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At least 145 records · Page 8

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NASA NTRS1996

The Effect of Gravity Axis Orientation on the Growth of Phthalocyanine Thin Films

Experimentally, many of the functions of electrical circuits have been demonstrated using optical circuits and, in theory, all of these functions may be accomplished using optical devices made of nonlinear optical materials. Actual construction of nonlinear optical devices is one of the most active areas in all optical research being done at this time. Physical vapor transport (PVT) is a promising technique for production of thin films of a variety of organic and inorganic materials. Film optical quality, orientation of microcrystals, and thickness depends critically on type of material, pressure of buffer gas and temperature of deposition. An important but understudied influence on film characteristics is the effect of gravity-driven buoyancy. Frazier, Hung, Paley, Penn and Long have recently reported mathematical modelling of the vapor deposition process and tested the predictions of the model on the thickness of films grown by PVT of 6-(2-methyl-4-nitroanilino)-2,4-hexadiyn-l-ol (DAMNA). In an historic experiment, Debe, et. al. offered definitive proof that copper phthalocyanine films grown in a low gravity environment are denser and more ordered than those grown at 1 g. This work seeks to determine the influence on film quality of gravity driven buoyancy in the low pressure PVT film growth of metal-free phthalocyanine.

Pearson, Earl F.↗

DOE OSTI2024

Nanoscale optical nonreciprocity with nonlinear metasurfaces

Optical nonreciprocity is manifested as a difference in the transmission of light for the opposite directions of excitation. Nonreciprocal optics is traditionally realized with relatively bulky components such as optical isolators based on the Faraday rotation, hindering the miniaturization and integration of optical systems. Here we demonstrate free-space nonreciprocal transmission through a metasurface comprised of a two-dimensional array of nanoresonators made of silicon hybridized with vanadium dioxide (VO 2 ). This effect arises from the magneto-electric coupling between Mie modes supported by the resonator. Nonreciprocal response of the nanoresonators occurs without the need for external bias; instead, reciprocity is broken by the incident light triggering the VO 2 phase transition for only one direction of incidence. Nonreciprocal transmission is broadband covering over 100 nm in the telecommunication range in the vicinity of λ = 1.5 µm. Each nanoresonator unit cell occupies only ~0.1 λ 3 in volume, with the metasurface thickness measuring about half-a-micron. Our self-biased nanoresonators exhibit nonreciprocity down to very low levels of intensity on the order of 150 W/cm 2 or a µW per nanoresonator. We estimate picosecond-scale transmission fall times and sub-microsecond scale transmission rise. Our demonstration brings low-power, broadband and bias-free optical nonreciprocity to the nanoscale.

42 ENGINEERING↗

DOE OSTI2024

Demonstration of Non-linear Optical Spectroscopy Enhancement utilizing Entangled Photons

Laser-based nonlinear optical spectroscopy approaches have enabled the direct sensing of important chemistry in nearly every fundamental or applied field of science. Yet in many applications, increased detectivity is needed to unravel fundamental mechanisms. One possibility is the use of quantum entanglement to increase detection cross-sections, but it is unproven that enhancement from quantum light extends to practical intensities for chemical sensing. In this report, we investigated the creation and use of entangled photons in nonlinear optical mixing for second harmonic generation and infrared imaging. We observe that the linear scaling of nonlinear mixing from entangled photon sources extends to the mW laser power regime, and enhances direct infrared imaging on Si-based charge coupled device cameras. These results motivate future experimentation on practical uses of entangled photons for nonlinear optical sensing applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1997

The Optical Properties of Ion Implanted Silica

We will present our investigation on the change in the optical properties of silica, 'suprasil', after keV through MeV implantation of copper, tin, silver and gold and after annealing. Suprasil-1, name brand of silica glass produced by Hereaus Amerisil, which is chemically pure with well known optical properties. Both linear nonlinear optical properties of the implanted silica were investigated before and after thermal annealing. All implants, except for Sn, showed strong optical absorption bands in agreement with Mie's theory. We have also used Z-scan to measure the strength of the third order nonlinear optical properties of the produced thin films, which is composed of the host material and the metallic nanoclusters. For implants with a measurable optical absorption band we used Doyle's theory and the full width half maximum of the absorption band to calculate the predicted size of the formed nanoclusters at various heat treatment temperatures. These results are compared with those obtained from direct observation using transmission electron microscopic techniques.

Smith, Cydale C.↗

NASA NTRS1999

Photonic Switching Devices Using Light Bullets

A unique ultra-fast, all-optical switching device or switch is made with readily available, relatively inexpensive, highly nonlinear optical materials. which includes highly nonlinear optical glasses, semiconductor crystals and/or multiple quantum well semiconductor materials. At the specified wavelengths. these optical materials have a sufficiently negative group velocity dispersion and high nonlinear index of refraction to support stable light bullets. The light bullets counter-propagate through, and interact within the waveguide to selectively change each others' directions of propagation into predetermined channels. In one embodiment, the switch utilizes a rectangularly planar slab waveguide. and further includes two central channels and a plurality of lateral channels for guiding the light bullets into and out of the waveguide. An advantage of the present all-optical switching device lies in its practical use of light bullets, thus preventing the degeneration of the pulses due to dispersion and diffraction at the front and back of the pulses. Another advantage of the switching device is the relative insensitivity of the collision process to the time difference in which the counter-propagating pulses enter the waveguide. since. contrary to conventional co-propagating spatial solitons, the relative phase of the colliding pulses does not affect the interaction of these pulses. Yet another feature of the present all-optical switching device is the selection of the light pulse parameters which enables the generation of light bullets in nonlinear optical materials. including highly nonlinear optical glasses and semiconductor materials such as semiconductor crystals and/or multiple quantum well semiconductor materials.

Goorjian, Peter M.↗

NASA NTRS2004

Solar Pumped High Power Solid State Laser for Space Applications

Highly coherent laser light provides a nearly optimal means of transmitting power in space. The simplest most direct means of converting sunlight to coherent laser light is a solar pumped laser oscillator. A key need for broadly useful space solar power is a robust solid state laser oscillator capable of operating efficiently in near Earth space at output powers in the multi hundred kilowatt range. The principal challenges in realizing such solar pumped laser oscillators are: (1) the need to remove heat from the solid state laser material without introducing unacceptable thermal shock, thermal lensing, or thermal stress induced birefringence to a degree that improves on current removal rates by several orders of magnitude and (2) to introduce sunlight at an effective concentration (kW/sq cm of laser cross sectional area) that is several orders of magnitude higher than currently available while tolerating a pointing error of the spacecraft of several degrees. We discuss strategies for addressing these challenges. The need to remove the high densities of heat, e.g., 30 kW/cu cm, while keeping the thermal shock, thermal lensing and thermal stress induced birefringence loss sufficiently low is addressed in terms of a novel use of diamond integrated with the laser material, such as Ti:sapphire in a manner such that the waste heat is removed from the laser medium in an axial direction and in the diamond in a radial direction. We discuss means for concentrating sunlight to an effective areal density of the order of 30 kW/sq cm. The method integrates conventional imaging optics, non-imaging optics and nonlinear optics. In effect we use a method that combines some of the methods of optical pumping solid state materials and optical fiber, but also address laser media having areas sufficiently large, e.g., 1 cm diameter to handle the multi-hundred kilowatt level powers needed for space solar power.

Fork, Richard L.↗

DOE OSTI2026

Cs X Si 15 P 21 ( X = Sn or Pb): Polar Noncentrosymmetric Si–P Frameworks Stabilized by Covalent X –P Bonding

Metal silicon phosphides composed of earth-abundant Si and P tend to exhibit semiconducting properties and adopt diverse crystal structures with relatively small additions of structure-directing elements. The potential of silicon phosphide materials in nonlinear optical applications has been hindered by the inability to systematically produce noncentrosymmetric structures with such a flexible framework. Here, in this work, two isostructural compounds with a novel noncentrosymmetric structure were made possible by the inclusion of elements with stereochemically active lone pairs (Sn 2+ and Pb 2+ ). The structures were determined through single-crystal and synchrotron powder X-ray diffraction. Analysis of chemical bonding in real space through the electron localization function revealed stereochemically active Pb 2+ and Sn 2+ species in a trigonal pyramidal coordination with {Pb/Sn}–P bonds. Such covalent bonding between Pb and P is quite uncommon in extended solids and has been reported in a few rare instances. Band structure calculations and linear optical measurements confirm the semiconducting nature of Cs X Si 15 P 21 ( X = Sn or Pb). The synthesis was optimized to yield high-purity polycrystalline samples. The nonlinear optical properties show promising second-harmonic generation (SHG) coefficients from the Kurtz–Perry method. First-principles calculations of the nonlinear optical properties support the experimentally determined SHG values and provide moderate values of birefringence, suggesting Cs X Si 15 P 21 could be phase-matchable and practical nonlinear optical materials in the mid-IR region.

crystal structure↗

NASA NTRS1976

Optical computing with laser light

Linear and nonlinear optical processing techniques (Fourier transformation, convolution and correlation, arithmetic operations - addition and subtraction with gratings, generalized orthogonal transformations; theta modulation, half-tone screen process, optical feedback) for mathematical computations are reviewed. The use of gratings and computer holograms in addition, subtraction, differentiation, and application of generalized transformations is discussed. Use of nonlinear optical elements with or without optical coherent feedback in such nonlinear operations as taking logarithms and thresholding is described. Applications in hybrid systems incorporating digital computer and optical processor with real-time interface devices, or optical threshold and logic devices for parallel processing to apply digital techniques to optical information are considered.

Lee, S. H.↗

NASA NTRS1997

Validity Using Pump-Probe Pulses to Determine the Optical Response of Niobate Crystals

A variety of niobate crystals have found their places in nonlinear optical applications as well as in laser devices. In recent years much attention has been paid to study the ultrafast optical response in a variety of photorefractive crystals such as KTa(1-x)Nb(x)O3 and KNbO3 crystals, glasses, semiconductors and polymers for applications in optical switching, information processing, optical computing, and all-optical device systems. Third-order optical nonlinearity is the most important property for realization of all-optical switching. Therefore experiments have been performed on the third order susceptibility using a variety of techniques such as the third-order harmonic generation, EFISH and degenerate four-wave mixing(DFWM). The latter has been conducted with a variety of pump wavelengths and with nanosecond, picosecond and femtosecond pulses. Niobate crystals, such as potassium niobate KNbO3, potassium tantalate niobate KTN family (KTa(1-x)Nb(x)O3), strontium barium niobate SBN (Sr(x)Ba(1-x)Nb2O6) and potassium-sodium niobate SBN (KNSBN) are attractive due to their photorefractive properties for application in optical storage and processing. The pulsed probe experiments performed on theses materials have suggested two types of time responses. These responses have been associated with an coherent response due to Chi(sup 3), and a long lived component due to excited state population. Recent study of DFWM on KNbO3 and KTN family reveals that the long lived component of those crystals depends on the crystal orientation. A slowly decaying signal is observable when the grating vector K(sub g) is not perpendicular to the C-axis of those photorefractive crystals', otherwise the optical response signal would be only a narrow coherent peak with FWHM equal to the cross-correlation width of the write beam pulses. Based on this understanding, we study the photodynamical process of a variety of niobate crystals using DFWM in a Kg perpindicular to C geometry with a ps-YAG: Nd laser operating at 532nm. However, the discrepancies in numerical estimations of Chi(sup 3) in these materials and other nonlinear optical media have resulted in a number of discussions. In order to better understand the photodynamical process of niobate crystals after an short pulse excitation we analyze the factors governing the coherent signal and present the DFWM spectra of niobate crystals.

Liu, Huimin↗

DOE OSTI2026

Enhanced second-harmonic generation from WS 2 /ReSe 2 heterostructure

Van der Waals stacking presents new opportunities for nonlinear optics with its remarkable tunability and scalability. However, the fundamental role of interlayer interactions in modifying the overall nonlinear optical susceptibilities remains elusive. In this work, we report anisotropic enhancement of second-harmonic generation (SHG) from a WS 2 /ReSe 2 heterobilayer, where the individual composite layers possess distinctive crystal phases. We investigate polarization-resolved response and twist-angle dependence in SHG and reveal that band alignment alone is insufficient to explain the observed anisotropy in the modified SHG response. Spectral shifts in excitonic features highlight band renormalization, supporting the role of hybridization between the two layers. Furthermore, SHG enhancement is highly anisotropic and can even be suppressed in some orientations, suggesting possible intensity-borrowing mechanisms within the heterostructure. Our work demonstrates the ability to tune both the intensity and polarization dependence of nonlinear optical responses with van der Waals stacking of distinctive crystal phases.

2D materials↗

NASA NTRS2011

Ridge Waveguide Structures in Magnesium-Doped Lithium Niobate

This work proposes to establish the feasibility of fabricating isolated ridge waveguides in 5% MgO:LN. Ridge waveguides in MgO:LN will significantly improve power handling and conversion efficiency, increase photonic component integration, and be well suited to spacebased applications. The key innovation in this effort is to combine recently available large, high-photorefractive-damage-threshold, z-cut 5% MgO:LN with novel ridge fabrication techniques to achieve high-optical power, low-cost, high-volume manufacturing of frequency conversion structures. The proposed ridge waveguide structure should maintain the characteristics of the periodically poled bulk substrate, allowing for the efficient frequency conversion typical of waveguides and the high optical damage threshold and long lifetimes typical of the 5% doped bulk substrate. The low cost and large area of 5% MgO:LN wafers, and the improved performance of the proposed ridge waveguide structure, will enhance existing measurement capabilities as well as reduce the resources required to achieve high-performance specifications. The purpose of the ridge waveguides in MgO:LN is to provide platform technology that will improve optical power handling and conversion efficiency compared to existing waveguide technology. The proposed ridge waveguide is produced using standard microfabrication techniques. The approach is enabled by recent advances in inductively coupled plasma etchers and chemical mechanical planarization techniques. In conjunction with wafer bonding, this fabrication methodology can be used to create arbitrarily shaped waveguides allowing complex optical circuits to be engineered in nonlinear optical materials such as magnesium doped lithium niobate. Researchers here have identified NLO (nonlinear optical) ridge waveguide structures as having suitable value to be the leading frequency conversion structures. Its value is based on having the low-cost fabrication necessary to satisfy the challenging pricing requirements as well as achieve the power handling and other specifications in a suitably compact package.

Himmer, Phillip↗

DOE OSTI2023

Nonlinear Loss Engineering in Near‐Zero‐Index Bulk Materials

Transparent conducting oxides (TCOs) show unprecedented optical nonlinearities in the near infrared wavelength range, where the real part of their linear refractive index approaches zero. More specifically, the Kerr nonlinearities of these materials have sparked widespread attention due to their magnitude and speed. However, due to the absorptive nature of these nonlinear processes, it is of fundamental interest to further investigate the imaginary component of the nonlinear index. The present work studies the nonlinear optical absorption properties of aluminium‐doped zinc oxide (AZO) thin films in their near‐zero‐index (NZI) spectral window. It is found that the imaginary part of the refractive index is reduced under optical excitation such that the field penetration depth more than doubles. An optically induced shift of the NZI bandwidth of ≈120 nm for a pump intensity of 1.3 TW cm −2 is also demonstrated. Looking into the optically induced spectral redistribution of the probe signal, local net gain is recorded, which is ascribed to a nonlinear adiabatic energy transfer. The present study adds key information about the fundamental interplay between real and imaginary nonlinear indices in NZI media, while advancing parametric amplification as viable direction for loss compensation.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Full complex amplitude control of second-harmonic generation via electrically tunable intersubband polaritonic metasurfaces

Nonlinear intersubband polaritonic metasurfaces based on coupling of the intersubband nonlinear optical response of quantum-engineered semiconductor heterostructures and electromagnetic modes of nanoresonators provide efficient frequency mixing with moderate pump intensities. The resonant nonlinear optical response, represented as a complex function, can be modulated via Stark tuning of intersubband transition energies under applied voltages. However, achieving full complex amplitude control (both phase and magnitude) remains challenging. In this work, we present and experimentally validate electrically tunable nonlinear intersubband polaritonic metasurfaces that achieve complete complex amplitude control for second-harmonic generation (SHG). Through a design featuring two in-plane flipped meta-atoms per unit cell, we achieve complete electrical control of both the amplitude and phase of the metasurface second-order nonlinear susceptibility, with a tuning range of 0 to 30 nm V −1 for the magnitude and 0-2π for the phase of the nonlinear optical response. Using these properties, we achieve complete on-off SHG modulation and beam diffraction tuning through electrically controlled amplitude and phase gratings.

Science & Technology - Other Topics↗

DOE OSTI2026

Strong-field Driven Sub-cycle Band Structure Modulation and Dephasing Control

In this work, we present measurements of ultrafast electric-field observables in magnesium oxide using a non-resonant nonlinear optical interaction. Using field observables, we show that strong laser fields modulate the band structure on sub-cycle timescales, thereby altering the material’s nonlinear optical response. We perform time-dependent perturbation theory calculations using a field-dependent dispersion relation and semiconductor Bloch equation calculations, both of which agree with experimental observations. Furthermore, we extract pulse decay times from the real-time signal electric field envelope and show sub-cycle control of dephasing times. Our work offers a new perspective on strong-field-driven electron dynamics in solids through electric-field observables. The demonstrated attosecond modulation of the nonlinear response could have important implications for quantum light generation and quantum spectroscopy using nonlinear optical processes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2025

Large Non‐Resonant Infrared Optical Second Harmonic Generation in Bulk Crystals of Van der Waals Semiconductor, SnP 2 Se 6

2D van der Waals (vdW) materials have emerged as a highly promising candidates for nonlinear optical (NLO) applications. This study presents the synthesis, comprehensive linear optical, and optical second harmonic generation (SHG) characterization of a novel 2D vdW semiconductor SnP2Se6 in its bulk single crystal form. It exhibits an indirect bandgap of ≈1.47 eV and an exceptional non-resonant SHG coefficient of d 33 ∼ −222 ± 30 pm V −1 at a fundamental wavelength of 2 µm, which is ≈7 times larger than that of the commercial AgGaSe 2 with a comparable bandgap. Density functional theory (DFT) calculations of the linear and nonlinear optical properties exhibit reasonable agreement with the experimental measurements, revealing the chemical origin of the enhanced properties. Moreover, SnP 2 Se 6 can exhibit both type-I and type-II phase matching over a wide spectral range, fulfilling one of the key criteria for an ideal NLO crystal. These exceptional properties position SnP 2 Se 6 as a highly promising candidate for NLO applications.

36 MATERIALS SCIENCE↗

NASA NTRS1987

Nonlinear intersubband optical absorption in a semiconductor quantum well

The third-order nonlinear intersubband absorption in a semiconductor quantum well is studied theoretically using the density matrix formalism including intrasubband relaxation. It is shown that the peak absorption is reduced by half for an optical intensity 1 MW/sq cm for the well size L = 126.5 A with 3.0 x 10 to the 16th/cu cm electrons.

Ahn, D.↗

NASA NTRS1996

Pulse Shepherding in Nonlinear Fiber Optics

In a wavelength division multiplexed fiber system, where pulses on different wavelength beams may co-propagate in a single mode fiber, the cross-phase-modulation (CPM) effects caused by the nonlinearity of the optical fiber are unavoidable. In other words, pulses on different wavelength beams can interact with and affect each other through the intensity dependence of the refractive index of the fiber. Although CPM will not cause energy to be exchanged among the beams, the pulse shapes and locations on these beams can be altered significantly. This phenomenon makes possible the manipulation and control of pulses co-propagating on different wavelength beams through the introduction of a shepherd pulse at a separate wavelength. How this can be accomplished is demonstrated in this paper.

Yeh, C.↗

NASA NTRS1996

Pulse Shepherding in Nonlinear Fiber Optics

In a wavelength division multiplexed (WDM) fiber system, where pulses on different wavelength beams may co-propagate in a single mode fiber, the cross phase modulation (CPM) effects caused by the nonlinearity of the optical fiber are unavoidable.

intensity↗