Measurement of third-order optical nonlinearity of C60M2 (M=Pd, Pt, and Sm) organometallic compounds by the femtosecond optically heterodyned optical Kerr effect
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Chromophore
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We will present the most recent results on the growth and characterization of novel high quality molecular crystals for nonlinear optics. These crystals are based on ionic or hydrogen bonding of new and known chromophores with large second-order hyperpolarizabilities. Detailed results of optical, electro-optical and nonlinear-optical properties of high quality and large size DAST crystals, of hydrazone derivatives and new co-crystals will be presented. It will be shown that optimized parallel alignment of chromophores as well as optimum structures for phase-matched frequency mixing have been realized. In addition, we report on the measurement of the highest known phase-matchable nonlinear susceptibility coefficient of 200 pm/v determined recently in our laboratory.
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A theoretical study on the nonlinear optical properties of both gold and nickel slit arrays inlaid with a third-order nonlinear dielectric medium is presented. In particular, we investigate the optical Kerr effect and third harmonic generation. The geometrical parameters, along with the optical properties of each metal, determine the electromagnetic environment near the slits and, in turn, the nonlinear optical response. The optical Kerr effect is only seen for slit arrays in gold, where the transmitted and reflected currents are modified with the incident intensity, while nickel slit arrays behave linearly within the same range of input intensities. However, third harmonic emission occurs for both systems, unveiling third-order nonlinearities taking place also in nickel structures.
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The third-order nonlinear optical(NLO) properties of(ZnS)6—12 were investigated under the time dependent density functional theory(TDDFT) at B3LYP/Lanl2DZ+6-31G level.The static third-order susceptibilities χ(3) and dynamic behavior of third-order polarizabilities γ in 0 — 2.5 eV were calculated by using the sum over states(SOS) method.The results show that the χ(3) of(ZnS)6—12 clusters are better than that of the other semiconducting clusters.(ZnS)7 and(ZnS)11,respectively,had a remarkable γ value of-2.38×10-33 and 1.26×10-33 esu at 1.6 and 2.0 eV.The(ZnS)6—12 clusters can produce an obvious phenomenon of the third-order polarizabilities when they are excited in a large γ value area.
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Abstract We present an unified overview and classification of the main nonlinear optical effects and the underlying nonlinear optical interactions. The physical origin of these effects is analyzed and related to material features and their behavior, their characteristics and efficiency are discussed in terms of the nonlinear propagation equations. Some aspects related to nonlinear optical materials and devices are presented and connections with quantum optics, nonlinear spectroscopy and optoelectronics are stressed.
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Coordination complex
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The generalized Thomas-Kuhn sum rules are used to characterize the nonlinear optical response of organic chromophores in terms of fundamental parameters that can be measured experimentally. The nonlinear optical performance of organic molecules is evaluated from the combination of hyper-Rayleigh scattering measurements and the analysis in terms of the fundamental limits. Different strategies for the enhancement of nonlinear optical behavior at the molecular and supramolecular level are evaluated and new paradigms for the design of more efficient nonlinear optical molecules are proposed and investigated.
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Recent progress and issues in reasearches on organic and polymeric nonlinear optical materials are reviewd in terms of crystals, Langmuir-Blodgett films, and chromopher-containing polymers for the second-order nonlinear optics, organics and polymers for the third-order nonlinear optics with some emphases on author's works.
Optical materials
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In order to design new organic NLO materials with both higher nonlinear optical susceptibilities, and reasonable optical loss characteristics, it is necessary to understand how different organic structural elements affect the nonlinearity of materials at the molecular level. Only recently, synthetic research groups have begun to devote the time and effort necessary to produce very pure model compounds of systematically varied structures for carefully controlled NLO measurements. In this presentation experimental results and the structural- NLO property trends developed from them are reviewed for the systematic investigations appearing in the literature with emphasis placed on studies conducted by our research group. With these results in mind, some new ways of looking at such organic molecular structures are presented with the intent of stimulating creative thought for novel NLO molecular design.
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We report the rise and fall of third-order optical polarizabilities in donor-acceptor substituted molecules featuring a systematically varied conjugation path. We identify the optimum conjugation length that optimizes the non-linear response in small molecules.
Phase conjugation
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