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At least 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Robust multiresonant nonlocal metasurfaces by rational design

Abstract Dielectric metasurfaces supporting optical resonances have become a promising platform for quantum and nonlinear optics. However, resonant metasurfaces remain limited in their capacity to independently control the behavior of many distinct resonances despite efforts in computational optimization and inverse design. In this work, we overcome longstanding limitations by introducing a generalized rational design paradigm based on symmetry. Specifically, we use symmetry-broken metasurfaces with periodic “quadromer” lattices comprised of four nanostructures per unit cell to enable extensive control of multiple optical resonances. The rationally designed metasurfaces are readily fabricable, and we experimentally demonstrate metasurfaces that support up to four high Q-factor resonances with deliberately chosen free-space polarizations, spectral separations, and mode profiles. Our design paradigm may unlock new applications for multiresonant metasurfaces in quantum and nonlinear optics, optical sensing, and augmented reality displays.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Second-harmonic generation tensors from high-throughput density-functional perturbation theory

Optical materials play a key role in enabling modern optoelectronic technologies in a wide variety of domains such as the medical or the energy sector. Among them, nonlinear optical crystals are of primary importance to achieve a broader range of electromagnetic waves in the devices. However, numerous and contradicting requirements significantly limit the discovery of new potential candidates, which, in turn, hinders the technological development. In the present work, the static nonlinear susceptibility and dielectric tensor are computed via density-functional perturbation theory for a set of 579 inorganic semiconductors. The computational methodology is discussed and the provided database is described with respect to both its data distribution and its format. Several comparisons with both experimental and ab initio results from literature allow to confirm the reliability of our data. The aim of this work is to provide a relevant dataset to foster the identification of promising nonlinear optical crystals in order to motivate their subsequent experimental investigation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1989

Optical pattern recognition; Proceedings of the Meeting, Los Angeles, CA, Jan. 17, 18, 1989

Papers on optical pattern recognition are presented, covering topics such as the estimation of satellite pose and motion parameters using a neural net tracker, associative memory, optical implmentation of programmable neural networks, optoelectronic neural networks, dynamic autoassociative neural memory, heteroassociative memory, bilinear pattern recognition processors, optical processing of optical correlation plane data, and a synthetic discriminant function-based nonlinear optical correlator. Other topics include an interactive optical-digital image processor, geometric transformations for video compression and human teleoperator display, quasiconformal remapping for compensation of human visual field defects, hybrid vision for automated spacecraft landing, advanced symbolic and inference optical correlation filters, and a rotationally invariant holographic tracking system. Additional topics include the detection of rotational and scale-varying objects with a programmable joint transform correlator, a single spatial light modulator binary nonlinear optical correlator, optical joint transform correlation, linear phase coefficient composite filters, and binary phase-only filters.

Liu, Hua-Kuang↗
NASA NTRS1993

Feasibility study: Monodisperse polymer particles containing laser-excitable dyes

The optical properties associated with small particles, which include aerosols, hydrosols and solid microspheres have an impact on several areas of science and engineering. Since the advent of high-speed computers and lasers, the interaction of light with matter in the form of small particles with a discontinuous optical boundary relative to the surroundings has been much better understood. Various nonlinear optical effects have been observed involving interaction of a laser beam with both solid microspheres and liquid microdroplets. These include observation of second and third harmonic generation, four wave mixing, optical visibility, two photon absorption, observation of stimulated emission and lasing, and Stimulated Raman Scattering. Many of these effects are observed with laser intensities which are orders of magnitude less than that required by threshold condition for interactions in macroscopic bulk medium. The primary reason for this is twofold. The front surface of the microsphere acts as a thick lens to enhance the internal intensity of the input laser radiation, and the spherical shape of the droplet acts as an optical cavity to provide feedback at specific wavelengths corresponding to the whispering gallery modes or the morphology dependent resonances (MDR's). The most interesting and significant recent finding in this field is undoubtedly the existence of resonance peaks in linear and nonlinear optical spectra. Such resonance peaks are only dependent on the particle morphology, which means the size, shape and refractive index of the particle. Because of the simultaneous presence of these resonances, they have been referred to by many names, including structural resonances, whispering modes or whispering gallery modes, creeping waves, circumferential waves, surfaces modes, and virtual modes. All of these names refer to the same phenomena, i.e. morphology dependent resonances (MDR's) which has already been described and predicted precisely by electromagnetic theory and Loentz-Mie theory since 1908. MDR's can become important when the particle size (radius a) approaches and exceeds the wavelength of the electromagnetic wave (lambda) and the refractive index of the particle is greater than that of the surrounding medium. Such resonances are easiest to observe from a single particle with high symmetry, such as a sphere, spheroid, or cylinder. MDR's correspond to solutions of the characteristic equations of the electromagnetic fields in the presence of a sphere.

Venkateswarlu, Putcha↗
DOE OSTI2024

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↗
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↗
DOE OSTI2025

Unconventional nonlinear Hall effects in twisted multilayer 2D materials

We present the first investigation of unusual nonlinear Hall effects in twisted multilayer 2D materials. Contrary to expectations, our study shows that these nonlinear effects are not merely extensions of their monolayer counterparts. Instead, we find that stacking order and pairwise interactions between neighboring layers, mediated by Berry curvatures, play a pivotal role in shaping their collective nonlinear optical response. By combining large-scale Real-Time Time-Dependent Density Functional Theory (RT-TDDFT) simulations with model Hamiltonian analyses, we demonstrate a remarkable second-harmonic transverse response in hexagonal boron nitride four-layers, even in cases where the total Berry curvature cancels out. Furthermore, our symmetry analysis of the layered structures provides a simplified framework for predicting nonlinear responses in multilayer materials in general. Our investigation challenges the prevailing understanding of nonlinear optical responses in layered materials and opens new avenues for the design and development of advanced materials with tailored optical properties.

36 MATERIALS SCIENCE↗
DOE OSTI2024

High‐Order Nonlinear Frequency Conversion in Transparent Conducting Oxide Thin Films

The study of conductive oxides has gained momentum within the photonics community due to their unique linear and nonlinear optical properties. Despite recent experiments reporting on high harmonic generation from thin films, the optical/electronic behavior of these compounds at the nanoscale is still not fully understood due to the lack of a suitable theoretical model. In the present work, aluminum zinc oxide is excited near its epsilon-near-zero crossing point using incident femtosecond pulses having peak power densities in the 1 TW cm −2 range. A relatively efficient frequency up-conversion including even and odd harmonics up to the seventh order is observed. A hydrodynamic-Maxwell theoretical approach is adopted, capable of simultaneously taking into account linear and nonlinear dispersions, nonlocal effects, surface, magnetic, and bulk nonlinearities in a spectral region that spans over two and a half octaves from the UV to the NIR region. The study enables a deeper understanding of the fundamental material parameters regulating optical nonlinearities, providing important insights to engineer this class of materials for applications in sensing, ultra-fast physics, and spectroscopy.

material modeling↗
DOE OSTI2025

Magnon-mediated exciton–exciton interaction in a van der Waals antiferromagnet

Excitons are fundamental excitations that govern the optical properties of semiconductors. Interactions between excitons can lead to various emergent phases of matter and large nonlinear optical responses. In most semiconductors, excitons interact via exchange interactions or phase-space filling. Correlated materials that host excitons coupled to other degrees of freedom could offer pathways for controlling these interactions. Here, in this study, we demonstrate magnon-mediated interactions between excitons in CrSBr, an antiferromagnetic semiconductor. These interactions manifest as the dependence of the exciton energy on the exciton density via a magnonic adjustment of the spin canting angle. Our study demonstrates the emergence of quasiparticle-mediated interactions in correlated quantum materials, leading to large nonlinear optical responses and potential device concepts such as magnon-mediated quantum transducers.

36 MATERIALS SCIENCE↗
NASA NTRS1989

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.↗
NASA NTRS1995

Photodeposition of amorphous polydiacetylene films from monomer solutions onto transparent substrates

Polydiacetylenes are a very promising class of polymers for both photonic and electronic applications because of their highly conjugated structures. For these applications, high-quality thin polydiacetylene films are required. We have discovered a novel technique for obtaining such films of a polydiacetylene derivative of 2-methyl-4-nitroaniline using photodeposition from monomer solutions onto UV transparent substrates. This heretofore unreported process yields amorphous polydiacetylene films with thicknesses on the order of I micron that have optical quality superior to that of films grown by standard crystal growth techniques. Furthermore, these films exhibit good third-order nonlinear optical susceptibilities; degenerate four-wave mixing experiments give x(3) values on the order of 10(exp -8) - 10(exp -7) esu. We have conducted masking experiments which demonstrate that photodeposition occurs only where the substrate is directly irradiated, clearly indicating that the reaction occurs at the surface. Additionally, we have also been able to carry out photodeposition using lasers to form thin polymer circuits. In this work, we discuss the photodeposition of polydiacetylene thin films from solution, perform chemical characterization of these films, investigate the role of the substrate, speculate on the mechanism of the reaction, and make a preliminary determination of the third-order optical nonlinearity of the films. This simple, straightforward technique may ultimately make feasible the production of polydiacetylene thin films for technological applications.

Paley, M. S.↗
DOE OSTI2025

Multistate Geometry of Shift Current and Polarization

The quantum metric and Berry curvature capture essential properties of nontrivial Bloch states and underpin many fascinating phenomena. However, it becomes increasingly evident that a more comprehensive understanding of quantum state geometry is necessary to explain properties involving Bloch states of multiple bands, such as optical transitions. To this end, we employ quantum state projectors to develop an explicitly gauge-invariant formalism and demonstrate its power with applications to nonlinear optics and the theory of electronic polarization. We provide a simple expression for the shift current that resolves its precise relation to the moments of electronic polarization, clarifies the treatment of band degeneracies, and reveals its decomposition into the sum of the skewness of the occupied states and intrinsically multistate geometry. The projector approach is applied to calculate nonlinear optical properties of transition metal dichalcogenides (TMDs) layers, using previously calculated minimal tight-binding models, and demonstrated analytically on a three-band generalization of the Rice-Mele chain to elucidate the different contributions. We close with comments on further applications of the projector operator approach to multistate geometry.

electric polarization↗
DOE OSTI2024

InAs Terahertz Metalens Emitter for Focused Terahertz Beam Generation

Metasurfaces have opened doors to combining multiple photonic functionalities in a single compact device. In particular, the ability to generate short terahertz (THz) pulses with precise wavefront engineering in a single THz metasurface redefined the role metasurfaces can play in THz systems. Here, an InAs metalens emitter which generates and focuses a THz pulse beam is demonstrated using a 130 nm thick InAs metasurface designed as a binary‐phase Fresnel zone plate. The THz beam is focused to a spot of ≈430 μm at 1 THz with a short focal length of 5 mm and large numerical aperture of 0.5. Nanoscale InAs Mie resonators comprising the metasurface enable THz generation with an amplitude as high as 20 times compared to plasmonic THz emitters and several times compared to a 1 mm thick ZnTe crystal. This InAs metasurface emitter provides a new paradigm for designing THz imaging, spectroscopy, and communication systems, where THz beam generation and shaping are performed with a single device without compromising the generation efficiency, while eliminating losses and avoiding limitations of phase matching of conventional nonlinear optics approaches.

47 OTHER INSTRUMENTATION↗
NASA NTRS2004

A Resonator for Low-Threshold Frequency Conversion

A proposed toroidal or disklike dielectric optical resonator (dielectric optical cavity) would be made of an optically nonlinear material and would be optimized for use in parametric frequency conversion by imposition of a spatially periodic permanent electric polarization. The poling (see figure) would suppress dispersions caused by both the material and the geometry of the optical cavity, thereby effecting quasi-matching of the phases of high-resonance-quality (high-Q) whispering-gallery electromagnetic modes. The quasi-phase-matching of the modes would serve to maximize the interactions among them. Such a resonator might be a prototype of a family of compact, efficient nonlinear devices for operation over a broad range of optical wavelengths. A little background information is prerequisite to a meaningful description of this proposal: (1) Described in several prior NASA Tech Briefs articles, the whispering-gallery modes in a component of spheroidal, disklike, or toroidal shape are waveguide modes that propagate circumferentially and are concentrated in a narrow toroidal region centered on the equatorial plane and located near the outermost edge. (2) For the sake of completeness, it must be stated that even though optical resonators of the type considered here are solid dielectric objects and light is confined within them by total internal reflection at dielectric interfaces without need for mirrors, such components are sometimes traditionally called cavities because their effects upon the light propagating within them are similar to those of true cavities bounded by mirrors. (3) For a given set of electromagnetic modes interacting with each other in an optically nonlinear material (e.g., modes associated with the frequencies involved in a frequency-conversion scheme), the threshold power for oscillation depends on the mode volumes and the mode-overlap integral. (4) Whispering-gallery modes are attractive in nonlinear optics because they maximize the effects of nonlinearities by occupying small volumes and affording high Q values

Iltchenko, Vladimir↗
DOE OSTI2026

Experimental Studies of Nonlinear Integrable Optics with Elliptic Potentials

The stable transport of charged particle beams is the core challenge in designing and operating accelerators. The current paradigm for transverse focusing is based on quadrupole and dipole elements, described as a linear integrable Hamiltonian by Courant and Snyder. The operational limits of high intensity accelerators are often determined by collective instabilities within the beam. Nonlinear elements may be added to suppress certain forms of these collective effects, but restrict the range of stable trajectories. These shortcomings motivate extending to a nonlinear integrable system which can offer the benefits of suppressing collective instabilities without limiting the stable trajectories. Danilov and Nagaitsev proposed a novel nonlinear integrable system with elliptical potentials, which could be implemented as magnetic elements in an accelerator. Such a system has been implemented for practical verification in the integrable optics test accelerator (IOTA), a small storage ring constructed for beam dynamics studies. Electron beam studies in IOTA treat the low-emittance beam as a macroparticle for detailed probing of the expected single particle dynamics. This dissertation details new measurements of the nonlinear integrable system relevant for practical implementation. Turn-by-turn measurements of the kicked beam responses are used for phase space reconstruction and analysis of the predicted nonlinear dynamics. The stability and aperture for various nonlinear configurations are measured with beam losses. Amplitude dependent detuning, a core figure of merit for suppressing instabilities, is measured and compared with high fidelity particle tracking simulations. The synchrotron radiation images of circulating beam allow direct measurements of the topology and lifetime in configurations where nonlinear focusing terms dominate.

Wieland, John [Michigan U.] (ORCID:000000028971852↗
NASA NTRS2021

On Parametric Generation of Deep UV Light in Monolithic Cavities With Cubic Nonlinearity

Coherent ultra violet (UV) light has broad applications in optical atomic clocks and quantum computers. Since availability of semiconductor tunable monochromatic lasers is limited at short wavelengths, optical nonlinear processes are frequently used to produce the desirable radiation wavelength. Optical crystals with quadratic nonlinearity are promising for this purpose because of their transparency and high optical damage threshold. In this paper we discuss a possibility of generation of coherent deep UV light utilizing high quality factor (-Q) monolithic optical microcavities made of crystalline optical materials characterized with cubic nonlinearities. We show that the generation is feasible in spite of the relatively small cubic nonlinearities, due to the ultra-broad-band high optical transparency of the crystals and associated high-Q achievable in the cavities created out of the materials. We found that the birefringence as well as the tensor nature of the nonlinear susceptibility of the crystalline optical materials can simplify the phase matching of the nonlinear processes.

Matsko, A.B.↗
NASA NTRS1991

Solid-state lasers for coherent communication and remote sensing

Work in the stabilization of monolithic Nd:YAG lasers and the application of these lasers to nonlinear optical frequency conversion is discussed. The intrinsic stability of semiconductor diode laser pumped solid state lasers has facilitated a number of demonstration in external resonant cavity harmonic generation and stable optical parametric oscillation. Relative laser frequency stabilization of 0.3 Hz was achieved, and absolute stability of a few hundred hertz is anticipated. The challenge is now to reproduce this frequency stability in the output of tunable nonlinear optical devices. Theoretical and experimental work toward this goal are continuing.

Byer, Robert L.↗
DOE OSTI2025

Unraveling the myths and mysteries of photon avalanching nanoparticles

Photon avalanching (PA) nanomaterials exhibit some of the most nonlinear optical phenomena reported for any material, allowing them to push the frontiers of applications ranging from nanoscale imaging and sensing to optical computing. But PA remains shrouded in mystery, with its underlying physics and limitations misunderstood. Photon avalanching is not, in fact, an avalanche of photons, at least not in the same way that snowballs beget more snowballing in an actual avalanche. In this focus article, we dispel these and other common myths surrounding PA in lanthanide-based nanoparticles and unravel the mysteries of this unique nonlinear optical effect. We hope that removing the misconceptions surrounding avalanching nanoparticles will inspire new interest and applications that harness the giant nonlinearity of PA across a broad range of scientific fields.

Skripka, Artiom↗