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A series of organometallic and organic salts, in which the cation has been designed to have a large molecular hyperpolarizability, has been prepared. Variation of the counterion (anion) in many cases leads to materials with large powder second harmonic generation (SHG) efficiencies, the highest of which is roughly 2000 times that of a urea reference.
A series of donor-acceptor acetylene compounds was synthesized in which systematic changes in both the conjugation length and the donor-acceptor strength were made. The effect of these structural changes on the spectroscopic and electronic properties of the molecules and, ultimately, on the measured second-order molecular hyperpolarizabilities (beta) was investigated. It was found that increases in the donor-acceptor strength resulted in increases in the magnitude of beta. For this class of molecules, the increase is dominated by the energy of the intramolecular charge-transfer transition, while factors such as the ground to excited-state dipole moment change and the transition-moment integral are much less important. Increasing the conjugation length from one to two acetylene linkers did not result in an increase in the value of beta; however, beta increased sharply in going from two acetylenes to three. This increase is attributed to the superposition of several nearly isoenergetic excited states.
The number of pixels per unit area sampling an image determines Nyquist resolution. Therefore, the highest pixel density is the goal. Unfortunately, as reduction in pixel size approaches the wavelength of light, sensitivity is lost and noise increases. Animals face the same problems and have achieved novel solutions. Emulating these solutions offers potentially unlimited sensitivity with detector size approaching the diffraction limit. Once an image is 'captured', cellular preprocessing of information allows extraction of high resolution information from the scene. Computer simulation of this system promises hyperacuity for machine vision.
It has been proposed that NLO thin film properties may be improved by low-gravity processing. Strong candidates for NLO thin film applications are the polythiophenes. Polymeric thiophenes are attractive materials due to their ease of preparation, stability, and high X(exp 3). A simple and convenient method for preparation of polythiophenes is electrochemical oxidation. We will apply some of our experience and lessons learned in low-gravity metal, metal/cermet electrode position to improve the quality of polythiophene(s) thin films. In low gravity electrode position of Ni at a high rate on an Au substrate often results in the production of an x-ray non diffracting surface. Cobalt metal deposition does not give this result nor does Ni when deposited similarly on a glassy carbon substrate. Co/Ni alloy composition produced during electrode position is strongly dependent upon the amount of convection. Code position of neutral inert cermets with metals is influenced significantly by the presence of gravity and the size of the cermets. Tracks left in the 1-g surfaces by unsuccessful particle occlusion indicate suspension of the large particles is not the only reason for poor volume percentages of the larger particles in the deposits. All size particles are more homogeneously distributed in the deposits in low-gravity electrocodeposition than in 1-g. Low gravity gives larger volume percentages for the larger particles in the deposits, while 1-g gives larger volume percentages for the smaller particles. Intermediate size particles give mixed results. The experimental cells were constructed with flat electrode end plates such that 1-g bench reference electrode positions could be carried out at various orientations with respect to gravity. A series of bench studies using similar designed cells are suggested so that convection modification can be applied to electrochemical thin film preparation. Convection effects can then be coupled with other parameter variations in current, temperature, concentration, solvent, electrolyte, and anode substrates to optimize the properties of NLO thin films before resorting to low-gravity processing.
One aspect of this project involves a collaborative effort with the Solid State Division of ORNL. The thrust behind this research is to develop ion implantion for synthesizing novel materials (quantum dots wires and wells, and metal colloids) for applications in all optical switching devices, up conversion, and the synthesis of novel refractory materials. In general the host material is typically a glass such as optical grade silica. The ions of interest are Au, Ag, Cd, Se, In, P, Sb, Ga and As. An emphasis is placed on host guest interactions between the matrix and the implanted ion and how the matrix effects and implantation parameters can be used to obtain designer level optical devices tailored for specific applications. The specific materials of interest are: CdSe, CdTe, InAs, GaAs, InP, GaP, InSb, GaSb and InGaAs. A second aspect of this research program involves using porous glass (25-200 A) for fabricating materials of finite size. In this part of the program, we are particularly interested in characterizing the thermodynamic and optical properties of these non-composite materials. We also address how phase diagram of the confined material is altered by the interfacial properties between the confined material and the pore wall.
Phase 1 of this work involved design work on a momentum transfer device. The progress on design and testing will be presented. Phase 2 involved the systematic study of the MPD thruster for dual uses. Though it was designed as a thruster for space vehicles, the characteristics of the plasma make it an excellent candidate for industrial applications. This project sought to characterize the system for use in materials processing and characterization. The surface modification on ZnCdTe, CdTe, and ZnTe will be presented. Phase 3 involved metal colloids and semiconductor quantum dots. One aspect of this project involves a collaborative effort with the Solid State Division of ORNL. The thrust behind this research is to develop ion implantation for synthesizing novel materials (quantum dots wires and wells, and metal colloids) for applications in all optical switching devices, up conversion, and the synthesis of novel refractory materials. The ions of interest are Au, Ag, Cd, Se, In, P, Sb, Ga, and As. The specific materials of interest are: CdSe, CdTe, InAs, GaAs, InP, GaP, InSb, GaSb, and InGaAs. A second aspect of this research program involves using porous glass (25-200 A) for fabricating materials of finite size. The results of some of this work will also be reported.
A new process for producing large bulk single crystals of benzil (C6H5COCOC6H5) is reported in this paper. Good quality crystals have been successfully grown using this approach to crystal growth. This method seems to be very promising for other thermally stable NLO organic materials also. The entire contents vycor crucible 1.5 inch in diameter and 2 inch deep was converted to single crystal. Purity of the starting growth material is also an important factor in the final quality of the grown crystals. The entire crystal can be very easily taken out of the crucible by simple maneuvering. Initial characterization of the grown crystals indicated that the crystals are as good as other crystals grown by conventional Bridgman Stockbarger technique.
The molecular polarizability characteristics for a large series of naphthoquinone and quinoline derivatives have been calculated. The dependence of calculated hyperpolarizability on the positions and the number of donor and acceptor substituents is discussed.
A series of novel NLO (chromophores) imidazole chromophores containing tricyanovinyl acceptor coupled with thiophene have been developed.
A qualitative model explaining sharp spectral peaks in emission of solid-state random laser materials with broad-band gain is proposed. The suggested mechanism of coherent emission relies on synchronization of phases in an ensemble of emitting centers, via time delays provided by a network of random scatterers, and amplification of spontaneous emission that supports the spontaneously organized coherent state. Laser-like emission from powders of solid-state luminophosphors, characterized by dramatic narrowing of the emission spectrum and shortening of emission pulses above the threshold, was first observed by Markushev et al. and further studied by a number of research groups. In particular, it has been shown that when the pumping energy significantly exceeds the threshold, one or several narrow emission lines can be observed in broad-band gain media with scatterers, such as films of ZnO nanoparticles, films of pi-conjugated polymers or infiltrated opals. The experimental features, commonly observed in various solid-state random laser materials characterized by different particle sizes, different values of the photon mean free path l*, different indexes of refraction, etc.. can be described as follows. (Liquid dye random lasers are not discussed here.)
Electro-Optic Polymers hold great promise in increased electro-optic coefficients as compared to their inorganic corollaries. Many researchers have focused on quantum chemistry to describe how the dipoles respond to temperature and electric fields. Much work has also been done for single layer films to confirm these results. For optical applications, waveguide structures are utilized to guide the optical waves in 3 layer stacks. Electrode poling is the only practical poling method for these structures. This research takes an electrical engineering approach to develop poling models and electrical and optical transfer functions of the waveguide structure. The key aspect of the poling model is the large boundary charge density deposited during the poling process. The boundary charge density also has a large effect on the electrical transfer function which is used to explain the transient response of the system. These models are experimentally verified. Exploratory experiment design is used to study poling parameters including time, temperature, and voltage. These studies verify the poling conditions for CLDX/APC and CLDZ/APEC guest host electro optic polymer films in waveguide stacks predicted by the theoretical developments.
A review is presented describing our recent work to correlate the first hyperpolarizability, of organic materials with the molecular parameter bond length alternation (BLA). Donor-acceptor polyenes displaying a wide BLA range were synthesized.
Compositions for use in non-linear optical devices. The compositions have first molecular electronic hyperpolarizability (.beta.) either positive or negative in sign and therefore display second order non-linear optical properties when incorporated into non-linear optical devices.
An application of focal-plane imaging that can be used as a real time diagnostic of beam crossing in various optical techniques is reported. We discuss two specific versions and demonstrate the capability of maximizing system performance with an example in a combined dual-pump coherent anti-Stokes Raman scattering interferometric Rayleigh scattering experiment (CARS-IRS). We find that this imaging diagnostic significantly reduces beam alignment time and loss of CARS-IRS signals due to inadvertent misalignments.
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The present conference on novel optoelectronics discusses topics in the state-of-the-art in this field in the Netherlands, quantum wells, integrated optics, nonlinear optical devices and fiber-optic-based devices, ultrafast optics, and nonlinear optics and optical bistability. Attention is given to the production of fiber-optics for telecommunications by means of PCVD, lifetime broadening in quantum wells, nonlinear multiple quantum well waveguide devices, tunable single-wavelength lasers, an Si integrated waveguiding polarimeter, and an electrooptic light modulator using long-range surface plasmons. Also discussed are backward-wave couplers and reflectors, a wavelength-selective all-fiber switching matrix, the impact of ultrafast optics in high-speed electronics, the physics of low energy optical switching, and all-optical logical elements for optical processing.
All-optical modulation using inherent third-order optical nonlinearity of a medium has garnered considerable interest in photonics and optoelectronics. Herein, nonlinear optical (NLO) properties of tellurite glasses and glass ceramics (GCs) containing four different rare earths (RE = La, Gd, Lu, and Y) have been deliberated in near-infrared regions under an ultrafast regime. The La-based glass exhibits ~10 times higher nonlinear refraction (n 2 ) and absorption (α 2 ) than reported NLO materials. The NLO susceptibility [χ (3) ] trend in the studied glasses is La > Gd > Lu > Y, matching with RE 3+ polarizability. Furthermore, Ln 2 Te 6 O 15 nanocrystallite-embedded transparent GCs exhibit a larger NLO coefficient due to the enhanced local field from oxygen vacancies in crystallites. Interestingly, the trend of χ (3) in GCs follows the sequence of Y > Lu > Gd > La, precisely opposite to the glasses. This observation challenges the general polarizability approach of RE 3+ ions, emphasizing that quadratic hyperpolarizability of RE 3+ is pivotal for NLO properties of GCs. Among the studied matrices, Y-containing GCs showed the lowest optical limiting (OL) threshold (5.4 mJ/cm 2 at 800 nm), much lower than those of the reported NLO materials, suggesting its potential as a femtosecond NIR-laser safety material. A combination of large α 2 and n 2 from the studied matrices indicates their advantage for harmonic generation, potentially aiding in the design of ultrafast signal processing devices.
Gold nanoparticle composites are known to display large optical nonlinearities. In order to assess the validity of generalized effective medium theories (EMT's) for describing the linear and nonlinear optical properties of metal nanoparticle composites, knowledge of the linear and nonlinear susceptibilities of the constituent materials is a prerequisite. In this study the inherent nonlinearity of the metal is measured directly (rather than deduced from a suitable EMT) using a very thin gold film. Specifically, we have used the z-scan technique at a wavelength near the transmission window of bulk gold to measure the third-order susceptibility of a continuous thin gold film deposited on a quartz substrate surface-modified with a self-assembled monolayer to promote adhesion and uniformity without affecting the optical properties. We compare our results with predictions which ascribe the nonlinear response to a Fermi-smearing mechanism. Further, we note that the sign of the nonlinear susceptibility is reversed from that of gold nanoparticle composites.