonlinear materials is presented, and the design of an all-optical logic device based on this concept is described. An efficient two-dimensional finite-difference time-domain code for studying third-order nonlinear optical phenomena is discussed, in which both the slowly varying and the rapidly varying components of the electromagnetic fields are considered. The algorithm solves the vector form Maxwell s equations for all field components and uses the nonlinear constitutive relation in matrix form as the equations required to describe the nonlinear system. The stability of the code is discussed and its accuracy demonstrated through the simulation of the self-phase modulation effect observed in Kerr media. Finally, the code is used to simulate polarization mixing in photonic crystal-based line defect and coupled resonator optical waveguides.

Polymer liquid crystal possesses advantages of polymer in chemical industry and liquid crystal in display industry,so it is attracted more attention in science and technology. Diacrylate is a polymer liquid crystal with photosensitive property, so ,it can be applied to optical storage . He-Ne laser induced polymerization in diacrylate mesogen RM257 and RM82 had been verified in previous study. Furthermore, holography pattern can be recorded in RM257 and RM82 by controlling both the temperature of sample and the time of exposing. In this study, we consider the study of nonlinear optical properties of diacrylate using Z-SCAN techeique.¡¨Z-SCAN¡¨ is a simply yet highly sensitive single-beam experimential technique ,it can be used to measure both nonlinear absorption and nonlinear refraction.In this study ,we measured effect of absorption of diacrylate in irradiation of He-Ne laser using Z-SCAN technique.To investigate the reason that He-Ne laser induced polymerization in both RM257 and RM82.

Optical imaging of soft biological tissue is highly desirable since it is nonionizing and provides sensitive contrast information which enables the detection of physiological functions and abnormalities, including potentially early cancer detection. However, due to the diffusive nature of light in soft biological tissue, it is difficult to achieve simultaneously good spatial resolution and good imaging depth with pure optical imaging modalities. This work focuses on the ultrasound-modulated optical tomography (UOT): a hybrid technique which combines the advantages of ultrasonic resolution and optical contrast. In this technique, focused ultrasound and optical radiation of high temporal coherence are simultaneously applied to soft biological tissue. The intensity of the sideband, or ultrasound ‗tagged‘ photons depends on the optical absorption in the region of interest where the ultrasound is focused. Demodulation of the optical speckle pattern yields the intensity of tagged photons for each location of the ultrasonic focal spot. Thus UOT yields an image with spatial resolution of the focused ultrasound — typically submillimeter — whose contrast is related to local optical absorption and the diffusive properties of light in the organ. Thus it extends all the advantages of optical imaging deep into highly scattering tissue. However lack of efficient tagged light detection techniques has so far prevented ultrasound-modulated optical tomography from achieving maturity. The signal-to-noise ratio (SNR) and imaging speed are two of the most important figures of merit and need further improvement for UOT to become widely applicable. In the first part of this work, nonlinear optics detection methods have been implemented to demodulate the ―tagged‖ photons. The most common of these is photorefractive (PR) two wave mixing (TWM) interferometry, which is a time-domain filtering technique. When used for UOT, it is found that this approach extracts not only optical properties but also mechanical properties for the area of interest. To improve on TWM, PR four wave mixing (FWM) experiments were performed to read out only the modulated light and at the same time strongly suppressing the ‗untagged‘ light. Spectral-hole burning (SHB) in a rare-earth-ion-doped crystal has been developed for UOT more recently. Experiments in Tm3 :Y3Al5O12 (Tm:YAG) show the outstanding features of SHB: large angle acceptance (etendue), light speckle processing in parallel (insensitive to the diffusive light nature) and real-time signal collection (immune to light speckle decorrelation). With the help of advanced laser stabilization techniques, two orders of magnitude improvement of SNR have been achieved in a persistent SHB material (Pr^3 :Y2SiO5) compared to Tm:YAG. Also slow light with PSHB further reduces noise in Pr:YSO UOT that is caused by polarization leakage by performing time-domain filtering.

The synchronously pumped femtosecond optical parametric oscillator (OPO) based on was periodically poled 5-mol.% MgO-doped lithuium niobate was demonstrated by means of non-critical quasi phase matching. The femtosecond OPO is cable of operating at room temperature and shows no photorefractive damage. The spectrum can be tuned by varying the cavity length up to 70 £gm, the temperature of the nonlinear crystal from room temperature to 150¢J, and the grating periods. The cavity was designed to resonate at 1.33 £gm with bandwidth of 100 nm. The maximum output intensity of the signal is 43 mW with TEM00 mode. The signal slope efficiency is 11%. The spectrum range of the idler is tunable from 1.8 to 2.8 £gm.

Short Pulse equation derived by Schafer and Wayne is a nonlinear partial differential equation that describes ultra short laser propagation in a dispersive optical medium such as optical fibers. Some properties of this equation e.g. traveling wave solution and its soliton structure and some of its conserved quantities were investigated. Conserved quantities were obtained by mass conservation law, lax pair method and transformation between Sine-Gordon and short pulse equation. As a result, loop soliton characteristic and six conserved quantities were found.

Herein are presented collective studies of amino acid-based surfactants, also known as lipoamino acids, at liquid interfaces. Chapter III describes an investigation of domain morphology of N-Stearoylglutamic acid (N-SGA) Langmuir monolayers at the air/water interface by epifluorescence microscopy. Anisotropic feather-like domains were observed in L-enantiomeric monolayers while symmetric circular domains were found in racemic N-SGA monolayers. At a surface pressure of 30 mN/m the enantiomeric domains melted at 31 ??C while the racemic domains melted at 27 ??C. This result is exactly opposite to the behavior found in bulk crystals where the racemate melts at a higher temperature. These results were explained in terms of different molecular packing and hydrogen bonding between bulk crystals and two-dimensional thin films for enantiomeric and racemic compounds. Chapter IV summarizes the investigations of hydrogen bonding in N-acyl amino acid monolayers by vibrational sum-frequency spectroscopy (VSFS). The intermolecular hydrogen bonding interaction between the adjacent molecules through amide-amide groups in N-stearoylalanine (N-SA) is characterized by an NH stretch peak at 3311 cm-1. This is the first time that the amide NH stretching signals have been detected with the VSFS technique. A similar peak was detected at 3341 cm-1on N-SGA monolayer. The higher frequency indicates that the H-bond strength is weaker due to the larger size of the glutamic acid residue. The NH stretch mode can thus be used as a fingerprint of hydrogen bonding among amide-amide groups. A peak at 3050 cm-1 due to hydrogen bonding among carboxyl groups was also resolved from the VSFS spectra. Molecular models of intermolecular hydrogen bonding were proposed.

Material development is necessary before all-optical signal processing (AOSP) can be realized. Traditional AOSP will require materials with a large magnitude of the real part of the third-order polarizability, while having a small imaginary magnitude of third-order polarizability. The aim of this thesis is to investigate the potential for polymethine dyes to be used for AOSP applications. The basic structure of a polymethine dye was synthetically modified in a variety of positions to observe the effects upon the linear and nonlinear optical properties. The modifications included variation in the terminal group, substituents in the polymethine bridge, and exchange of the counterion. The dyes were generally synthesized using the Vilsmeyer-Haack reaction to form simple polymethine precursors, and then complexity was added by performing the Knoevenagel condensation with various acceptors and the polymethine precursor. Ion metathesis was often employed to exchange the initial counterion for a counterion that provided increased solubility in common organic solvents. The third-order nonlinear optical polarizabilities were characterized by Dr. Joel Hales who used the open- and closed-aperture Z-scan technique at 1300 nm and non-degenerate two-photon absorption experiments to identify the position of the two-photon absorption bands.

Structure-property relationships for two-photon absorption (2PA) in branched organic chromophores is a topic of current interest, as is the design of chromophores with advantageous properties for two-photon laser scanning microscopy (2PLSM). The main goals of this dissertation were to study and explain the one-photon absorption (1PA) and 2PA properties of cruciform chromophores based on 1,4-distyryl-2,5-bis(phenylethynyl)benzene with varying electron donor (D) and acceptor (A) groups, and to characterize the 2PLSM-relevant response of some of these chromophores and a set of dipolar chromophores to binding with zinc ions. The compounds were studied by 1PA, fluorescence and 2PA spectroscopy. A ππ* exciton model was developed to explain the spectral properties of the 1,4-distyryl-2,5-bis(phenylethynyl)benzene cruciform with no D or A groups or with four identical D groups at the termini of the linear arms of the chromophore. This model indicated that there is some coupling and mixing of the lowest excited states e of the linear arms, leading to splitting of the 1PA spectrum of the cruciform. There was little coupling or mixing of the higher excited states e′ accessed in 2PA, leading to a two-band 2PA spectrum for the chromophore, in contrast to cruciform compounds in the literature with identical conjugated arms, which have one visible 2PA band. For cruciforms with D groups on the styryl arm and A character on the terminal phenyls of the phenylethynyl arms (D/A cruciforms), the ππ* exciton model was complemented with a charge-transfer (CT) exciton model describing interactions of charge-transfer pathways between the D and A groups. This model explained the broadness of the 1PA band of D/A cruciforms as well as the two 2PA bands observed for these chromophores. The fluorescence and 2PA spectral responses to binding of Zn²⁺ ions to the D or A groups of some cruciform compounds were also assessed, to provide insight into the design of new analyte-sensing cruciforms for 2PLSM that take advantage of enhancement or reduction of D/A character upon analyte binding. It was found that canceling charge donation from the D groups in differing D/A cruciforms resulted in fluorescence and 2PA spectra nearly indistinguishable from each other, suggesting that turn-off of D groups is not an optimal modality of 2PLSM analyte sensing in cruciforms. Binding Zn²⁺ to A groups was shown to result in an increase in the D/A character of the cruciform, with fluorescence peak energies that changed depending on the location of the A group. It is suggested that the use of non-binding donors and analyte-binding A groups in differing patterns on the arms could be a valuable design motif to achieve 2PLSM sensor compounds based on this cruciform structure. The 2PA spectra of a set of dipolar Zn²⁺ sensing dyes designed for ratiometric imaging in 2PLSM were also studied. These dyes had moderate 2PA strength, with redshifts of fluorescence 2PA spectra on Zn²⁺ binding. The isosbestic point of 2PA of most chromophores was within the range of 2PLSM excitation sources commonly used, rendering these dyes good candidates for use in ratiometric sensing in 2PLSM.

We have used ultrafast optics, primarily focused on the nonlinear processes of Polarization Gating and of Optical Parametric Amplification, one for measurement and the other for imaging purposes. For measurement, we have demonstrated a robust method of measurement to simultaneously measure both optical pulses used in a pump-probe type configuration. We refer to this method of pulse measurement as Double Blind Polarization Gating FROG. We have demonstrated this single-shot method for measuring two unknown pulses using one device. In addition to pulse measurement, we have demonstrated the processes of Optical Parametric Amplification (OPA) applicability to imaging of complex objects. We have done this where the Fourier transform plane is used during the interaction. We have amplified and wavelength converted a complex image. We observe a gain of ~100, and, although our images were averaged over many shots, we used a single-shot geometry, capable of true single-shot OPA imaging. To our knowledge, this is the first Fourier-plane OPA imaging of more than a single spatial-frequency component of an image. We observe more than 30 distinct spatial frequency components in both our amplified image and our wavelength shifted image. We have demonstrated all-optical spatial filtering for these complex images. We have demonstrated that direct Fourier filtering of spatial features is possible by using a shaped pump beam. We can isolate certain portions of the image simply by rotating the crystal.

Although mathematical cryptography has been widely used, its security has only been proven under certain assumptions such as the computational power of opponents. As an alternative, quantum communication, in particular quantum key distribution (QKD) can get around unproven assumptions and achieve unconditional security. However, the key generation rate of practical QKD systems is limited by device imperfections, excess noise from the quantum channel, limited rate of true random-number generation, quantum entanglement preparation, and/or post-processing efficiency. This dissertation contributes to improving the performance of quantum communication systems. First, it proposes a new continuous-variable QKD (CVQKD) protocol that loosens the efficiency requirement on post-processing, a bottleneck for long-distance CVQKD systems. It also demonstrates an experimental implementation of the proposed protocol. To achieve high rates, the CVQKD experiment uses a continuous-wave local oscillator (CWLO). The excess noise caused by guided acoustic-wave Brillioun scattering (GAWBS) is avoided by a frequency-shift scheme, resulting in a 32 dB noise reduction. The statistical distribution of the GAWBS noise is characterized by quantum tomography. Measurements show Gaussian statistics upto 55 dB of dynamical range, which validates the security calculations in the proposed CVQKD protocol. True random numbers are required in quantum and classical cryptography. A second contribution of this thesis is that it experimentally demonstrates an ultrafast quantum random-number generator (QRNG) based on amplified spontaneous emission (ASE). Random numbers are produced by a multi-mode photon counting measurement on ASE light. The performance of the QRNG is analyzed with quantum information theory and verified with NIST standard random-number test. The QRNG experiment demonstrates a random-number generation rate at 20 Gbits/s. Theoretical studies show fundamental limits for such QRNGs. Quantum entanglement produced in nonlinear optical processes can help to increase quantum communication distance. A third contribution is the research on nonlinear optics of graphene, a novel 2D material with unconventional physical properties. Based on a quantum-dynamical model, optical responses of graphene are derived, showing for the first time a link between the complex linear optical conductivity and the quantum decoherence. Nonlinear optical responses, in particular four-wave mixing, is studied for the first time. The theory predicts saturation effects in graphene and relates the saturation threshold to the ultrafast quantum decoherence and carrier relaxation in graphene. For the experimental part, four-wave mixing in graphene is demonstrated. Twin-photon production in graphene is under investigation.