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NASA NTRS1998

Photonic and Opto-Electronic Applications of Polydiacetylene Films Photodeposited from Solution and Polydiacetylene Copolymer Networks

Polydiacetylenes (PDAS) are attractive materials for both electronic and photonic applications because of their highly conjugated electronic structures. They have been investigated for applications as both one-dimensional (linear chain) conductors and nonlinear optical (NLO) materials. One of the chief limitations to the use of PDAs has been the inability to readily process them into useful forms such as films and fibers. In our laboratory we have developed a novel process for obtaining amorphous films of a PDA derived from 2-methyl4-nitroaniline using photodeposition with Ultraviolet (UV) light from monomer solutions onto transparent substrates. Photodeposition from solution provides a simple technique for obtaining PDA films in any desired pattern with good optical quality. This technique has been used to produce PDA films that show potential for optical applications such as holographic memory storage and optical limiting, as well as third-order NLO applications such as all-optical refractive index modulation, phase modulation and switching. Additionally, copolymerization of diacetylenes with other monomers such as methacrylates provides a means to obtain materials with good processibility. Such copolymers can be spin cast to form films, or drawn by either melt or solution extrusion into fibers. These films or fibers can then be irradiated with UV to photopolymerize the diacetylene units to form a highly stable cross-linked PDA-copolymer network. If such films are electrically poled while being irradiated, they can achieve the asymmetry necessary for second-order NLO applications such as electro-optic switching. On Earth, formation of PDAs by the above mentioned techniques suffers from defects and inhomogeneities caused by convective flows that can arise during processing. By studying the formation of these materials in the reduced-convection, diffusion-controlled environment of space we hope to better understand the factors that affect their processing, and thereby, their nature and properties. Ultimately it may even be feasible to conduct space processing of PDAs for technological applications.

Paley, Mark S.↗

NASA NTRS1998

Development of Polyimides-Based NLO Materials for Electrooptical Applications

Development of thermally stable optical materials for nonlinear optics have recently focused on the covalent incorporation of NLO chromophores into high performance polymers, especially thermally stable and processable polyamides. One key aspect for the incorporation of robust NLO chromophores into high Tg polymers is to sustain poling induced order. Other advantages include high loading level of chromophores, and elimination of possible phase separation as well as chromophore sublimation at processing or working temperature. We have prepared several polyimide based polymers which are covalently linked with thermally stable chromophores that we have developed, since polyamides generally exhibit high Tg and good film transparency. Here, we report the development and subsequent incorporation of indoline based chromophores into polyamides, leading to thermally stable NLO polymers.

Rutherford, Jacqueline↗

NASA NTRS1996

Superconductivity Devices: Commercial Use of Space

The work described in this report covers various aspects of the Rainbow solid-state actuator and sensor technologies. It is presented in five parts dealing with sensor applications, nonlinear properties, stress-optic and electrooptic properties, stacks and arrays, and publications. The Rainbow actuator technology is a relatively new materials development which had its inception in 1992. It involves a new processing technique for preparing pre-stressed, high lead containing piezoelectric and electrostrictive ceramic materials. Ceramics fabricated by this method produce bending-mode actuator devices which possess several times more displacement and load bearing capacity than present-day benders. Since they can also be used in sensor applications, Rainbows are part of the family of materials known as smart ceramics. During this period, PLZT Rainbow ceramics were characterized with respect to their piezoelectric properties for potential use in stress sensor applications. Studies of the nonlinear and stress-optic/electrooptic birefringent properties were also initiated during this period. Various means for increasing the utility of stress-enhanced Rainbow actuators are presently under investigation.

Haertling, Gene↗

DOE OSTI2023

Resonance Effect in Brunel Harmonic Generation in Thin Film Organic Semiconductors

Abstract Nonlinear optical properties of organic semiconductors (OSCs) have been extensively investigated in the perturbative regime, while strong light induced high‐order processes in solid‐state OSCs are less studied. Here, below‐threshold harmonic generation is examined, both experimentally and theoretically, in two solid‐state thin film OSCs, that is, tetraphenylporphyrin and zinc tetraphenylporphyrin. Results show that the π–π* excitations of the porphyrin ring system generate the harmonic emission. The contribution of the Brunel harmonic to the 5th harmonic emission is uncovered, where the resonant 5‐photon transition ( S 0 → S 2 transition) is found to lead to an early onset of non‐perturbative behavior. A similar resonance effect is expected in Brunel harmonic generation in other organic materials.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Angle-resolved nonresonant two-photon single ionization of argon using 9.3-eV photons produced via high-order harmonic generation

Here we present an experimental study on the photoionization dynamics of nonresonant one-color two-photon single valence ionization of neutral argon atoms. Using 9.3-eV photons produced via high harmonic generation and a three-dimensional momentum imaging spectrometer, we detect the photoelectrons and ions produced from nonresonant two-photon ionization in coincidence. Photoionization from the $3p$ orbital produces a photoelectron scattering wave function with $p$- and $f$-partial-wave components, which interfere and result in a photoelectron angular distribution with peak amplitude perpendicular to the vacuum ultraviolet polarization. The comparison between the present results and the two previous sets of theoretical calculations [Phys. Rev. A 44, 324 (1991), and J. Phys. B: At. Mol. Phys. 16, 2737 (1983)] indicates that electron-electron correlation contributes appreciably to the two-photon ionization dynamics.

74 ATOMIC AND MOLECULAR PHYSICS↗

NASA NTRS2007

Recent Advances in Photonic Devices for Optical Computing and the Role of Nonlinear Optics-Part II

The twentieth century has been the era of semiconductor materials and electronic technology while this millennium is expected to be the age of photonic materials and all-optical technology. Optical technology has led to countless optical devices that have become indispensable in our daily lives in storage area networks, parallel processing, optical switches, all-optical data networks, holographic storage devices, and biometric devices at airports. This chapters intends to bring some awareness to the state-of-the-art of optical technologies, which have potential for optical computing and demonstrate the role of nonlinear optics in many of these components. Our intent, in this Chapter, is to present an overview of the current status of optical computing, and a brief evaluation of the recent advances and performance of the following key components necessary to build an optical computing system: all-optical logic gates, adders, optical processors, optical storage, holographic storage, optical interconnects, spatial light modulators and optical materials.

Abdeldayem, Hossin↗

DOE OSTI2024

Statistical mechanics and pressure of composite multimoded weakly nonlinear optical systems

Statistical mechanics can provide a versatile theoretical framework for investigating the collective dynamics of weakly nonlinear-wave settings that can be utterly complex to describe otherwise. In optics, composite systems arise due to interactions between different frequencies and polarizations. The purpose of this work is to develop a thermodynamic theory that takes into account the synergistic action of multiple components. We find that the type of the nonlinearity involved can have important implications in the thermalization process and, hence, can lead to different thermal equilibrium conditions. Importantly, we derive closed-form expressions for the actual optomechanical pressure that is exerted on the system. In particular, the total optomechanical pressure is the sum of the partial pressures due to each component. Our results can be applied to a variety of weakly nonlinear optical settings such as multimode fibers, bulk waveguides, photonic lattices, and coupled microresonators. We present two specific examples, where two colors interact in a one-waveguide array with either a cubic or quadratic nonlinearity.

Efremidis, Nikolaos K. (ORCID:0000000298300268)↗

DOE OSTI2022

Gamma-radiation-induced negative nonlinear absorption in quartz glass

The effect of ionizing radiation on the nonlinear optical properties of materials needs to be considered for applications that employ high-power laser pulses in extreme radiation environments. The Heraeus Infrasil302 optical quartz glass was irradiated by gamma rays, and its nonlinear absorption was measured using the open-aperture Z-scan technique with nanosecond laser pulses. Irradiation results in a negative nonlinear absorption coefficient whose magnitude increases with irradiation dose. Nonlinear absorption coefficients of -0.78, -1.14, -1.29, and -1.88~ × ~10 -13 m/W are measured for gamma doses of 600 krad, 1.2 Mrad, 3.6 Mrad, and 10 Mrad, respectively. Thermal annealing restores the optical properties of quartz-glass to their unirradiated values. It is suggested that metallic impurities introduced by the manufacturing process have a role in inducing saturated absorption in irradiated quartz glass, which manifests as negative nonlinear absorption coefficient, and is demonstrated by comparing Infrasil302 quartz results to equivalent irradiated measurements for Spectrosil2000 quartz.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2021

Anomalous two-photon Compton scattering

Abstract X-ray free-electron lasers can generate radiation pulses with extreme peak intensities at short wavelengths. This enables the investigation of laser–matter interactions in a regime of high fields, yet at a non-relativistic ponderomotive potential, where ordinary rules of light–matter interaction may no longer apply and nonlinear processes are starting to become observable. Despite small cross-sections, first nonlinear effects in the hard x-ray regime have recently been observed in solid targets, including x-ray-optical sum-frequency generation (XSFG), x-ray second harmonic generation (XSHG) and two-photon Compton scattering (2PCS). Nonlinear interactions of bound electrons in the x-ray range are fundamentally different from those dominating at optical frequencies. Whereas in the optical regime nonlinearities are predominantly caused by anharmonicities of the atomic potential in the chemical bonds, x-ray nonlinearities far above atomic resonances are expected to be due to nonlinear oscillations of quasi-free electrons, including inner-shell atomic electrons. While the quasi-free-electron model agrees reasonably well with the experimental data for XSFG and XSHG, 2PCS measurements have led to unexpected results: the energy of the nonlinearly scattered photons from non-relativistic electrons shows a substantial unexpected red shift in addition to the Compton shift that is well beyond that predicted by a nonlinear quantum electrodynamics model for free electrons. A potential explanation for the spectral broadening is based on a previously unexplored scattering process that involves the whole atom rather than just quasi-free electrons. A first simulation that includes the atomic binding potential was successful in describing a broadening of the spectrum of the nonlinearly scattered photons to longer wavelengths for soft x-rays. However, the same model does not show any broadening at hard x-ray wavelengths, which is in agreement with other simulation approaches. To this point no calculation has been able to reproduce the experimentally observed broadening. Here we present further experimental data of 2PCS for an extended parameter range using additional diagnostics. In particular, we present measurements of the electron momentum distribution during the interaction that strongly suggest that the spectral broadening is not caused by an increased plasma temperature. We extend our measurement of the magnitude of the red shift in beryllium to > 1.9 k e V in addition to the Compton shift expected for free electrons and expand the measurement of the angular distribution to include forward scattering angles. We also present first measurements of 2PCS from diamond.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

NASA NTRS1981

Role of optical computers in aeronautical control applications

The role that optical computers play in aircraft control is determined. The optical computer has the potential high speed capability required, especially for matrix/matrix operations. The optical computer also has the potential for handling nonlinear simulations in real time. They are also more compatible with fiber optic signal transmission. Optics also permit the use of passive sensors to measure process variables. No electrical energy need be supplied to the sensor. Complex interfacing between optical sensors and the optical computer is avoided if the optical sensor outputs can be directly processed by the optical computer.

Baumbick, R. J.↗

NASA NTRS1985

ICIASF '85 - International Congress on Instrumentation in Aerospace Simulation Facilities, 11th, Stanford University, CA, August 26-28, 1985, Record

Developments related to laser Doppler velocimetry are discussed, taking into account a three-component dual beam laser-Doppler-anemometer to be operated in large wind tunnels, a new optical system for three-dimensional laser-Doppler-anemometry using an argon-ion and a dye laser, and a two-component laser Doppler velocimeter by switching fringe orientation. Other topics studied are concerned with facilities, instrumentation, control, hot wire/thin film measurements, optical diagnostic techniques, signal and data processing, facilities and adaptive wall test sections, data acquisition and processing, ballistic instrument systems, dynamic testing and material deformation measurements, optical flow measurements, test techniques, force measurement systems, and holography. Attention is given to nonlinear calibration of integral wind tunnel balances, a microcomputer system for real time digitized image compression, and two phase flow diagnostics in propulsion systems.

Source record↗

NASA NTRS1988

A review of melt and vapor growth techniques for polydiacetylene thin films for nonlinear optical applications

Methods for the growth of polydiacetylene thin films by melt and vapor growth and their subsequent polymerization are summarized. Films with random orientations were obtained when glass or quartz were used as substrates in the vapor growth process. Oriented polydiacetylene films were fabricated by the vapor deposition of diacetylene monomer onto oriented polydiacetylene on a glass substrate and its subsequent polymerization by UV light. A method for the growth of oriented thin films by a melt-shear growth process as well as a method of film growth by seeded recrstallization from the melt between glass plates, that may be applied to the growth of polydiacetylene films, are described. Moreover, a method is presented for the fabrication of single crystal thin films of polyacetylenes by irradiation of the surface of diacetylene single crystals to a depth between 100 and 2000 angstroms.

Penn, B. G.↗

NASA NTRS1991

Growth of bulk single crystals of organic materials for nonlinear optical devices - An overview

Highly perfect single crystals of nonlinear optical organic materials are required for use in optical devices. An overview of the bulk crystal growth of these materials by melt, vapor, and solution processes is presented. Additionally, methods that may be used to purify starting materials, detect impurities at low levels, screen materials for crystal growth, and process grown crystals are discussed.

Penn, Benjamin G.↗

DOE OSTI2021

Impact of Photon Recycling, Grain Boundaries, and Nonlinear Recombination on Energy Transport in Semiconductors

Energy carrier transport and recombination in semiconductors can be directly monitored with optical microscopy, revealing key insights into fundamental photophysics and informs efficient optoelectronic device design. Oftentimes, energy transport is measured by monitoring a time-resolved expanding carrier profile after optical excitation under a focused laser beam. Although this approach has gained widespread adoption, the presence of competing dynamic processes, such as diffusion and photon recycling, has made it difficult to accurately extract and understand important semiconductor properties. Here, we develop and apply a new framework for modeling energy transport in both excitonic and free carrier semiconductors. Here, we demonstrate that processes such as nonlinear recombination and photon recycling can have a significant impact on the apparent energy carrier profiles, especially for excitonic materials with short radiative lifetimes. Additionally, we find that film microstructure can lead to unique transport profiles that strongly depends on material boundary behavior and the difference between feature size and diffusion length. Here, these findings provide a deeper understanding of energy transport in semiconducting materials and provide new strategies for the design and optimization of electronic and optoelectronic devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1992

Nondestructive measurement of intensity of optical fields using spontaneous parametric down conversion

Results of nondestructive measurements of intensity (photons per mode) of light from different sources are discussed. The procedure of measurement does not destroy the state of the optical field. The method is based on using the second order nonlinearity of crystal media lacking a center of symmetry and the nonclassical properties of the process of Spontaneous Parametric Down Conversion (SPDC).

Penin, A. N.↗

NASA NTRS1999

Coherent Pump-Probe Interactions and Terahertz Intersubband Gain in Semiconductor Quantum Wells

In recent years there has been considerable interest in intersubband-transition-based infrared semiconductor quantum well (QW) lasers because of their potential applications. In the mid-infrared range, both electrically-injected quantum cascade lasers [1] and optically-pumped multiple QW lasers [2] have been experimentally realized. In these studies, optical gain is due to population inversion between the lasing subbands. It was also proposed that stimulated Raman scattering in QW systems can produce net infrared optical gain [3j. In such a nonlinear optical scheme, the appearance of optical gain that may lead to intersubband Raman lasers does not rely on the population inversion. Since, in tile resonant Raman process (Raman gain is the largest in this case), the pump field induces population redistribution among subbands in the QW s ystem, it seems that a realistic estimate of the optical gain has to include this effect. Perturbative calculations used in the previous work [3] may overestimate the Raman gain. In this paper we present a nonperturbative calculation of terahertz gain of optically-pumped semiconductor step quantum wells. Limiting optical transitions within the conduction band of QW, we solve the pump-field-induced nonequilibrium distribution function for each subband of the QW system from a set of coupled rate equations. Both intrasubband and intersubband relaxation processes in the quantum well system are included. Taking into account the coherent interactions between pump and THz (signal) waves, we we derive the susceptibility of the QW system for the THz field. For a GaAs/AlGaAs step QW, we calculate the Thz gain spectrum for different pump frequencies and intensities. Under moderately strong pumping (approximately 0.3 MW/sq cm), a significant THz gain (approximately 300/m) is predicted. It is also shown that the coherent wave interactions (resonant stimulated Raman processes) contribute significantly to the THz gain.

Liu, Ansheng↗

NASA NTRS1988

Study of nonlinear optical sBs phenomena in mid IR fibers

This is the first reported attempt at investigation of the sBs phenomena in mid IR fibers using externally fed or laser self generated low frequency and microwave frequency phonon waves as diagnostic probes of such processes. The observation of laser excited phonon emissions in the mid IR fiber and direct modulation of CO2 laser pulse transmission by externally imposed low frequency radiation is the first indication of the predicted low sBs threshold in these fibers in the phonon rich mid IR spectral region. The prospect of wide applications of the sBs process in optical switching, phase conjugation and ultimately optical computing and possible deleterious effects in mid IR laser heterodyne spectroscopy, sideband modulation and transmitted power limitation is discussed.

Yu, Chung↗

NASA NTRS2008

Microwave-to-Optical Conversion in WGM Resonators

Microwave-to-optical frequency converters based on whispering-gallery-mode (WGM) resonators have been proposed as mixers for the input ends of microwave receivers in which, downstream of the input ends, signals would be processed photonically. A frequency converter as proposed (see figure) would exploit the nonlinearity of the electromagnetic response of a WGM resonator made of LiNbO3 or another suitable ferroelectric material. Up-conversion would take place by three-wave mixing in the resonator. The WGM resonator would be de - signed and fabricated to obtain (1) resonance at both the microwave and the optical operating frequencies and (2) phase matching among the input and output microwave and optical signals as described in the immediately preceding article. Because the resonator would be all dielectric there would be no metal electrodes signal losses would be very low and, consequently, the resonance quality factors (Q values) of the microwave and optical fields would be very large. The long lifetimes associated with the large Q values would enable attainment of high efficiency of nonlinear interaction with low saturation power. It is anticipated that efficiency would be especially well enhanced by the combination of optical and microwave resonances in operation at input signal frequencies between 90 and 300 GHz.

Savchenkov, Anatoliy↗