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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.
The results of numerical simulations of quantum state evolution in the process of second harmonic generation (SHG) are discussed. It is shown that at a particular moment of time in the fundamental mode initially coherent state turns into a superposition of two macroscopically distinguished states. The question of whether this superposition exhibits quantum interference is analyzed.
A novel diacetylene derivative of 2-Methyl-4-NitroAniline (MNA), a well-known material for Second-Harmonic Generation (SHG), is synthesized. This monomer DiAcetylene MethylNitroAniline, (DAMNA) is characterized by means of the Kurtz technique at 1064 nm and is found to have an SHG powder efficiency 62.5 % that of MNA itself. Thin crystalline films of DAMNA are grown onto quartz, Teflon, and Kapton substrates by means of vapor deposition in vacuum. These films are then polymerized in the solid state by exposure to long-wavelength UV radiation to give crystalline polydiacetylene thin films (PDAMNA). The films are next characterized for SHG, using an unpolymerized DAMNA film as a reference. Interestingly, films grown onto Teflon exhibit greater orientation and significantly greater SHG than those grown onto quartz and Kapton. This result is promising in that it demonstrates the potential of PDAMNA as both a crystalline and polymeric material for SHG applications, in which highly oriented thin films are desired. Computational modeling (usingAM1) is also carried out on DAMNA and is compared to the experimental results.
Bulk single crystals of triethylphosphine sulfide (C2H5)3P(S), a potential nonlinear optical organic material has been grown from melt using Bridgman- Stockbarger method. Commercially available material triethylphosphine sulfide procured from Johnson Matthey was purified by physical vapor transport using low pressure sublimaton (about 30 mTorr). Modified Bridgman-Stockbarger technique is characterized by the smallest possible quantity of product in the melt for a short period of time. The temperature gradient was chosen to be about 10 C/cm and the ampoule was lowering rate was chosen to be 0.2-0.3 mm/h. For various growth conditions, several single crystal of triethylphosphine sulfide have been grown with sizes 10X10X15mm(exp 3). The second harmonic generation (SHG) efficiency was measured and has been found to be comparable to phase matched potassium dihydrogen phosphate crystals. Further characterization of the grown single crystals is in progress and the results will be presented at the symposium.
A search for potential nonlinear optical (NLO) compounds has been performed using the Cambridge Structural Database and molecular modeling. We have studied a series of mono-substituted derivatives of dicyanovinylbenzene as the NLO properties of one of its derivatives (o-methoxy-dicyanovinylbenzene, DIVA) were described earlier. The molecular geometry in the series of the compounds studied was investigated with an X- ray analysis and discussed along with results of molecular mechanics and ab initio quantum chemical calculations. The influence of crystal packing on the molecular planarity has been revealed. Two new compounds from the series studied were found to be active for second harmonic generation (SHG) in the powder. The measurements of SHG efficiency have shown that the o-F- and p-Cl-derivatives of dicyanovinylbenzene are about 10 and 20- times more active than urea, respectively. The peculiarities of crystal structure formation in the framework of balance between the van der Waals and electrostatic interactions have been discussed. The crystal morphology of DIVA and two new SHG-active compounds have been calculated on the basis of their known crystal structures.
In this paper, the status of a high-energy, all solid-state Nd:YAG laser pumped nonlinear optics based UV converter development is discussed. The high-energy UV transmitter technology is being developed for ozone sensing applications from space based platforms using differential lidar technique. The goal is to generate greater than 200 mJ/pulse with 10-50 Hz PRF at wavelengths of 308 nm and 320 nm. A diode-pumped, all-solid-state and single longitudinal mode Nd:YAG laser designed to provide conductively cooled operation at 1064 nm has been built and tested. Currently, this pump laser provides an output pulse energy of >1 J/pulse at 50 Hz PRF and a pulsewidth of 22 ns with an electrical-to-optical system efficiency of greater than 7% and a M(sup 2) value of <2. The single frequency UV converter arrangement basically consists of an IR Optical Parametric Oscillator (OPO) and a Sum Frequency Generator (SFG) setups that are pumped by 532 nm wavelength obtained via Second Harmonic Generation (SHG). In this paper, the operation of an inter cavity SFG with CW laser seeding scheme generating 320 nm wavelength is presented. Efforts are underway to improve conversion efficiency of this mJ class UV converter by modifying the spatial beam profile of the pump laser.
A second-harmonic generator (SHG) serves as the source of the visible laser beam in an onboard calibration scheme for NASA's planned Space Interferometry Mission (SIM), which requires an infrared laser beam and a visible laser beam coherent with the infrared laser beam. The SHG includes quasi-phase-matched waveguides made of MgO-doped, periodically poled lithium niobate, pigtailed with polarization- maintaining optical fibers. Frequency doubling by use of such waveguides affords the required combination of coherence and sufficient conversion efficiency for the intended application. The spatial period of the poling is designed to obtain quasi-phase- matching at a nominal middle excitation wavelength of 1,319.28 nm. The SHG is designed to operate at a warm bias (ambient temperature between 20 and 25 C) that would be maintained in its cooler environment by use of electric heaters; the heater power would be adjusted to regulate the temperature precisely and thereby maintain the required precision of the spatial period. At the state of development at the time of this reporting, the SHG had been packaged and subjected to most of its planned space-qualification tests.
The need for fast electro-optic switches and modulators for optical communication, and laser frequency conversion has created a demand for new second-order non-linear optical materials. One approach to produce such materials is to align chromophores with large molecular hyperpolarizabilities in polymers. Recently fulvenes and benzofulvenes which contain electron donating groups have been shown to exhibit large second-order non-linear optical properties. The resonance structures shown below suggest that intramolecular charge transfer (ICT) should be favorable in omega - (hydroxyphenyl)benzofulvenes and even more favorable in omega-omega - (phenoxy)benzofulvenes because of the enhanced donor properties of the O group. This ICT should lead to enormously enhanced second-order hyperpolarizability. We have prepared all three new omega - (hydroxyphenyl)benzofulvenes by the condensation of indene with the appropriate hydroxyaryl aldehyde in MeOH or MeOH/H2O under base catalysis. In a similar fashion we have prepared substituted benzofulvenes with multipal donor groups. Preliminary studies show that some of our benzofulvene derivatives exhibit second order harmonic generation (SHG). Measurements were carried out by preparing host-guest polymers. The results of our work on benzofulvene derivatives in host-guest polymers when covalently bonded in the polymer will be described.
The stable operation of a mode-locked dye laser synchronously pumped by the second harmonic of an Nd:YAG laser produced in an Nd codoped germanosilicate optical fiber is reported. The optical fiber preparation technique, which results in a second harmonic conversion efficiency of 2 percent, is described. This optical fiber SHG conversion efficiency is the highest reported to date using a continuous-wave mode-locked laser.
Data obtained from the electric field induced second harmonic generation (EFISH) and Kurtz Powder Methods will be provided to MSFC for further refinement of their method. A theoretical model for predicting the second-order nonlinearities of organic salts is being worked on. Another task is the synthesis of a number of salts with various counterions. Several salts with promising SHG activities and new salts will be tested for the presence of two crystalline forms. The materials will be recrystallized from dry and wet solvents and compared for SHG efficiency. Salts that have a high SHG efficiency and no tendency to form hydrates will be documented. The synthesis of these materials are included in this report. A third task involves method to aid in the growth of large, high quality single crystals by solution processes. These crystals will be characterized for their applicability in the fabrication of devices that will be incorporated into optical computers in future programs. Single crystals of optimum quality may be obtained by crystal growth in low-gravity. The final task is the design of a temperature lowering single crystal growth apparatus for ground based work. At least one prototype will be built.
Precise laser remote sensing of aerosol extinction and backscatter in the atmosphere requires a high-power, pulsed, frequency doubled Nd:YAG laser that is wavelength- stabilized to a narrow absorption line such as found in iodine vapor. One method for precise wavelength control is to injection seed the Nd:YAG laser with a low-power CW laser that is stabilized by frequency converting a fraction of the beam to 532 nm, and to actively frequency-lock it to an iodine vapor absorption line. While the feasibility of this approach has been demonstrated using bulk optics in NASA Langley s Airborne High Spectral Resolution Lidar (HSRL) program, an ideal, lower cost solution is to develop an all-waveguide, frequency-locked seed laser in a compact, robust package that will withstand the temperature, shock, and vibration levels associated with airborne and space-based remote sensing platforms. A key technology leading to this miniaturization is the integration of an efficient waveguide frequency doubling element, and a low-voltage phase modulation element into a single, monolithic, planar light-wave circuit (PLC). The PLC concept advances NASA's future lidar systems due to its compact, efficient and reliable design, thus enabling use on small aircraft and satellites. The immediate application for this technology is targeted for NASA Langley's HSRL system for aerosol and cloud characterization. This Phase I effort proposes the development of a potassium titanyl phosphate (KTP) waveguide phase modulator for future integration into a PLC. For this innovation, the proposed device is the integration of a waveguide-based frequency doubler and phase modulator in a single, fiber pigtail device that will be capable of efficient second harmonic generation of 1,064-nm light and subsequent phase modulation of the 532 nm light at 250 MHz, providing a properly spectrally formatted beam for HSRL s seed laser locking system. Fabrication of the integrated PLC chip for NASA Langley, planned for the Phase II effort, will require full integration and optimization of the waveguide components (SHG waveguide, splitters, and phase modulator) onto a single, monolithic device. The PLC will greatly reduce the size and weight, improve electrical- to-optical efficiency, and significantly reduce the cost of NASA Langley s current stabilized HSRL seed laser system built around a commercial off-the-shelf seed laser that is free-space coupled to a bulk doubler and bulk phase modulator.