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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 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Dispersion of the Nonlinear Susceptibility of MoS2 and WS2 from Second-Harmonic Scattering Spectroscopy

Dispersion of the absolute second-order susceptibility of both MoS2 and WS2 is assessed on a wide spectral excitation range (710–1300 nm) by using second-harmonic scattering spectroscopy (SHS). SHS is an accurate ensemble measurement here applied on well-dispersed suspensions of monodisperse liquid-exfoliated nanosheets showing a high monolayer content. The as-derived, high susceptibility values shed light on the discrepancies between available literature values while evidencing resonances associated with the main excitonic transitions.

CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SU↗
DOE OSTI2024

QRCODE: Massively parallelized real-time time-dependent density functional theory for periodic systems

We present a new software module, QRCODE (Quantum Research for Calculating Optically Driven Excitations), for massively parallelized real-time time-dependent density functional theory (RT-TDDFT) calculations of periodic systems in the open-source Qbox software package. Our approach utilizes a custom implementation of a fast Fourier transformation scheme that significantly reduces inter-node message passing interface (MPI) communication of the major computational kernel and shows impressive scaling up to 16,344 CPU cores. In addition to improving computational performance, QRCODE contains a suite of various time propagators for accurate RT-TDDFT calculations. As benchmark applications of QRCODE, we calculate the current density and optical absorption spectra of hexagonal boron nitride (h-BN) and photo-driven reaction dynamics of the ozone-oxygen reaction. We also calculate the second and higher harmonic generation of monolayer and multi-layer boron nitride structures as examples of large material systems. Our optimized implementation of RT-TDDFT in QRCODE enables large-scale calculations of real-time electron dynamics of chemical and material systems with enhanced computational performance and impressive scaling across several thousand CPU cores.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2022

Near-zero-index ultra-fast pulse characterization

Transparent conducting oxides exhibit giant optical nonlinearities in the near-infrared window where their linear index approaches zero. Despite the magnitude and speed of these nonlinearities, a “killer” optical application for these compounds has yet to be found. Because of the absorptive nature of the typically used intraband transitions, out-of-plane configurations with short optical paths should be considered. In this direction, we propose an alternative frequency-resolved optical gating scheme for the characterization of ultra-fast optical pulses that exploits near-zero-index aluminium zinc oxide thin films. Besides the technological advantages in terms of manufacturability and cost, our system outperforms commercial modules in key metrics, such as operational bandwidth, sensitivity, and robustness. The performance enhancement comes with the additional benefit of simultaneous self-phase-matched second and third harmonic generation. Because of the fundamental importance of novel methodologies to characterise ultra-fast events, our solution could be of fundamental use for numerous research labs and industries.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2026

Peptide‐Induced Ferroelectricity in Charge‐Transfer Supramolecular Materials

Organic ferroelectrics are of great interest in sustainable energy conversion, information storage, flexible electronics, and potential biomedical applications as soft implants, among many other applications. Despite their broad potential, the development of organic ferroelectrics has remained limited, with only a few known examples in solid-state systems, primarily due to the lack of well-established design strategies compared to inorganic systems. Bio-inspired supramolecular chemistry offers a path to create functional nanostructures that are water-processable and biocompatible. We report here on supramolecular charge transfer (CT) systems in which peptides are covalently linked to dyads of electron-donating and electron-accepting moieties, creating amphiphiles that self-assemble into nanoscale ribbons in water. The peptide chirality-induced symmetry breaking in these crystalline nanostructures not only results in second harmonic activity but also generates ferroelectric behavior across multiple CT systems, demonstrating a versatile supramolecular approach to the design of new organic ferroelectrics. Furthermore, culturing primary neuron cells on coatings of the ferroelectric materials promoted axonal growth and enhanced action potentials, indicating improved neuronal maturity facilitated by the polar structure of the ferroelectric nanomaterials. The supramolecular strategy used here holds promise to create new water-processable ferroelectric biomaterials, opening avenues for innovative applications in cell charge transfer, neuronal axon growth, peptide symmetry breaking, self-assembling peptides, supramolecular ferroelectrics, proliferation, and bioelectronics.

charge transfer↗
DOE OSTI2022

Non-premixed counterflow methane flames in DC/AC/NS electric fields

The response of counterflow diffusion flames to sub-breakdown DC and AC electric fields, as well as their superposition with ns pulse discharge waveforms, is studied in the plane-to-plane electrode geometry. Sub-breakdown DC and low-frequency AC electric fields cause the flame displacement toward the grounded electrode, in the direction of the applied field, indicating that the body force on the positive ions exceeds that on the electrons and negative ions. As the AC frequency increases, the flame response becomes less pronounced, due to the reduction of the electrohydrodynamic (EHD) body force impulse over the AC half-period. The electric field in the electrode gap is determined by ps Electric Field Induced Second Harmonic (E-FISH) generation, with absolute calibration using sub-breakdown ns pulses overlapped with the measured electric field waveform. The results show that the electric field distribution across the flame in the current saturation regime follows the Laplacian field. This indicates that the space charge density in the gap is too low to distort the applied DC or AC field, consistent with the kinetic modeling predictions. Combining a nanosecond pulse discharge with a sub-breakdown DC field generates a diffuse plasma across the entire gap. Time-resolved and spatially resolved measurements of the electric field in the discharge indicate the ionization wave propagation between the electrodes. The present results do not exhibit a detectable flame displacement enhancement by ns discharge pulses combined with a sub-breakdown field, observed previously. Kinetic modeling calculations show that the absence of this effect in the plane-to-plane geometry is due to the rapid plasma self-shielding. This indicates that alternative electrode geometries limiting the self-shielding would be more effective for the plasma / electric field enhanced flameholding and flame stabilization applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

X-ray pulse generation with ultra-fast flipping of its orbital angular momentum

A method to temporally tailor the properties of X-ray radiation carrying Orbital Angular Momentum (OAM) is presented. In simulations, an electron beam is prepared with a temporally modulated micro-bunching structure which, when radiating at the second harmonic in a helical undulator, generates OAM light with a corresponding temporally modulated intensity. This method is shown to generate attosecond pulse trains of OAM light without the need for any additional external optics, making the wavelength range tunable. In addition to the OAM pulse train, the method can be adapted to generate radiation where the handedness of the OAM mode may also be temporally modulated (flipped).

43 PARTICLE ACCELERATORS↗
DOE OSTI2024

Wavelength modulation laser-induced fluorescence for plasma characterization

Laser-Induced Fluorescence (LIF) spectroscopy is an essential tool for probing ion and atom velocity distribution functions (VDFs) in complex plasmas. VDFs carry information about the kinetic properties of species that is critical for plasma characterization. Accurate interpretation of these functions is challenging due to factors such as multicomponent distributions, broadening effects, and background emissions. Our research investigates the use of Wavelength Modulation (WM) LIF to enhance the sensitivity of VDF measurements. Unlike standard Amplitude Modulation (AM) methods, WM–LIF measures the derivative of the LIF signal. This approach makes variations in VDF shape more pronounced. VDF measurements with WM–LIF were investigated with both numerical modeling and experimental measurements. The developed model enables the generation of both WM and AM signals, facilitating comparative analysis of fitting outcomes. Experiments were conducted in a weakly collisional argon plasma with magnetized electrons and non-magnetized ions. Measurements of the argon ion VDFs employed a narrow-band tunable diode laser, which scanned the 4p 4 D 7/2 –3d 4 F 9/2 transition centered at 664.553 nm in vacuum. A lock-in amplifier detected the second harmonic WM signal, which was generated by modulating the laser wavelength with an externally controlled piezo-driven mirror of the diode laser. Finally, our findings indicate that the WM–LIF signal is more sensitive to fitting parameters, allowing for better identification of VDF parameters such as the number of distribution components, their temperatures, and velocities. In addition, WM–LIF can serve as an independent method to verify AM measurements and is particularly beneficial in environments with substantial light noise or background emissions, such as those involving thermionic cathodes and reflective surfaces.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Unconventional fieldlike spin torques in CrPt 3

The topological semimetal CrPt 3 has potential for generating unconventional spin torques due to its ferrimagnetic ordering, topological band structure, and high anomalous Hall effect. CrPt 3 exhibits ferrimagnetic behavior only in its chemically ordered phase and is paramagnetic in its chemically disordered phase. By controlling the growth and annealing temperatures, we prepare epitaxial films of both chemically ordered and chemically disordered phases of CrPt 3 , allowing us to investigate the effect of magnetic ordering on unconventional-torque generation. We use angle-dependent spin-torque-ferromagnetic-resonance and second-harmonic Hall measurements to probe the spin torques generated from epitaxial CrPt 3 in CrPt 3 /Cu/Ni 81 ⁢Fe 19 heterostructures. With current applied along specific directions with respect to the crystal order, we reveal unconventional spin torques in both ordered and disordered films. When current flows parallel to the [$1\bar{1}1$] and [ $\bar{1}11$] directions, we observe an unconventional fieldlike torque that is opposite in sign for the two directions. Finally, our calculations reveal that this unconventional torque originates from an indirect nonlocal spin-orbit torque due to spin scattering at the CrPt 3 /Cu interface, in addition to symmetry breaking at this interface.

ferromagnetic resonance↗
DOE OSTI2025

Second harmonic Bessel-Gauss beam shaping with elliptic axicon aberrations

The second harmonic (SH) of an axicon generated Bessel-Gauss beam is created through the nonlinear interaction of photons with a crystal, resulting in the energy doubling of the output photons. In this work, we show experimentally that in addition to frequency doubling, the SH of Bessel-Gauss beams under asymmetric aberrations from an elliptic axicon exhibit intriguing beam formation. Particularly, the central region of the SH beam profile is composed of two central spots of various geometries surrounded by nested ellipses; one of which is the configuration of two central gamma dots with similar radius knotted by nested ellipses for a zeroth-order Bessel-Gauss pump. These SH beams consistently maintain their spatial profile throughout propagation, reminiscing the behavior of screw dislocations in wave patterns. Our numerical simulations produce beam dynamics consistent with that of experiments and further implicate the remarkable interweaving of bright spots with dark vortices. This is especially noticeable when the beams dynamically oscillate along the optical axis, resulting in the genesis of spatially polarized beams with a knotted framework. The insights gained from our study establish a novel paradigm for exploring interactions of Bessel-like beams with vortex dynamics. This, in turn, has the potential to spark innovations in optical applications, fostering new methodologies to harness and manipulate complex light structures. Our experimental findings could spur new methods of generating logical states of light and new opportunities for material processing control. Published by the American Physical Society 2025

Wang, Tianhong (ORCID:0000000169104201)↗
DOE OSTI2022

Random quasi-phase-matching for pulse characterization from the near to the long wavelength infrared

Experiments requiring ultrafast laser pulses require a full characterization of the electric field to glean meaning from the experimental data. Such characterization typically requires a separate parametric optical process. As the central wavelength range of new sources continues to increase so too does the need for nonlinear crystals suited for characterizing these wavelengths. Here we report on the use of poly-crystalline zinc selenide as a universal nonlinear crystal in the frequency resolved optical gating characterization technique from the near to long-wavelength infrared. Due to its property of random quasi-phase-matching it’s capable of phase matching second-harmonic and sum-frequency generation of ultra-broadband pulses in the near and long wavelength infrared, while being crystal orientation independent. With the majority of ultra-fast laser sources being in this span of wavelengths, this work demonstrates a greatly simplified approach towards ultra-fast pulse characterization spanning from the near to the long-wavelength infrared. To our knowledge there is no single optical technique capable of such flexible capabilities.

Davis, Brandin (ORCID:0000000166964548)↗
DOE OSTI2025

Directionally asymmetric nonlinear optics in ferrorotational MnTiO 3

Ferrorotationally ordered materials possess a planar chiral lattice of electric dipoles that are a promising platform for exhibiting directionally asymmetric response functions. A key characteristic of such order is that enantiomorph conversion occurs when the solid is flipped by 180° about an in-plane axis. Using second-harmonic interferometry, we show here that when circularly polarized light is incident on MnTiO 3 , the generated harmonic intensity depends on whether the incident light is parallel or antiparallel to the ferrorotational axis. For a particular photon helicity, constructive interference occurs in one direction while destructive interference occurs in the other. Here, our observations represent a fundamentally new optical effect, associated with circularly polarized light in ferrorotational solids, that is distinct from conventional optical activity observed in three-dimensional chiral and Faraday media.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Dephasingless two-color terahertz generation

A laser pulse composed of a fundamental and an appropriately phased second harmonic can drive a time-dependent current of photoionized electrons that generates broadband THz radiation. Over the propagation distances relevant to many experiments, dispersion causes the relative phase between the harmonics to evolve. This “dephasing” slows the accumulation of THz energy and results in a multi-cycle THz pulse with significant angular dispersion. Here, we introduce a novel optical configuration that compensates the relative phase evolution, allowing for the formation of a half-cycle THz pulse with almost no angular dispersion. The configuration uses the spherical aberration of an axilens to map a prescribed radial phase variation in the near field to a desired longitudinal phase variation in the far field. Simulations that combine this configuration with an ultrashort flying focus demonstrate the formation of a half-cycle THz pulse with a controlled emission angle and 1/4 the angular divergence of the multi-cycle pulse created by a conventional optical configuration.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Second-order magnetic responses in quantum magnets: Magnetization under ac magnetic fields

Here we investigate second-order magnetic responses of quantum magnets against ac magnetic fields. We focus on the case where the z component of the spin is conserved in the unperturbed Hamiltonian and the driving field is applied in the xy plane. We find that linearly polarized driving fields induce a second-harmonic response, while circularly polarized fields generate only a zero-frequency response, leading to a magnetization with a direction determined by the helicity. Employing an unbiased numerical method, we demonstrate the nonlinear magnetic effect driven by the circularly polarized field in the XXZ model and show that the magnitude of the magnetization can be predicted by the dynamical spin structure factor in the linear response regime.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Demonstration of a kilowatt average power, 1 J, green laser

A λ = 515 nm laser generating joule-level pulses at 1 kHz repetition rate was demonstrated by frequency doubling 1.2 J, 2 ns temporally shaped square pulses from a cryogenically cooled Yb:YAG laser in an LBO crystal. A doubling efficiency of 78% resulted in 0.94 J second-harmonic pulses at 1 kHz. The unconverted light interacted with a second LBO crystal to generate > 100 mJ second-harmonic pulses to reach a total green average power of 1.04 kW. A conversion efficiency of 89% was achieved for 0.58 J green pulses at 1 kHz. These results open the possibility to pump high energy femtosecond lasers at kilohertz repetition rates.

42 ENGINEERING↗
DOE OSTI2024

Spatiotemporal control of two-color terahertz generation

A laser pulse composed of a fundamental and properly phased second harmonic exhibits an asymmetric electric field that can drive a time-dependent current of photoionized electrons. The current produces an ultrashort burst of terahertz (THz) radiation. When driven by a conventional laser pulse, the THz radiation is emitted into a cone with an angle determined by the dispersion of the medium. Here we demonstrate that the programmable-velocity intensity peak of a spatiotemporally structured, two-color laser pulse can be used to control the emission angle, focal spot, and spectrum of the THz radiation. Of particular interest for applications, a structured pulse with a subluminal intensity peak can drive highly focusable, on-axis THz radiation. Published by the American Physical Society 2024

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Cascaded Optical Nonlinearities in Dielectric Metasurfaces

Since the discovery of the laser, optical nonlinearities have been at the core of efficient light conversion sources. Typically, thick transparent crystals or quasi-phase matched waveguides are utilized in conjunction with phase-matching techniques to select a single parametric process. In recent years, due to the rapid developments in artificially structured materials, optical frequency mixing has been achieved at the nanoscale in subwavelength resonators arrayed as metasurfaces. Phase matching becomes relaxed for these wavelength-scale structures, and all allowed nonlinear processes can, in principle, occur on an equal footing. This could promote harmonic generation via a cascaded (consisting of several frequency mixing steps) process. However, so far, all reported work on dielectric metasurfaces have assumed frequency mixing from a direct (single step) nonlinear process. In this work, we prove the existence of cascaded second-order optical nonlinearities by analyzing the second- and third-wave mixing from a highly nonlinear metasurface in conjunction with polarization selection rules and crystal symmetries. We find that the third-wave mixing signal from a cascaded process can be of comparable strength to that from conventional third-harmonic generation and that surface nonlinearities are the dominant mechanism that contributes to cascaded second-order nonlinearities in our metasurface.

36 MATERIALS SCIENCE↗
DOE OSTI2024

The Role of Laser Wavelength on the Early-stage Electron Density Evolution in Laser-Produced Plasma

In this study, a laser-produced plasma (LPP) was generated by focusing fundamental (1064 nm), second (532nm), and fourth (266 nm) harmonic radiation from a 6 ns Nd:YAG laser at a laser intensity of 10 GW/cm2 onto a copper target placed in vacuum. The early time evolution of the plasma between 0-70 ns following laser ablation was then analyzed using Nomarski interferometry. The dependence of plasma properties such as the electron density distribution, plume velocity, and plume morphology on the laser wavelength are discussed.

(280.5395) Plasma Diagnostics, (140.3440) Laser-in↗