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At least 19 records

All sources NASA NTRS DOE OSTI

DOE OSTI2023

Enhancement of second-order optical nonlinearities and nanoscale periodic domain patterning in ferroelectric boron-substituted aluminum nitride thin films

The discovery and development of CMOS-compatible, nonlinear optical materials is essential to produce integrated photonic devices with advanced functionalities. AlN is a strong candidate for on-chip device demonstration due to its intrinsic second-order optical nonlinearities, large bandgap, and well-established fabrication techniques. However, AlN is not easily phase matched for the largest coefficient d 33 ; the coefficients that could potentially be dispersion phase-matched, d 31 and d 15 , have weak nonlinearities. This work investigates ferroelectric Al 1-x B x N (x = 0 to 0.11) for viability as a large bandgap nonlinear optical material with unique suitability towards ultraviolet light generation using second harmonic generation. The linear and nonlinear optical properties are characterized accounting for material anisotropy. With increasing B concentration, a large enhancement from near negligible values to d 31 = 0.9 ± 0.1 pm/V and d 15 = 1.2 ± 0.1 pm/V is observed. This compares favorably to other large bandgap materials like β-Ba(BO 2 ) 2 , where the largest nonlinear coefficient is d 22 ~ 2.3 pm/V at 800 nm. This is accompanied by a change in the bandgap from 6.1 eV to 5.8 eV as B substitution goes from 0 to 11%. A periodically poled, quasi-phase-matched ferroelectric domain pattern with 400 nm domain size and a wall roughness of <16 nm is demonstrated.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Giant optical nonlinearity of Fermi polarons in atomically thin semiconductors

In this study, realizing strong nonlinear optical responses is a long-standing goal of both fundamental and technological importance. Recently, substantial efforts have been focused on exploring excitons in solids to achieve nonlinearities even down to few-photon levels. However, a crucial tradeoff arises as strong light–matter interactions require large oscillator strength and short radiative lifetime of excitons, which limits their nonlinearity. Here we experimentally demonstrate strong nonlinear optical responses with large oscillator strength by exploiting the coupling between excitons and carriers in an atomically thin semiconductor. By controlling the electric field and electrostatic doping of trilayer WSe 2 , we observe the hybridization between intralayer and interlayer excitons and the formation of Fermi polarons. Substantial optical nonlinearity is observed under continuous-wave and pulsed laser excitation, where the Fermi polaron resonance blueshifts by as much as ~10 meV. Intriguingly, we observe a remarkable asymmetry in the optical nonlinearity between electron and hole doping, which is tunable by the applied electric field. We attribute these features to the optically induced valley polarization due to the interactions between excitons and free charges. Our results establish atomically thin heterostructures as a highly versatile platform for engineering nonlinear optical response with applications to classical and quantum optoelectronics.

2d materials↗

NASA NTRS1993

Films Containing Optically Nonlinear Diacetylene Monomer

Solid films exhibiting nonlinear optical properties prepared as mixtures of poly(methyl methacrylate) with various amounts of diacetylene monomer called "compound 1" in article, "Synthesizing Diacetylenes With Nonlinear Optical Properties" (MFS-26186). Useful as phase-conjugate mirrors in laser-beam communications and as optical switches in optical computers. This particular diacetylene monomer exhibits strong third-order nonlinear optical properties, both in pure form and in solution.

Paley, Mark S.↗

DOE OSTI2026

Polarization Control via Artificial Optical Nonlinearity in Dielectric Metasurfaces

Nonlinear optical phenomena are generally governed by geometry in matter systems, as they depend on the spatial arrangement of atoms within materials or molecules. Metasurfaces, through precisely designed geometries on a subwavelength scale, allow the optical response of a material to be tailored far beyond its natural properties. Therefore, metasurfaces are highly appealing for enabling the engineering of nonlinear optical interactions. Current studies of nonlinear metasurfaces predominantly focus on the phase control of the generated light. Nonetheless, investigating the tensorial nature of the nonlinearity of metasurfaces and its effect on the polarization of the generated light is critical to fully unlocking a range of applications, such as nonlinear vector beam generation and nonlinear polarization imaging. Here, we study the artificial optical nonlinearity of a dielectric metasurface originating from its meta-atom symmetry and describe the third-order nonlinear behavior by considering the polarization degree of freedom. We establish an effective nonlinear medium model that serves as a design toolbox for developing amorphous silicon-based geometric metasurfaces with customizable features for third-harmonic generation. We further extract quantitative values of the artificial nonlinear susceptibility tensor elements related to the investigated nonlinear process and geometry. The implemented functional devices demonstrate the versatility of dielectric metasurfaces in shaping the emitted light in terms of amplitude, phase, and polarization for the precise engineering of advanced nonlinear architectures targeting applications in nonlinear imaging and complex light generation.

Diffraction↗

NASA NTRS1993

Optimization of microscopic and macroscopic second order optical nonlinearities

Nonlinear optical materials (NLO) can be used to extend the useful frequency range of lasers. Frequency generation is important for laser-based remote sensing and optical data storage. Another NLO effect, the electro-optic effect, can be used to modulate the amplitude, phase, or polarization state of an optical beam. Applications of this effect in telecommunications and in integrated optics include the impression of information on an optical carrier signal or routing of optical signals between fiber optic channels. In order to utilize these effects most effectively, it is necessary to synthesize materials which respond to applied fields very efficiently. In this talk, it will be shown how the development of a fundamental understanding of the science of nonlinear optics can lead to a rational approach to organic molecules and materials with optimized properties. In some cases, figures of merit for newly developed materials are more than an order of magnitude higher than those of currently employed materials. Some of these materials are being examined for phased-array radar and other electro-optic switching applications.

Marder, Seth R.↗

NASA NTRS1994

Photodeposition of Thin Polydiacetylene Films from Solution that Exhibit Large Third-Order Optical Nonlinearities

One promising class of organic compounds for applications in the field of nonlinear optics (NLO) are polydiacetylenes, which are of interest because they are highly conjugated polymers capable of exhibiting very large optical nonlinearities with fast response times. During the course of crystal growth studies in anticipation of a space experiment, we discovered a novel, simple method for the formation of polydiacetylene thin films by photodeposition from monomer solutions onto quartz or glass substrates. Characterization of these PDAMNA films is not trivial; they are not soluble in common organic solvents, which makes the standard solution-based methods of polymer analysis useless.

Paley, M. S.↗

DOE OSTI2023

Plasmon-enhanced optical nonlinearity in graphene nanomeshes

Using the density-matrix formalism, here we show that graphene nanomeshes (GNMs)—graphene sheets patterned with antidots—have large plasmon-enhanced nonlinear optical response. GNMs can be designed to behave as quasi-one-dimensional plasmonic crystals in which plasmons with large propagation lengths are efficiently excited. The associated third-order Kerr and third-harmonic-generation susceptibility can be as high as 10 –7 and 10 –9 m 2 V –2 , respectively, over the mid-to-near-infrared frequency range. Furthermore, carrier-density tuning in GNMs can flip the propagation direction of plasmonic waves and enables bidirectional switching of optical signals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Supramolecular Metal Halide Complexes for High-Temperature Nonlinear Optical Switches

Nonlinear optical (NLO) switching materials, which exhibit reversible intensity modulation in response to thermal stimuli, have found extensive applications across diverse fields, including sensing, photoelectronics, and photonic applications. While significant progress has been made in solid-state NLO switching materials, these materials typically showcase their highest NLO performance near room temperature. However, this performance drastically deteriorates upon heating, primarily due to the phase transition undergone by the materials from non-centrosymmetric to centrosymmetric phase. Here, we introduce a new class of NLO switching materials, solid-state supramolecular compounds 18-Crown-6 ether@Cu 2 Cl 4 ·4H 2 O (1·4H 2 O), exhibiting reversible and stable NLO switching when subjected to near-infrared (NIR) photoexcitation and/or thermal stimuli. The reversible crystal structure in response to external stimuli is attributed to the presence of a weakly coordinated bridging water molecule, facilitated by hydrogen bonding/chelation interactions between the metal halide and crown-ether supramolecules. We observed an exceptionally high second-harmonic generation (SHG) signal under continuous photoexcitation, even at temperatures exceeding 110°C. In addition, the bridging water molecules within the complex can be released and recaptured in a fully reversible manner, all without requiring excessive energy input. This feature allows for precise control of SHG signal activation and deactivation through structural transformations, resulting in a high-contrast off/on ratio, reaching values in the million-fold range.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2007

Nonlinear Optics and Applications

Nonlinear optics is the result of laser beam interaction with materials and started with the advent of lasers in the early 1960s. The field is growing daily and plays a major role in emerging photonic technology. Nonlinear optics play a major role in many of the optical applications such as optical signal processing, optical computers, ultrafast switches, ultra-short pulsed lasers, sensors, laser amplifiers, and many others. This special review volume on Nonlinear Optics and Applications is intended for those who want to be aware of the most recent technology. This book presents a survey of the recent advances of nonlinear optical applications. Emphasis will be on novel devices and materials, switching technology, optical computing, and important experimental results. Recent developments in topics which are of historical interest to researchers, and in the same time of potential use in the fields of all-optical communication and computing technologies, are also included. Additionally, a few new related topics which might provoke discussion are presented. The book includes chapters on nonlinear optics and applications; the nonlinear Schrodinger and associated equations that model spatio-temporal propagation; the supercontinuum light source; wideband ultrashort pulse fiber laser sources; lattice fabrication as well as their linear and nonlinear light guiding properties; the second-order EO effect (Pockels), the third-order (Kerr) and thermo-optical effects in optical waveguides and their applications in optical communication; and, the effect of magnetic field and its role in nonlinear optics, among other chapters.

Abdeldayem, Hossin A.↗

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)↗

NASA NTRS2002

Enhancement of Optical Nonlinearities Via Whispering Gallery Mode Splitting

An iterative method is applied to the analysis of N coupled ring-resonators, and the results are compared with multilayered spheres. Splitting of the whispering gallery modes into N higher-Q modes occurs when the round-trip phase shifts in each ring (or layer) are equal, in agreement with results for planar resonators. This mode-splitting is, therefore, a universal phenomenon for resonant structures, and can lead to reduced thresholds for nonlinear optical effects.

Chang, Hongrok↗

NASA NTRS2002

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.↗

DOE OSTI2022

Ultra-low-power second-order nonlinear optics on a chip

Second-order nonlinear optical processes convert light from one wavelength to another and generate quantum entanglement. Creating chip-scale devices to efficiently control these interactions greatly increases the reach of photonics. Existing silicon-based photonic circuits utilize the third-order optical nonlinearity, but an analogous integrated platform for second-order nonlinear optics remains an outstanding challenge. Here we demonstrate efficient frequency doubling and parametric oscillation with a threshold of tens of micro-watts in an integrated thin-film lithium niobate photonic circuit. We achieve degenerate and non-degenerate operation of the parametric oscillator at room temperature and tune its emission over one terahertz by varying the pump frequency by hundreds of megahertz. Finally, we observe cascaded second-order processes that result in parametric oscillation. These resonant second-order nonlinear circuits will form a crucial part of the emerging nonlinear and quantum photonics platforms.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS2005

Nonlinear optical whispering gallery mode resonators

Whispering gallery mode (WGM) optical resonators comprising nonlinear optical materials, where the nonlinear optical material of a WGM resonator includes a plurality of sectors within the optical resonator and nonlinear coefficients of two adjacent sectors are oppositely poled.

Ilchenko, Vladimir↗

DOE OSTI2025

Nonlinear optics in 2D materials: From classical to quantum

Nonlinear optics has long been a cornerstone of modern photonics, enabling a wide array of technologies, from frequency conversion to the generation of ultrafast light pulses. Recent breakthroughs in two-dimensional (2D) materials have opened a frontier in this field, offering new opportunities for both classical and quantum nonlinear optics. These atomically thin materials exhibit strong light–matter interactions and large nonlinear responses, thanks to their tunable lattice symmetries, strong resonance effects, and highly engineerable band structures. In this paper, we explore the potential that 2D materials bring to nonlinear optics, covering topics from classical nonlinear optics to nonlinearities at the few-photon level. We delve into how these materials enable possibilities, such as symmetry control, phase matching, and integration into photonic circuits. The fusion of 2D materials with nonlinear optics provides insights into the fundamental behaviors of elementary excitations—such as electrons, excitons, and photons—in low-dimensional systems and has the potential to transform the landscape of next-generation photonic and quantum technologies.

2D materials↗

DOE OSTI2025

Femtojoule optical nonlinearity for deep learning with incoherent illumination

Optical neural networks (ONNs) are a promising computational alternative for deep learning due to their inherent massive parallelism for linear operations. However, the development of energy-efficient and highly parallel optical nonlinearities, a critical component in ONNs, remains an outstanding challenge. Here, we introduce a nonlinear optical microdevice array (NOMA) compatible with incoherent illumination by integrating the liquid crystal cell with silicon photodiodes at the single-pixel level. We fabricate NOMA with more than half a million pixels, each functioning as an optical analog of the rectified linear unit at ultralow switching energy down to 100 femtojoules per pixel. With NOMA, we demonstrate an optical multilayer neural network. Our work holds promise for large-scale and low-power deep ONNs, computer vision, and real-time optical image processing.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Linear and Nonlinear Optical Properties of Iridium Nanoparticles Grown via Atomic Layer Deposition

Nonlinear optical phenomena enable novel photonic and optoelectronic applications. Especially, metallic nanoparticles and thin films with nonlinear optical properties offer the potential for micro-optical system integration. For this purpose, new nonlinear materials need to be continuously identified, investigated, and utilized for nonlinear optical applications. While noble-metal nanoparticles, nanostructures, and thin films of silver and gold have been widely studied, iridium (Ir) nanoparticles and ultrathin films have not been investigated for nonlinear optical applications yet. Here, we present a combined theoretical and experimental study on the linear and nonlinear optical properties of iridium nanoparticles deposited via atomic layer deposition (ALD). Linear optical constants, such as the effective refractive index and extinction coefficient, were evaluated at different growth stages of nanoparticle formation. Both linear and nonlinear optical properties of these Ir ALD coatings were calculated theoretically using the Maxwell Garnett theory. The third-order susceptibility of iridium nanoparticle samples was experimentally investigated using the z-scan technique. According to the experiment, for an Ir ALD coating with 45 cycles resulting in iridium nanoparticles, the experimentally determined nonlinear third-order susceptibility is about χ Ir (3) = (2.4 – i2.1) × 10 –17 m 2 /V 2 at the fundamental wavelength of 700 nm. The theory fitted to the experimental results predicts a 5 × 10 6 -fold increase around 230 nm. This strong increase is due to the proximity to the Mie resonance of iridium nanoparticles.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Flat nonlinear optics with intersubband polaritonic metasurfaces

Nonlinear intersubband polaritonic metasurfaces produce some of the strongest second- and third-order nonlinear optical responses reported for condensed matter systems at infrared frequencies. These metasurfaces are fabricated as two-dimensional arrays of nanoresonators from multi-quantum-well semiconductor heterostructures, designed to produce strong nonlinear responses associated with intersubband transitions. By optimally coupling the optical modes of the nanoresonators to vertically polarized intersubband transitions in semiconductor heterostructures, one can boost the nonlinear response associated with intersubband transitions, make intersubband transitions interact with free-space radiation at normal incidence, and hence produce optically thin flat nonlinear optical elements compatible with free-space optical setups. As a result of the strong nonlinear response in these systems, significant nonlinear conversion efficiencies (>0.1 %) can be attained in deeply subwavelength optical films using modest pumping intensities of only 10–100 kW/cm 2 . Subwavelength metasurface thickness relaxes phase-matching constraints limiting the operation of bulk nonlinear crystals. Furthermore, the amplitude and phase of the nonlinear optical response in intersubband polaritonic metasurfaces can be tailored for a specific pump wavelength and a nonlinear process of interest through the co-optimization of quantum engineering of electron states in semiconductor heterostructures and photonic engineering of the metasurface nanoresonators design. Additionally, an applied voltage can dynamically control the amplitude and phase of the nonlinear optical response at a nanoresonator level. Here, we review the current state of the art in this rapidly expanding field, focusing on nonlinear processes supporting second-harmonic generation, saturable absorption, and optical power limiting.

flat optics↗