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Results for “NONLINEAR OPTICS”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Bent HgI 2 Molecules in the Melt and Sulfide Glasses: Implications for Nonlinear Optics

Nonlinear optical (NLO) crystals are widely used in advanced photonic technologies for second harmonic and difference frequency generation (SHG and DFG, respectively), producing coherent light at frequencies where existing lasers are unavailable. Isotropic glasses do not exhibit SHG or DFG, except temporarily induced anisotropy under external stimuli. Nevertheless, recent reports on glasses with chiral structural motifs show promising permanent NLO properties. We introduce an alternative solution: hybrid molecular/network glasses with noncentrosymmetric HgI 2 monomers. Mercury (II) iodide consists of linear HgI 2 triatomic molecules in the vapor phase and in the yellow orthorhombic polymorph stable above 400 K. At lower temperatures, the tetragonal red form is composed of corner-sharing HgI 4/2 tetrahedra forming a layered extended framework. There is a gap in the molecular evolution; direct structural measurements of the liquid HgI 2 phase are missing. Using high-energy X-ray scattering, pulsed neutron diffraction, and Raman spectroscopy supported by structural and vibrational modeling, we show that the mercury(II) iodide melt and HgI 2 -containing sulfide glasses are built up by bent HgI 2 monomers (the bond angle <I-Hg-I = 156 ± 2° in the melt). Here, the noncentrosymmetric entities imply intrinsic optical nonlinearity of the second order, confirmed by a strong SHG response.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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 OSTI2017

A unified materials approach to mitigating optical nonlinearities in optical fiber. III. Canonical examples and materials road map

Abstract This paper, Part III in the Trilogy (Ballato, Cavillon, Dragic, 2018; Dragic, Cavillon, Ballato, et al ., 2018a,b), provides a road map for the development of simple core/clad optical fibers whose enhanced performance—in particular, marked reductions in optical nonlinearities—is achieved materially and not through the more conventional present routes of geometrically complex fiber design. More specifically, the material properties that give rise to Brillouin, Raman and Rayleigh scattering, transverse mode instabilities ( TMI ), and n 2 ‐mediated nonlinear effects are compiled and results on a wide range of optical fibers are discussed with a focus on trends in performance with glass composition. Furthermore, optical power scaling estimations as well as binary and ternary property diagrams associated with Rayleigh scattering, the Brillouin gain coefficient ( BGC ) and the thermo‐optic coefficient (d n /d T ) are developed and employed to graphically represent general trends with composition along with compositional targets for a single intrinsically low nonlinearity, silica‐based optical fiber that can achieve the power scaling goals of future high energy fiber laser applications. A foundational finding of this work is that the high‐silica content optical fibers fabricated using conventional chemical vapor deposition methods will not suffice to meet the power scaling demands of future high‐power and high‐energy fiber lasers.

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↗
DOE OSTI2015

Z-scan: A simple technique for determination of third-order optical nonlinearity

Z-scan is a simple experimental technique to measure intensity dependent nonlinear susceptibilities of third-order nonlinear optical materials. This technique is used to measure the sign and magnitude of both real and imaginary part of the third order nonlinear susceptibility (χ{sup (3)}) of nonlinear optical materials. In this paper, we investigate third-order nonlinear optical properties of Ag-polymer composite film by using single beam z-scan technique with Q-switched, frequency doubled Nd: YAG laser (λ=532 nm) at 5 ns pulse. The values of nonlinear absorption coefficient (β), nonlinear refractive index (n{sub 2}) and third-order nonlinear optical susceptibility (χ{sup (3)}) of permethylazine were found to be 9.64 × 10{sup −7} cm/W, 8.55 × 10{sup −12} cm{sup 2}/W and 5.48 × 10{sup −10} esu, respectively.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Effect of alpha and Gaussian refractive index profiles on the design of highly nonlinear optical fibre for efficient nonlinear optical signal processing

We propose an index profiled, highly nonlinear ultra-flattened dispersion fibre (HN-UFF) with appreciable values of fibre parameters such as dispersion, dispersion slope, effective area, nonlinearity, bending loss and splice loss. The designed fibre has normal zero flattened dispersion over S, C, L, U bands and extends up to 1.9857 μm. The maximum dispersion variation observed for this fibre is as low as 1.61 ps km{sup −1} nm{sup −1} over the 500-nm optical fibre transmission spectrum. This fibre also has two zero dispersion wavelengths at 1.487 and 1.9857 μm and the respective dispersion slopes are 0.02476 and 0.0068 ps nm{sup −2} km{sup −1}. The fibre has a very low ITU-T cutoff wavelength of 1.2613 μm and a virtuous nonlinear coefficient of 9.43 W{sup −1} km{sup −1}. The wide spectrum of zero flattened dispersion and a good nonlinear coefficient make the designed fibre very promising for different nonlinear optical signal processing applications. (fibre optics)

42 ENGINEERING↗
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↗
DOE OSTI2016

Possibilities of joint application of adaptive optics technique and nonlinear optical phase conjugation to compensate for turbulent distortions

The efficiency of integrating the nonlinear optical technique based on forming a reverse wavefront and the conventional adaptive optics into a unified complex (for example, for adaptive focusing of quasi-cw laser radiation) is demonstrated. Nonlinear optical phase conjugation may provide more exact information about the phase fluctuations in the corrected wavefront in comparison with the adaptive optics methods. At the same time, the conventional methods of adaptive optics provide an efficient control of a laser beam projected onto a target for a rather long time. (adaptive optics)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Optical nonlinearities of colloidal InP@ZnS core-shell quantum dots probed by Z-scan and two-photon excited emission

Spectrally resolved nonlinear optical properties of colloidal InP@ZnS core-shell quantum dots of various sizes were investigated with the Z-scan technique and two-photon fluorescence excitation method using a femtosecond laser system tunable in the range from 750 nm to 1600 nm. In principle, both techniques should provide comparable results and can be interchangeably used for determination of the nonlinear optical absorption parameters, finding maximal values of the cross sections and optimizing them. We have observed slight differences between the two-photon absorption cross sections measured by the two techniques and attributed them to the presence of non-radiative paths of absorption or relaxation. The most significant value of two-photon absorption cross section σ{sub 2} for 4.3 nm size InP@ZnS quantum dot was equal to 2200 GM, while the two-photon excitation action cross section σ{sub 2}Φ was found to be 682 GM at 880 nm. The properties of these cadmium-free colloidal quantum dots can be potentially useful for nonlinear bioimaging.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Sub-wavelength modulation of χ (2) optical nonlinearity in organic thin films

Modulating the second-order nonlinear optical susceptibility (χ (2) ) of materials at the nanoscale represents an ongoing technological challenge for a variety of integrated frequency conversion and nonlinear nanophotonic applications. Here we exploit the large hyperpolarizability of intermolecular charge transfer states, naturally aligned at an organic semiconductor donor–acceptor (DA) interface, as a means to control the magnitude and sign of χ (2) at the nanoscale. Focusing initially on a single pentacene-C 60 DA interface, we confirm that the charge transfer transition is strongly aligned orthogonal to the heterojunction and find that it is responsible for a large interfacial nonlinearity probed via second harmonic generation that is sufficient to achieve d 33 > 10pm V –1 , when incorporated in a non-centrosymmetric DA multilayer stack. Lastly, using grating-shadowed oblique-angle deposition to laterally structure the DA interface distribution in such multilayers subsequently enables the demonstration of a χ (2) grating with 280 nm periodicity, which is the shortest reported to date.

36 MATERIALS SCIENCE↗
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 OSTI2017

Nonlinear optical higher-order effects in an optical lattice clock

The development of optical frequency standards with a relative uncertainty of reproducing the time and frequency units at a level as low as 10{sup −17}–10{sup −18} calls for an unprecedented accuracy in estimating the role of higher orders of optical nonlinearity, caused by the influence of the optical lattice on the frequency shift of the ‘clock transition’. This paper presents a systematic calculation of the contributions of multipole nonlinear anharmonic effects to the error of clocks based on optical lattices for alkaline-earth-like Sr, Yb, and Hg atoms. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Enhanced optical nonlinearities in the near-infrared using III-nitride heterostructures coupled to metamaterials

We use planar metamaterial resonators to enhance, by more than two orders of magnitude, the optical second harmonic generation, in the near infrared, obtained from intersubband transitions in III-Nitride heterostructures. The improvement arises from two factors: employing an asymmetric double quantum well design and aligning the resonators’ cross-polarized resonances with the intersubband transition energies. The resulting nonlinear metamaterial operates at wavelengths where single photon detection is available, and represents a new class of sources for quantum photonics related phenomena.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Optical nonlinearities of excitons in monolayer MoS 2

We calculate linear and nonlinear optical susceptibilities arising from the excitonic states of monolayer MoS 2 for in-plane light polarizations, using second-quantized bound and unbound exciton operators. Optical selection rules are critical for obtaining the susceptibilities. We derive the valley-chirality rule for the second-order harmonic generation in monolayer MoS 2 and find that the third-order harmonic process is efficient only for linearly polarized input light while the third-order two-photon process (optical Kerr effect) is efficient for circularly polarized light using a higher order exciton state. The absence of linear absorption due to the band gap and the unusually strong two-photon third-order nonlinearity make the monolayer MoS 2 excitonic structure a promising resource for coherent nonlinear photonics.

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↗
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 OSTI2018

Resonance-enhanced optical nonlinearity in the Weyl semimetal TaAs

The second-order conductivity of a material, σ (2) , relating current to the square of electric field, is nonzero only when inversion symmetry is broken, unlike the conventional linear conductivity. Second-order nonlinear optical responses are thus powerful tools in basic research as probes of symmetry breaking; they are also central to optical technology as the basis for generating photocurrents and frequency doubling. The recent surge of interest in Weyl semimetals with acentric crystal structures has led to the discovery of a host of σ (2) -related phenomena in this class of materials, such as polarization-selective conversion of light to dc current (photogalvanic effects) and the observation of giant second-harmonic generation (SHG) efficiency in TaAs at photon energy 1.5 eV. Here, we present measurements of the SHG spectrum of TaAs, revealing that the response at 1.5 eV corresponds to the high-energy tail of a resonance at 0.7 eV, at which point the second harmonic conductivity is approximately 200 times larger than seen in the standard candle nonlinear crystal, GaAs. This remarkably large SHG response provokes the question of ultimate limits on σ (2) , which we address by a new theorem relating frequency-integrated nonlinear response functions to the third cumulant (or "skewness") of the polarization distribution function in the ground state.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Nonlinear optical control of chiral charge pumping in a topological Weyl semimetal

Solids with topologically robust electronic states exhibit unusual electronic and optical properties that do not exist in other materials. A particularly interesting example is chiral charge pumping, the so-called chiral anomaly, in recently discovered topological Weyl semimetals, where simultaneous application of parallel DC electric and magnetic fields creates an imbalance in the number of carriers of opposite topological charge (chirality). Here, using time-resolved terahertz measurements on the Weyl semimetal TaAs in a magnetic field, we optically interrogate the chiral anomaly by dynamically pumping the chiral charges and monitoring their subsequent relaxation of the nonequilibrium state. Theory based on Boltzmann transport shows that the observed effects originate from an optical nonlinearity in the chiral charge pumping process. Our measurements reveal that the nonequilibrium chiral excitation relaxation time is much greater than 1 ns. The observation of terahertz-controlled chiral carriers with long coherence times and topological protection suggests the application of Weyl semimetals for quantum optoelectronic technology.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗