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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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Methods for microwave characterization of electro-optic crystals for quantum transduction

Microwave-optic quantum transducers are essential devices to develop distributed quantum networks and implement related quantum communication protocols. Three dimensional high-coherence time microwave cavities embedded with electro-optic nonlinear dielectric materials provide promising platforms to boost the efficiency of the microwave-optic frequency conversion. However, so far, the properties for such dielectric crystals operating at milli-Kelvin cryogenic temperatures have not been well understood. Here, we propose a scheme to precisely measure and benchmark the dielectric constant and analyze the dissipation mechanisms of electro-optic materials, such as Lithium Niobate, at the quantum threshold. We will use Fermilab’s three dimensional superconducting cavities with long coherence time. The proposed method of microwave characterization lays the foundations for engineering quantum transduction devices and quantum sensors with high conversion efficiency and fidelity.

Zorzetti, Silvia↗
NASA NTRS1990

Compounds Generate Optical Second Harmonics

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

Marder, Seth R.↗
DOE OSTI2025

Joint Experimental and Computational Characterization of Sum-Frequency Generation between a Continuous Wave Laser and an Ultrafast Frequency Comb Laser for Tunable Laser Development

Ultrafast optical frequency combs allow for both high spectral and temporal resolution in molecular spectroscopy and have become a powerful tool in many areas of chemistry and physics. Ultrafast lasers and frequency combs generated from ultrafast mode-locked lasers often need to be converted to other wavelengths. Commonly used wavelength conversions are optical parametric oscillators, which require an external optical cavity, and supercontinuum generation combined with optical parametric amplifiers. Whether commercial or home-built, these systems are complex and costly. Here, we investigate an alternative, simple, and easy-to-implement approach to tunable frequency comb ultrafast lasers enabled by new continuous-wave laser technology. Sum-frequency generation between an Nd:YAG continuous-wave laser and a Yb:fiber femtosecond frequency comb in a beta-barium borate (BBO) crystal is explored. The resulting sum-frequency beam is a pulsed frequency comb with the same repetition rate as the Yb:fiber source. SNLO simulation software is used to simulate the results and provide benchmarks for designing future systems to achieve wavelength conversion and tunability in otherwise difficult-to-reach spectral regions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Growth of Large‐Sized 2D Ultrathin SnSe Crystals with In‐Plane Ferroelectricity

Abstract Tin (II) selenide (SnSe) is an emerging 2D material with many intriguing properties, such as record‐high thermoelectric figure of merit (ZT), purely in‐plane ferroelectricity, and excellent nonlinear optical properties. To explore these functional properties and related applications, a crucial step is to develop controllable routes to synthesize large‐area, ultrathin, and high‐quality SnSe crystals. Physical vapor deposition (PVD) constitutes a reliable method to synthesize 2D SnSe, however, effects of various growth parameters have not yet been systematically investigated, and current PVD‐synthesized flakes are often thick (>10 nm) with small lateral sizes (<10 µm). In this work, high‐quality 2D SnSe crystals are synthesized via low‐pressure PVD, which display in‐plane ferroelectric domains observed by piezoresponse force microscopy and polarization‐dependent reflection spectroscopy. Detailed studies regarding the roles of various parameters are further carried out, including substrate pre‐annealing, growth duration, temperature, and pressure, which enable to rationally optimize the growth and obtain 2D SnSe crystals with lateral sizes up to ≈23.0 µm and thicknesses down to ≈2.0 nm (3–4 layers). This work paves the way for the controlled growth of large‐area 2D SnSe, facilitating the future exploration of many interesting multiferroic properties and applications with atomic thickness.

2D materials↗
DOE OSTI2020

Nonlinear propagating modes beyond the phonons in fluorite-structured crystals

The vibrational energy of crystals is known to propagate in a fixed number of phonon branches allowed by symmetry. In the realm of nonlinear dynamics, however, additional nonlinear propagating modes are possible. Nonlinear propagating modes have unique properties that are important in many disciplines including optical communications, conducting polymers, biology, magnetism, and nuclear physics. Yet, despite the crucial importance of crystal lattice vibrations in fundamental and applied science, such additional propagating modes have not been observed in ordinary crystals. Here, we show that propagating modes exist beyond the phonons in fluorite-structured thoria, urania, and natural calcium fluoride using neutron scattering and first-principles calculations. These modes are observed at temperatures ranging from 5 K up to 1200 K, extend to frequencies 30–40% higher than the maximum phonon frequency, and travel at velocities comparable to or higher than the fastest phonon. The nonlinear origin of the modes is explained in part via perturbation theory, which approximately accounts for nonlinearity. Given that these modes are still clearly observed at 5 K, they are likely an inherent feature of the quantum ground state. The existence of these waves in three-dimensional crystals may have ramifications for material properties.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Lightwave-electronic harmonic frequency mixing

Electronic frequency mixers are fundamental building blocks of electronic systems. Harmonic frequency mixing in particular enables broadband electromagnetic signal analysis across octaves of spectrum using a single local oscillator. However, conventional harmonic frequency mixers do not operate beyond hundreds of gigahertz to a few terahertz. If extended to the petahertz scale in a compact and scalable form, harmonic mixers would enable field-resolved optical signal analysis spanning octaves of spectra in a monolithic device without the need for frequency conversion using nonlinear crystals. Here, we demonstrate lightwave-electronic harmonic frequency mixing beyond 0.350 PHz using plasmonic nanoantennas. We demonstrate that the mixing process enables complete, field-resolved detection of spectral content far outside that of the local oscillator, greatly extending the range of detectable frequencies compared to conventional heterodyning techniques. Our work has important implications for applications where optical signals of interest exhibit coherent femtosecond-scale dynamics spanning multiple harmonics.

Science & Technology - Other Topics↗
DOE OSTI2020

Disassembling 2D van der Waals crystals into macroscopic monolayers and reassembling into artificial lattices

Two-dimensional materials from layered van der Waals (vdW) crystals hold great promise for electronic, optoelectronic, and quantum devices, but technological implementation will be hampered by the lack of high-throughput techniques for exfoliating single-crystal monolayers with sufficient size and high quality. Here, we report a facile method to disassemble vdW single crystals layer by layer into monolayers with near-unity yield and with dimensions limited only by bulk crystal sizes. The macroscopic monolayers are comparable in quality to microscopic monolayers from conventional Scotch tape exfoliation. The monolayers can be assembled into macroscopic artificial structures, including transition metal dichalcogenide multilayers with broken inversion symmetry and substantially enhanced nonlinear optical response. This approach takes us one step closer to mass production of macroscopic monolayers and bulk-like artificial materials with controllable properties.

Science & Technology - Other Topics↗
NASA NTRS2011

Controlling Second Harmonic Efficiency of Laser Beam Interactions

A method is provided for controlling second harmonic efficiency of laser beam interactions. A laser system generates two laser beams (e.g., a laser beam with two polarizations) for incidence on a nonlinear crystal having a preferred direction of propagation. Prior to incidence on the crystal, the beams are optically processed based on the crystal's beam separation characteristics to thereby control a position in the crystal along the preferred direction of propagation at which the beams interact.

Barnes, Norman P.↗
DOE OSTI2023

Nonlinear Dispersion Relation and Out‐of‐Plane Second Harmonic Generation in MoSSe and WSSe Janus Monolayers

Janus transition metal dichalcogenides are an emerging class of atomically thin materials with engineered broken mirror symmetry that gives rise to long‐lived dipolar excitons, Rashba splitting, and topologically protected solitons. They hold great promise as a versatile nonlinear optical platform due to their broadband harmonic generation tunability, ease of integration on photonic structures, and nonlinearities beyond the basal crystal plane. Here, second and third harmonic generation in MoSSe and WSSe Janus monolayers is studied. Polarization‐resolved spectroscopy is used to map the full second‐order susceptibility tensor of MoSSe, including its out‐of‐plane components. In addition, the effective third‐order susceptibility and the second‐order nonlinear dispersion close to exciton resonances for both MoSSe and WSSe are measured at room and cryogenic temperatures. This work sets a bedrock for understanding the nonlinear optical properties of Janus transition metal dichalcogenides and probing their use in the next‐generation on‐chip multifaceted photonic devices.

36 MATERIALS SCIENCE↗
NASA NTRS1996

Two-Photon Ghost Image and Interference-Diffraction

One of the most surprising consequences of quantum mechanics is entanglement of two or more distance particles. The two-particle entangled state was mathematically formulated by Schrodinger. Based on this unusual quantum behavior, EPR defined their 'physical reality' and then asked the question: 'Can Quantum-Mechanical Description of Physical Reality Be Considered Complete?' One may not appreciate EPR's criterion of physical reality and insist that 'no elementary quantum phenomenon is a phenomenon until it is a recorded phenomenon'. Optical spontaneous parametric down conversion (SPDC) is the most effective mechanism to generate an EPR type entangled two-photon state. In SPDC, an optical beam, called the pump, is incident on a birefringent crystal. The pump is intense enough so that nonlinear effects lead to the conversion of pump photons into pairs of photons, historically called signal and idler. Technically, the SPDC is said to be type-1 or type-2, depending on whether the signal and idler beams have parallel or orthogonal polarization. The SPDC conversion efficiency is typically on the order of 10(exp -9) to 10(exp -11), depending on the SPDC nonlinear material. The signal and idler intensities are extremely low, only single photon detection devices can register them. The quantum entanglement nature of SPDC has been demonstrated in EPR-Bohm experiments and Bell's inequality measurements. The following two experiments were recently performed in our laboratory, which are more closely related to the original 1935 EPR gedankenezperiment. The first experiment is a two-photon optical imaging type experiment, which has been named 'ghost image' by the physics community. The signal and idler beams of SPDC are sent in different directions, so that the detection of the signal and idler photons can be performed by two distant photon counting detectors. An aperture object (mask) is placed in front of the signal photon detector and illuminated by the signal beam through a convex lens. Surprisingly, an image of this aperture is observed in the idler beam, by scanning the idler photon detector in the transverse plane of the idler beam, if we are sure that the idler photon detector 'catches' the 'twin brother' of the signal, which can be easily performed by a coincidence measurement. This effect is even more striking when we found that the object-lens-image relationship satisfies the Gaussian thin lens equation. The second experiment demonstrates two-photon 'ghost' interference-diffraction. The experimental set up is similar to the image experiment, except that rather than a lens and an aperture it is a Young's double-slit (or a single-slit) inserted into the path of the signal beam. We could not find any interference (or diffraction) pattern behind the slit. Surprisingly, an interference (or diffraction) pattern is observed when scanning the detector in the idler beam, if we are sure that the idler photon detector 'catches' the 'twin brother' of the signal.

Shih, Y. H.↗
NASA NTRS1994

Microgravity sciences application visiting scientist program

Contract NAS8-38785, Microgravity Experimental and Theoretical Research, is a project involving a large number of individual research programs related to: determination of the structure of human serum albumin and other biomedically important proteins; analysis of thermodynamic properties of various proteins and models of protein nucleation; development of experimental techniques for the growth of protein crystals in space; study of the physics of electrical double layers in the mechanics of liquid interfaces; computational analysis of vapor crystal growth processes in microgravity; analysis of the influence of magnetic fields in damping residual flows in directional solidification processes; crystal growth and characterization of II-VI semiconductor alloys; and production of thin films for nonlinear optics. It is not intended that the programs will be necessarily limited to this set at any one time. The visiting scientists accomplishing these programs shall serve on-site at MSFC to take advantage of existing laboratory facilities and the daily opportunities for technical communications with various senior scientists.

Source record↗
DOE OSTI2022

Observation of light-driven band structure via multiband high-harmonic spectroscopy

Intense light–matter interactions have revolutionized our ability to probe and manipulate quantum systems at sub-femtosecond timescales, opening routes to the all-optical control of electronic currents in solids at petahertz rates. Such control typically requires electric-field amplitudes in the range of almost volts per angstrom, when the voltage drop across a lattice site becomes comparable to the characteristic bandgap energies. In this regime, intense light–matter interaction induces notable modifications to the electronic and optical properties, dramatically modifying the crystal band structure. Yet, identifying and characterizing such modifications remain an outstanding problem. As the oscillating electric field changes within the driving field’s cycle, does the band structure follow and how can it be defined? Here we address this fundamental question, proposing all-optical spectroscopy to probe the laser-induced closing of the bandgap between adjacent conduction bands. Our work reveals the link between nonlinear light–matter interactions in strongly driven crystals and the sub-cycle modifications in their effective band structure.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Ba 6 (Cu x Z y )Sn 4 S 16 (Z = Mg, Mn, Zn, Cd, In, Bi, Sn): High Chemical Flexibility Resulting in Good Nonlinear-Optical Properties

Seven acentric sulfides Ba 6 (Cu x Z y )Sn 4 S 16 (Z = Mg, Mn, Zn, Cd, In, Bi, Sn) were grown by a high-temperature salt flux method. The crystal structures of the Ba 6 (Cu x Z y )Sn 4 S 16 (Z = Mg, Mn, Zn, Cd, In, Bi, Sn) compounds were determined by single-crystal X-ray diffraction with the aid of solid-state NMR spectroscopy. The Ba 6 (Cu x Z y )Sn 4 S 16 (Z = Mg, Mn, Zn, Cd, In, Bi) compounds are isostructural and crystallize in the Ba 6 Ag 4 Sn 4 S 16 structure type. The Sn-containing compound exhibits high structural similarity to Ba 6 (Cu x Z y )Sn 4 S 16 (Z = Mg, Mn, Zn, Cd, In, Bi) with the presence of an interstitial atomic position partially occupied by Sn atoms. The chemical bonding characteristics of Ba 6 (Cu 2.9 Sn 0.4 )Sn 4 S 16 were understood with electron localization function calculations coupled with crystal orbital Hamilton population calculations. The Ba–S and Cu–S interactions are dominantly ionic, but the Sn–S interactions consist of strong covalent bonding characteristics in Ba 6 (Cu 2.9 Sn 0.4 )Sn 4 S 16 . The monovalent Cu atoms, mixed with certain metals with various oxidation states, significantly shift the optical properties of the Ba 6 (Cu x Z y )Sn 4 S 16 (Z = Mg, Mn, Zn, Cd, In, Bi) compounds. This results in a good balance between the second-harmonic-generation (SHG) response and laser damage threshold (LDT). Ba 6 (Cu 1.9 Zn 1.1 )Sn 4 S 16 possesses a high SHG response and a high LDT of 2.8 × AGS and 3 × AGS, respectively. Here, a density functional theory calculation revealed that CuS 4 and SnS 4 tetrahedra significantly contribute to the SHG response in Ba 6 (Cu 2 Mg)Sn 4 S 16 , which also confirmed that CuS 4 tetrahedra are crucial for the stability and optical properties of the Ba 6 (Cu x Z y )Sn 4 S 16 (Z = Mg, Mn, Zn, Cd, In, Bi, Sn) compounds revealed by electronic structure analysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2008

Phase Matching of Diverse Modes in a WGM Resonator

Phase matching of diverse electromagnetic modes (specifically, coexisting optical and microwave modes) in a whispering-gallery-mode (WGM) resonator has been predicted theoretically and verified experimentally. Such phase matching is necessary for storage of microwave/terahertz and optical electromagnetic energy in the same resonator, as needed for exploitation of nonlinear optical phenomena. WGM resonators are used in research on nonlinear optical phenomena at low optical intensities and as a basis for design and fabrication of novel optical devices. Examples of nonlinear optical phenomena recently demonstrated in WGM resonators include low-threshold Raman lasing, optomechanical oscillations, frequency doubling, and hyperparametric oscillations. The present findings regarding phase matching were made in research on low-threshold, strongly nondegenerate parametric oscillations in lithium niobate WGM resonators. The principle of operation of such an oscillator is rooted in two previously observed phenomena: (1) stimulated Raman scattering by polaritons in lithium niobate and (2) phase matching of nonlinear optical processes via geometrical confinement of light. The oscillator is partly similar to terahertz oscillators based on lithium niobate crystals, the key difference being that a novel geometrical configuration of this oscillator supports oscillation in the regime. The high resonance quality factors (Q values) typical of WGM resonators make it possible to achieve oscillation at a threshold signal level much lower than that in a non-WGM-resonator lithium niobate crystal.

Savchenkov, Anatoliy↗
DOE OSTI2024

Light-induced electronic polarization in antiferromagnetic Cr 2 O 3

In a solid, the electronic subsystem can exhibit incipient order with lower point group symmetry than the crystal lattice. Ultrafast external fields that couple exclusively to electronic order parameters have rarely been investigated, however, despite their potential importance in inducing exotic effects. Here we show that when inversion symmetry is broken by the antiferromagnetic order in Cr 2 O 3 , transmitting a linearly polarized light pulse through the crystal gives rise to an in-plane rotational symmetry-breaking (from C 3 to C 1 ) via optical rectification. Using interferometric time-resolved second harmonic generation, we show that the ultrafast timescale of the symmetry reduction is indicative of a purely electronic response; the underlying spin and crystal structures remain unaffected. The symmetry-broken state exhibits a dipole moment, and its polar axis can be controlled with the incident light. Furthermore, our results establish a coherent nonlinear optical protocol by which to break electronic symmetries and produce unconventional electronic effects in solids.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Design of an optical amplifier for amplified OSC in IOTA facility at Fermilab

Optical stochastic cooling (OSC) is a cutting-edge beam cooling technology to reduce, control the 3 dimensional spread and the motion of particle beams. It has recently been successfully, experimentally, demonstrated in Fermilab's IOTA storage ring, marking a major step forward in beam cooling. OSC has the potential to significantly improve both the performance and flexibility as a beam cooling system. One promising way to boost OSC performance is by adding a high-gain optical amplifier. However, this amplifier must be carefully designed to meet the specific constraints of the OSC system. A major challenge lies in the limited optical delay, which is just 6 mm for the case of IOTA, set by the beam bypass, restricts us to use a short-length gain medium. This, along with IOTA’s high repetition rate and the relatively long duration of the optical pulses, limits the peak power available for the pump laser without damaging the crystal, which is crucial for achieving strong nonlinear gain. Additionally, it's essential to preserve the phase coherence of the undulator radiation during amplification, which further complicates the amplifier design. This report details a specialized amplifier setup that addresses these challenges, includes simulations of the integrated system, and summarizes the latest experimental progress and results.

Mondal, Abhishek [Fermilab]↗
NASA NTRS1992

CONCAP 4: A Complex Autonomous Payload (CAP) for growing organic thin films in microgravity

A GAS facility has been developed for carrying out low temperature experiments. The arrangement being used on CONCAP IV-01 is designed for thin film growth in microgravity and can process up to twelve samples per mission. The nonlinear optical oven hardware can also be made suitable for other low temperature applications, such as gradient freeze and solution growth of crystals.

Carswell, W. E.↗