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The research accomplished in this project consists of four tasks each dealing with a different class of nonlinear optical (NLO) materials. Task (I): Second-order nonlinear optical materials. We developed new chromophores and processing to produce electro-optic materials with enhanced optical transparency towards the visible (>=700 nm), increased chemical and thermal stability and stability of poled alignment for 1000 hours at 100 deg C. Several approaches showed promises and we accomplished a great deal. Also, we developed polyurethane cross-linking polymers to produce thermally stable poling alignment in both molecular-ionic type and neutral type second-order chromophores. In both cases stability up to 1000 hours at 100 deg C was achieved. In another approach, in collaboration with Professor Shea of University of California, Irvine, we have employed ormosils to produce stable poled alignments. Task (II): Third-order nonlinear optical materials. We synthesized a group of phosphoylides containing a polarizable P atom and investigated their X(3) behavior via femtosecond Kerr gate measurements. By using optically heterodyned and phase-tuned Kerr gate techniques, we obtained both the signs and the magnitudes of the real and the imaginary components of X(3).
Organic Nonlinear Optical Materials provides an extensive description of the preparation and characterization of organic materials for applications in nonlinear and electro-optics. The book discusses the fundamental optimization and practical limitations of a number of figures of merit for various optical parameters and gives a clinical appraisal o
""Furnishes table of nonlinear optical properties of organic substances as well as experimental procedures for measuring the nonlinearity of the elements tabulated, including composite materials-offering support for scientists and engineers involved in characterizing, optimizing, and producing materials for manufacturing optical devices.
When nonlinear optical (NLO) effects were first observed experimentally in the early 1960s, the door to a new field of research was opened. Over the last 50 years, this area has expanded rapidly, supported by applications and devices that are based on nonlinear effects. The search for small, and yet fast and highly efficient devices for, e.g., data processing, data storage, or logic gates, is ongoing. Materials with nonlinear optical properties, and in particular organometallic complexes and coordination compounds, have been found to be strong candidates in this area for a number of reasons. An overview of the results that have been published by research groups in this field over the last decade is given in the opening Chapter. Understanding the highly complex physical processes of nonlinear optics, and maximizing these effects to make practical use of them, is a challenge for theoreticians, physicists and chemists. The overlap of these fields enables us to develop models to derive strategies towards building efficient NLO materials. The focus of the present work is on two aspects of ruthenium acetylide complexes incorporating pi-conjugated systems. The first part considers the effects on NLO properties, resulting from lengthening the pi-delocalized system in unbranched octupolar (star-shaped) ruthenium acetylide complexes. Acetylide complexes of bis(bidentate)-ligated Ru have proven to provide desired physical and optical properties; the star-shaped design of the complexes allows access to mono-disperse macromolecular entities that combine large pi-conjugated systems, while incorporating the desired metal centers. In this part of the work, a number of systematically varied octupolar ruthenium acetylide complexes were synthesized and characterized. Their optical and physical properties are discussed, and their nonlinear optical properties were explored by frequency-dependent Z-scan measurements. A variety of new NLO scaling factors are suggested and were applied to NLO data, and the applicability of the new NLO scaling factors was explored. Linear, oligo(phenylethynyl)-bridged ruthenium acetylide complex analogues of the star-shaped complexes were also synthesized, in order to establish the different NLO properties of linear (dipolar) vs. star-shaped (octupolar) arrangements. The second part of this work presents a group of systematically varied mono-disperse, branched ruthenium acetylide complexes (dendrimers). The main interest was the variation of the core unit. Six first-generation organometallic dendrimers with nitrogen, boron, and phenyl cores were synthesized and characterized. The NLO properties of two nitrogen-cored zero-generation dendrimers and an analogous nitrogen-cored first-generation dendrimer were explored; comparison to analogous organic zero-, first- and second-generation dendrimers revealed a drastic enhancement of the NLO properties on incorporation of the metal centers. A number of star-shaped and dendritic mixed-metal osmium-ruthenium acetylide complexes were also synthesized. --provided by Candidate.