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At least 55 records · Page 3

Gradient-based optimization of complex nanoparticle heterostructures enabled by deep learning on heterogeneous graphs

Applications of deep learning (DL) to design nanomaterials are hampered by a lack of suitable data representations and training data. Here, in this study, we report efforts to overcome these limitations and leverage DL to optimize the nonlinear optical properties of core–shell upconverting nanoparticles (UCNPs). UCNPs, which have applications in fields such as biosensing, super-resolution microscopy and three-dimensional printing, can emit visible and ultraviolet light from near-infrared excitations. We report a large-scale dataset of UCNP emission spectra based on accurate but expensive kinetic Monte Carlo simulations (N > 6,000) and use these data to train a heterogeneous graph neural network using a physically motivated representation of UCNP nanostructure. Applying gradient-based optimization on the trained graph neural network, we identify structures with 6.5× higher predicted emission under 800-nm illumination than any UCNP in our training set. Our work reveals design principles for UCNP heterostructures and presents a roadmap for DL-based inverse design of nanomaterials.

Sivonxay, Eric [Lawrence Berkeley National Laborat

Novel photovoltaic delta-doped GaAs superlattice structure

An asymmetric delta-doped GaAs structure is described which exhibits novel photovoltaic effects and low-intensity nonlinear optics. Of particular interest in this kind of structure is the ability to design the electrooptical and nonlinear optical properties and the material response time over a wide range by appropriate design of the doping profile.

Glass, A. M.

Compounds Generate Optical Second Harmonics

Newly synthesized organic salts found to generate relatively large second-harmonic signals when illuminated by fundamental signals in near-infrared spectrum. Made by crystallizing, with appropriate counterions, organic ions having large molecular hyperpolarizibilities. Large second-order nonlinear susceptibilities observed. These and other compounds having large nonlinear optical properties used in electro-optical modulators, switches, and signal-processing equipment.

Marder, Seth R.

Bulk Electro-Optical Polymer Component

Polymer serves in high-voltage sensors and laser-beam modulators. Electro-optical polymer of relatively low cost formed as bulk specimen from azo dye 4-(4-nitrophenylazo)-N-ethyl, N-2-hydroxyethylaniline, also known as Disperse Red 1 or DR1, and transparent epoxy. More stable than prior electro-optical polymers based on DR1 and poly(methylmethacrylate). If polymer were sandwiched between electrodes, it provides direct measurement of high voltage via electro-optical effect. Has significant nonlinear optical properties. Material useful in microelectronics, micro-optics, integrated optics, and testing of materials. Polymer withstands electric fields up to 120 kV/cm.

Gottsche, Allan

Optical Computers and Space Technology

The rapidly increasing demand for greater speed and efficiency on the information superhighway requires significant improvements over conventional electronic logic circuits. Optical interconnections and optical integrated circuits are strong candidates to provide the way out of the extreme limitations imposed on the growth of speed and complexity of nowadays computations by the conventional electronic logic circuits. The new optical technology has increased the demand for high quality optical materials. NASA's recent involvement in processing optical materials in space has demonstrated that a new and unique class of high quality optical materials are processible in a microgravity environment. Microgravity processing can induce improved orders in these materials and could have a significant impact on the development of optical computers. We will discuss NASA's role in processing these materials and report on some of the associated nonlinear optical properties which are quite useful for optical computers technology.

Abdeldayem, Hossin A.

Poling of Microwave Electro-Optic Devices

The desire to transmit high frequency, microwave RF signals over fiber optic cables has necessitated the need for electro-optic modulation devices. However, in order to reap these potential benefits, it is necessary to develop the devices and their associated fabrication processes, particularly those processes associated with the poling of the devices. To this end, we entered into a cooperative research agreement with Richard Kunath of NASA LeRC. A graduate student in my group, Tony Kowalczyk, worked closely with the group at NASA to develop processes for construction of a microwave frequency electro-optic modulator. Materials were commercially obtained from Amoco Chemical and in collaboration with Lockheed-Martin. The photolithography processes were developed at NASA LeRC and the electric-field poling process was carried out in our laboratory at CWRU. During the grant period, the poling process conditions were investigated for these multilayer devices. Samples were poled and the resulting nonlinear optical properties were evaluated in our laboratory. Following the grant period, Kowalczyk went to NASA under a NRC fellowship, and I continued to collaborate as a consultant. Publications listed at the end of this report came out of this work. Another manuscript is in preparation and will be submitted shortly.

Singer, Kenneth D.

Fabrication and Characterization of Thin Film Ion Implanted Composite Materials for Integrated Nonlinear Optical Devices

Ion implantation has been shown to produce a high density of metal colloids within the layer regions of glasses and crystalline materials. The high-precipitate volume fraction and small size of metal nanoclusters formed leads to values for the third-order susceptibility much greater than those for metal doped solids. This has stimulated interest in use of ion implantation to make nonlinear optical materials. On the other side, LiNbO3 has proved to be a good material for optical waveguides produced by MeV ion implantation. Light confinement in these waveguides is produced by refractive index step difference between the implanted region and the bulk material. Implantation of LiNbO3 with MeV metal ions can therefore result into nonlinear optical waveguide structures with great potential in a variety of device applications. We describe linear and nonlinear optical properties of a waveguide structure in LiNbO3-based composite material produced by silver ion implantation in connection with mechanisms of its formation.

Sarkisov, S.

Structure Orientation in Phthalocyanine Film Growth by Vapor Deposition in Electrical Fields

Films of phthalocyanines were grown by vapor deposition in an electric field on to quartz substrates coated with a very thin layer of gold or indium tin oxide and compared to films grown in the absence of an electric field. A comparison of morphology, nonlinear optical properties, and crystal structure was also made. The films were characterized using scanning electron microscopy, x-ray diffraction, and FTIR. Films grown in the absence of an electric field had a fiber like morphology and those grown in electric fields having a maximum strength of 4000 V/cm had a dense-columnar structure. The crystal structure of films grown in an electric field was different than those grown in the absence of a field.

Banks, C. E.

Enhancement of Optical Nonlinearities in Composite Media and Structures via Local Fields and Electromagnetic Coupling Effects

This talk will review the linear and nonlinear optical properties of metal nanoparticles and dielectric microparticles, with an emphasis on local field effects, and whispering gallery modes (WGMs), as well as the conjunction of these two effects for enhanced Raman. In particular, enhanced optical properties that result from electromagnetic coupling effects will be discussed in the context of Mie scattering from concentric spheres and bispheres. Predictions of mode splitting and photonic bandgaps in micro-spheres will be presented and will be shown to be analogous to effects that occur in coupled resonator optical waveguides (CROW). Slow and fast light in SCISSOR / CROW configurations will also be discussed.

Smith, David D.

Unconventional Imaging with Contained Granular Media

Typically, the cost of a space-borne imaging system is driven by the size and mass of the primary aperture. The solution that we propose uses a method to construct an imaging system in space in which the nonlinear optical properties of a cloud of micron-sized particles, shaped into a specific surface by electromagnetic means, and allows one to form a very large and lightweight aperture of an optical system, hence reducing overall mass and cost. Recent work at JPL has investigated the feasibility of a granular imaging system, concluding that such a system could be built and controlled in orbit. We conducted experiments and simulation of the optical response of a granular lens. In all cases, the optical response, measured by the Modulation Transfer Function, of hexagonal reflectors was closely comparable to that of a conventional spherical mirror. We conducted some further analyses by evaluating the sensitivity to fill factor and grain shape, and found a marked sensitivity to fill factor but no sensitivity to grain shape. We have also found that at fill factors as low as 30%, the reflection from a granular lens is still excellent. Furthermore, we replaced the monolithic primary mirror in an existing integrated model of an optical system (WFIRST Coronagraph) with a granular lens, and found that the granular lens that can be useful for exoplanet detection provides excellent contrast levels. We will present our testbed and simulation results in this paper.

Sidick, Erkin

Reverse Polarizability of Rare Earth Ions (La 3+ , Gd 3+ , Lu 3+ , Y 3+ ) in Tellurite Glasses and Glass Ceramics for Optical Limiting

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.

36 MATERIALS SCIENCE

Preparation of polymeric diacetylene thin films for nonlinear optical applications

A method for producing polymeric diacetylene thin films having desirable nonlinear optical characteristics has been achieved by producing amorphous diacetylene polymeric films by simultaneous polymerization of diacetylene monomers in solution and deposition of polymerized diacetylenes on to the surface of a transparent substrate through which ultraviolet light has been transmitted. These amorphous polydiacetylene films produced by photo-deposition from solution possess very high optical quality and exhibit large third order nonlinear optical susceptibilities, such properties being suitable for nonlinear optical devices such as waveguides and integrated optics.

Frazier, Donald O.

A database for solid-state laser, optical, and nonlinear materials

The database contains the physical properties of laser, optical, and nonlinear materials used by the laser models of a laser-modeling software system. The database is subdivided into two parts: spectra and tabulated data. The spectra are ASCII files of laser-material's absorption and emission spectra, and laser-diode's emission spectra. The tabulated data contains physical properties of laser, optical, and nonlinear materials, including crystalline, thermal, and mechanical properties. A menu-driven interface allows the execution from a personal directory where the user can store files containing input parameters for a specific model or the results of model's calculations.

Cross, P. L.

Ramifications of X-Site Ion Modification in a Zero-Dimensional Piezoelectric Tetrahalozincate

Using mixtures of A, B, or X site ions in piezoelectric hybrid organic inorganic materials has been shown to be an effective strategy to improve piezoelectric properties. Here, we investigated the effect of increasing Br content within histammonium tetrachlorozincate [HistNH3Zn(Cl x Br 1–x )4] by varying the relative amounts of Cl and Br from x = 0% to 100% on nonlinear optical and piezoelectric properties. We found that the crystal structures were unchanged with Br percentages up to 100%, but the melting point of the materials changed substantially with increasing Br content. On the other hand, the nonlinear optical properties were only moderately affected with increasing Br content. The piezoelectric response of each material was measured and compared with DFT calculated values, both of which agreed that the overall the materials had relatively similar d 33 coefficients. The x = 75% Br compound had the largest magnitude d 33 value at maximum strain at both 29 °C (−97.56 pm/V) and 40 °C (−92.00 pm/V). The observed negative piezoelectric response is a rare trait that was ascribed to the large number of intermolecular interactions between lattice elements, as described by others.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

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

Spontaneously formed phonon frequency combs in van der Waals solid CrGeTe 3 and CrSiTe 3

Optical phonon engineering through nonlinear effects has been utilized in ultrafast control of material properties. However, nonlinear optical phonons typically exhibit rapid decay due to strong mode-mode couplings, limiting their effectiveness in temperature or frequency sensitive applications. Here we report the observation of long-lived nonlinear optical phonons through the spontaneous formation of phonon frequency combs in the van der Waals material CrXTe 3 (X=Ge, Si) using high-resolution Raman scattering. Unlike conventional optical phonons, the highest A g mode in CrGeTe 3 splits into equidistant, sharp peaks forming a frequency comb that persists for hundreds of oscillations and survives up to 200K. These modes correspond to localized oscillations of Ge 2 Te 6 clusters, isolated from Cr hexagons, behaving as independent quantum oscillators. Introducing a cubic nonlinear term to the harmonic oscillator model, we simulate the phonon time evolution and successfully replicate the observed comb structure. Similar frequency comb behavior is observed in CrSiTe 3 , demonstrating the generalizability of this phenomenon. Our findings demonstrate that Raman scattering effectively probes high-frequency nonlinear phonon modes, offering insight into the generation of long-lived, tunable phonon frequency combs with potential applications in ultrafast material control and phonon-based technologies.

36 MATERIALS SCIENCE

Fabrication and Atomic Force Microscopy Characterization of Molecular Composites of Fullerenes in Aerogel Matrix for Optical Limiting

An optical limiter is a device which exhibits a decrease in the transmittance in a material with an increase in intensity of light. Sol-gel techniques offer many advantages in the fabrication of materials. These materials possess many desirable properties for nonlinear optical (NLO) device applications which include transparency, high thermal and chemical stabilities, very low refractive index and dielectric constants. C60 shows a higher excited state absorption cross section than the ground state absorption cross section over the complete visible spectrum, and the spectrum of the excited state absorption of C60 has the same general shape as the ground state absorption. This fact suggests that fullerenes are ideal optical limiting materials. Aerogels are fabricated by sol-gel processing. One of the key issues is the dispersion of fullerenes into small and uniform pores of silica aerogel host matrices. The aerogel network was characterized by Raman spectroscopy. Atomic force microscopy is a technique with many advantages to characterize the aerogel materials. The morphology of the cleaved surface for a C60/aerogel sample shows that there are long paralleled shaped stripes with 20-30 nm in width and about 500 nm in length on the cleaved surface. The cleaved surface also was etched by 5% HF solution for one minutes, and it became smoother after HF etching. The main feature in on the surface is the spherical particles with the size of few nanometers, and no aggregated fullerenes appear. The fullerenes are well dispersed in the aerogel matrices.

Lu, W. J .