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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Direct visualization and control of antiferromagnetic domains and spin reorientation in a parent cuprate

Here, we report magnetic optical second-harmonic generation (SHG) polarimetry and imaging on Sr 2 Cu 3 O 4 Cl 2 , which allows direct visualization of the mesoscopic antiferromagnetic (AFM) structure of a parent cuprate. Temperature- and magnetic-field-dependent SHG reveals large domains with 90° relative orientations that are stabilized by a combination of uniaxial magnetic anisotropy and the Earth's magnetic field. Below a temperature T R ~ 97 K, we observe an unusual 90° spin reorientation transition, possibly driven by competing magnetic anisotropies of the two copper sublattices, which swaps the AFM domain states while preserving the domain structure. This allows deterministic switching of the AFM states by thermal or laser heating. Near T R , the domain walls become exceptionally responsive to an applied magnetic field, with the Earth's field sufficient to completely expel them from the crystal. Our findings unlock opportunities to study the mesoscopic AFM behavior of parent cuprates and explore their potential for AFM technologies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Spatio-temporal electric field distributions in an atmospheric plasma jet impinging on a microchannel array surface

The electric field distribution in the ionization waves (IWs) propagating over a microchannel array dielectric surface, with the channels either empty or filled with distilled water, is measured by ps electric field induced second harmonic generation. The surface IW is initiated by the atmospheric pressure N 2 –Ar plasma jet impinging on the surface vertically and powered by ns pulse discharge bursts. The results show that the electric field inside the microchannels, specifically its horizontal component, is enhanced by up to a factor of 2. The field enhancement region is localized within the channels. The vertical electric field inside the channels lags in time compared to the field measured at the ridges, indicating the transient reversal of the IW propagation direction across the channels (toward the jet). This is consistent with the phase-locked plasma emission images and confirmed by the kinetic modeling predictions, which show that the IW ‘jumps’ over the empty channels and propagates into the channels only after the jump between the adjacent ridges. When the channels are filled with water, the wave speed increases by up to 50%, due to the higher effective dielectric constant of the surface. No evidence of a significant electric field enhancement near the dielectric surface (ceramic or water) has been detected, within the spatial resolution of the present diagnostic, ~100 μ m.

plasmas and liquids↗
DOE OSTI2023

Extrinsic Nonlinear Kerr Rotation in Topological Materials under a Magnetic Field

Topological properties in quantum materials are often governed by symmetry and tuned by crystal structure and external fields, and hence, symmetry-sensitive nonlinear optical measurements in a magnetic field are a valuable probe. Here, we report nonlinear magneto-optical second harmonic generation (SHG) studies of nonmagnetic topological materials including bilayer WTe 2 , monolayer WSe 2 , and bulk TaAs. The polarization-resolved patterns of optical SHG under a magnetic field show nonlinear Kerr rotation in these time-reversal symmetric materials. For materials with 3-fold rotational symmetric lattice structure, the SHG polarization pattern rotates just slightly in a magnetic field, whereas in those with mirror or 2-fold rotational symmetry, the SHG polarization pattern rotates greatly and distorts. Further, these different magneto-SHG characters can be understood by considering the superposition of the magnetic field-induced time-noninvariant nonlinear optical tensor and the crystal-structure-based time-invariant counterpart. The situation is further clarified by scrutinizing the Faraday rotation, whose subtle interplay with crystal symmetry accounts for the diverse behavior of the extrinsic nonlinear Kerr rotation in different materials. Our work illustrates the application of magneto-SHG techniques to directly probe nontrivial topological properties, and underlines the importance of minimizing extrinsic nonlinear Kerr rotation in polarization-resolved magneto-optical studies.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Stabilization of the Polar Structure and Giant Second-Order Nonlinear Response of Single Crystal γ-NaAs 0.95 Sb 0.05 Se 2

The dearth of suitable materials significantly restricts the practical development of infrared (IR) laser systems with highly efficient and broadband tuning. Recently, γ-NaAsSe 2 is reported, and it exhibits a large nonlinear second-harmonic generation (SHG) coefficient of 590 pm V —1 at 2 µm. However, the crystal growth of γ-NaAsSe 2 is challenging because it undergoes a phase transition to centrosymmetric δ-NaAsSe 2 . Herein, the stabilization of non-centrosymmetric γ-NaAsSe 2 by doping the As site with Sb, which results in γ-NaAs 0.95 Sb 0.05 Se 2 is reported. The congruent melting behavior is confirmed by differential thermal analysis with a melting temperature of 450 °C and crystallization temperature of 415 °C. Single crystals with dimensions of 3 mm × 2 mm are successfully obtained via zone refining and the Bridgman method. The purification of the material plays a significant role in crystal growth and results in a bandgap of 1.78 eV and thermal conductivity of 0.79 Wm —1 K —1 . The single-crystal SHG coefficient of γ-NaAs 0.95 Sb 0.05 Se 2 exhibits an enormous value of |d 11 | = 648 ± 74 pm V —1 , which is comparable to that of γ-NaAsSe 2 and ≈20× larger than that of AgGaSe 2 . Importantly, the bandgap of γ-NaAs 0.95 Sb 0.05 Se 2 (1.78 eV) is similar to that of AgGaSe 2 , thus rendering it highly attractive as a high-performing nonlinear optical material.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Decoding THz‐Driven Dynamic Fingerprints of Ferroelectric Nanotwin Networks

Ultrafast polarization dynamics in ferroelectrics are of considerable interest for high-speed tunable dielectrics and electro-optics. Extended domain wall networks formed in ferroelectric twin nanodomains can support collective dynamics in the terahertz regime but require techniques that track polarization and strain evolution driven by ultrafast stimulus. Here, we use multi-modal probing of THz-pulse-driven excitations in PbTiO 3 /SrTiO 3 superlattices by combining X-ray free electron laser measurements that directly tracks lattice changes, with optical second harmonic generation that tracks the electronic potential coupled with the lattice potential. Dynamical phase-field modeling enables fingerprinting of these collective modes as superpositions of domain “breathing” through wall oscillations and polarization “rotations” with still walls. Ultrafast domain wall motion at 0.1–0.5 THz is observed at practical fields of 100 kV/cm with wall velocities of >4000 m/s, approaching typical speed of sound in PbTiO 3 . A unique “charging” mode is discovered that can electrically charge and discharge domain walls on ∼4 ps time scale thus dynamically tuning wall conductivity. Integrated experimental and theoretical fingerprinting of the dynamical landscape presented here enables ultrafast control of ferroics for high-speed microelectronics and optical applications.

THz dynamics↗
DOE OSTI2024

Single-mode squeezed-light generation and tomography with an integrated optical parametric oscillator

Quantum optical technologies promise advances in sensing, computing, and communication. A key resource is squeezed light, where quantum noise is redistributed between optical quadratures. We introduce a monolithic, chip-scale platform that exploits the χ (2) nonlinearity of a thin-film lithium niobate (TFLN) resonator device to efficiently generate squeezed states of light. Our system integrates all essential components—except for the laser and two detectors—on a single chip with an area of one square centimeter, reducing the size, operational complexity, and power consumption associated with conventional setups. Using the balanced homodyne measurement subsystem that we implemented on the same chip, we measure a squeezing of 0.55 decibels and an anti-squeezing of 1.55 decibels. We use 20 milliwatts of input power to generate the parametric oscillator pump field by using second harmonic generation on the same chip. Our work represents a step toward compact and efficient quantum optical systems posed to leverage the rapid advances in integrated nonlinear and quantum photonics.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2026

Enhanced Second and Third Harmonic Generations in Metasurfaces Enabled through Point Group Design and Accidental Bound States in the Continuum

Here, we investigate enhanced second‑ and third‑harmonic generation (SHG and THG) in GaAs metasurfaces by combining electromagnetic point‑group designs with accidental bound states in the continuum (BICs). Using group theory, we predict the existence, suppression, and polarization selection rules of SHG and THG for metasurfaces belonging to the D 2h and C 2v point groups. In D 2h metasurfaces, inversion symmetry suppresses SHG while enabling polarization‑selective THG, which is strongly enhanced near accidental BICs with ultrahigh Q‑factors approaching 107. By breaking inversion symmetry to form C 2v metasurfaces through the introduction of nanogaps, SHG is now allowed and is dramatically enhanced near accidental BICs. Importantly, accidental BICs preserve polarization selection rules while providing a robust parameter range for high‑Q resonances, in contrast to quasi‑BICs induced by symmetry breaking. Our results demonstrate that the combination of point‑group theory and accidental‑BIC engineering offers a predictive and robust route toward highly efficient nonlinear metasurfaces.

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

The Dual Wavelength UV Transmitter Development for Space Based Ozone DIAL Measurements

The objective of this research is to develop efficient 1-micron to UV wavelength conversion technology to generate tunable, single mode, pulsed UV wavelengths of 320 nm and 308 nm. The 532 nm wavelength radiation is generated by a 1064 nm Nd:YAG laser through second harmonic generation. The 532 nm pumps an optical parametric oscillator (OPO) to generate 803 nm. The 320 nm is generated by sum frequency generation (SFG) of 532 nm and 803 nm wavelengths The hardware consists of a conductively cooled, 1 J/pulse, single mode Nd:YAG pump laser coupled to an efficient RISTRA OPO and SFG assembly-Both intra and extra-cavity approaches are examined for efficiency.

Prasad, Narasimha S.↗
DOE OSTI2024

Frequency-domain computing using nonlinear acoustic-wave device on lithium niobate

Abstract Multiply-accumulation are crucial computing operations in signal processing, numerical simulations, and machine learning. In recent years, optical analog approaches have demonstrated higher computing performance and better power efficiency than their digital counterparts. However, analog computing chips usually need large areas and complex structures for parallel computing, as a single device element only executes one computing operation at a single time. Here, we demonstrate frequency-domain computing using the nonlinear acoustic-wave devices on lithium niobate, featuring a normalized external second-harmonic generation conversion efficiency of ~ 5.7 × 10-4 W-1. The second-order sum-frequency nonlinear process of lithium niobate enables multiplication of inputs encoded in the frequency domain. Compared to the analog schemes, our device features a notably simpler design, and nanofabrication requires only one lift-off. Using a single acoustic-wave device within an area of 0.03 mm2, we can simultaneously conduct over 130,000 multiply-accumulation operations. Our acoustic-wave device shows applications in real and complex vector convolutions and image processing. This demonstration sets the stage for experimental realizations into frequency-domain integrated nonlinear acoustic computing systems, potentially shaping future developments in acoustic neural networks and quantum computing.

chai, mingzhao (ORCID:0009000466226341)↗
DOE OSTI2026

Nonlinear regenerative amplification using tunable intracavity cascaded quadratic nonlinearities

Conventional nonlinear regenerative amplification utilizes Kerr (i.e., self-focusing) nonlinearity to broaden the spectrum via self-phase modulation during the direct amplification of ultrashort pulses, which helps overcome spectral gain narrowing for high-energy, ultrashort-pulse generation. We introduce cascaded quadratic nonlinearities from a type-I second-harmonic generation crystal, which can be tuned in both magnitude and sign via the phase-mismatching condition, inside a regenerative amplifier to enable nonlinearity-tunable regenerative amplification. We demonstrate, both experimentally and numerically, a nonlinear Yb:YAG thin-disk regenerative amplifier with either positive or negative net nonlinearity that delivers 1-kHz, >0.4-mJ pulses as short as ∼200 fs and high-quality beams free of self-focusing. The laser’s average power can be scaled to >100 W when seeded and operated at a much higher repetition rate to benefit various applications.

47 OTHER INSTRUMENTATION↗
NASA NTRS1993

Generation of 369.4 nm Radiation by Efficient Doubling of a Diode Laser

A resonant cavity second harmonic generation system has been developed to produce 369.4 nm radiation from a 738.8 nm diode laser with 10 mW nominal output power. This system utilizes a polarization technique to lock the cavity to the laser frequency. In this paper we report on an evaluation of the system using a Titanium:Sapphire laser as the input source, and preliminary results with a diode laser source. To our knowledge, this is the deepest uv light ever produced by frequency-doubling a diode laser.

Williams, A.↗
NASA NTRS2008

Single-mode, All-Solid-State Nd:YAG Laser Pumped UV Converter

In this paper, the status of a high-energy, all solid-state Nd:YAG laser pumped nonlinear optics based UV converter development is discussed. The high-energy UV transmitter technology is being developed for ozone sensing applications from space based platforms using differential lidar technique. The goal is to generate greater than 200 mJ/pulse with 10-50 Hz PRF at wavelengths of 308 nm and 320 nm. A diode-pumped, all-solid-state and single longitudinal mode Nd:YAG laser designed to provide conductively cooled operation at 1064 nm has been built and tested. Currently, this pump laser provides an output pulse energy of >1 J/pulse at 50 Hz PRF and a pulsewidth of 22 ns with an electrical-to-optical system efficiency of greater than 7% and a M(sup 2) value of <2. The single frequency UV converter arrangement basically consists of an IR Optical Parametric Oscillator (OPO) and a Sum Frequency Generator (SFG) setups that are pumped by 532 nm wavelength obtained via Second Harmonic Generation (SHG). In this paper, the operation of an inter cavity SFG with CW laser seeding scheme generating 320 nm wavelength is presented. Efforts are underway to improve conversion efficiency of this mJ class UV converter by modifying the spatial beam profile of the pump laser.

Prasad, Narasimha S.↗
DOE OSTI2023

Plasma Emission, Wave Speeds, and Temperatures of Laser-Supported Plasmas in Air

A study of the generation and subsequent expansion of plasmas using a single beam (532 nm) from the second harmonic generator of a Q-switched Nd:YAG laser is described. The plasmas in air are studied using an intensified charge-coupled device camera over periods of 1000 ns following the laser pulses. The plasma experimental results are interpreted in terms of wave speeds and plasma temperatures. Energy balance equations are considered to estimate the plasma temperatures and the laser-supported radiation (LSR) and the laser-supported detonation (LSD) wave speeds. Within 1000 ns observation time, the circular spectral images turn elliptical because of plasma expansion toward the laser beam. The plasma expansion increases with increasing laser irradiance. A laser irradiance range of [Formula: see text] yields LSR wave speeds between 45 and 170 km/s and LSD wave speeds of 90–130 km/s. The measured wave speeds are compared with the LSR and the LSR wave speed models. The plasma temperatures are between 90,000 and 120,000 K at 15 ns after the laser pulse based on measured emission spectra and are between 640,000 and 760,000 K at 3 ns based on the LSR model.

Engineering↗
NASA NTRS1995

Generation Of 369.4-Nanometers Second Harmonic From A Diode Laser

Experimental laser system features polarization feedback scheme maintaining frequency lock. Generates light at wavelength of 369.4 nanometers by second-harmonic generation from 738.8-nanometers laser diode. System prototype of source of 369.4-nanometers radiation used to optically pump 2S1/2 ' 2P1/2 transition in 171Yb+ ions in lightweight, low-power trapped-ion frequency-standard apparatus.

Williams, Angelyn P.↗
DOE OSTI2022

Electric field distribution in a non-self-sustained RF discharge with ionization generated by Ns discharge pulses

Abstract Electric field in a capacitively coupled, non-self-sustained RF discharge nitrogen plasma with external ionization generated by high-voltage ns pulses has been measured by ps Electric field induced second harmonic generation (EFISH). The measurements are made both in the bulk of the plasma and in the sheaths, using the absolute calibration by the Laplacian field between two plane electrodes. The results are compared with the kinetic modeling calculations. The RF electric field in the sheaths is significantly higher compared to that in the plasma, due to the displacement of the electrons by the drift oscillations and the resultant plasma self-shielding. However, the kinetic modeling predictions indicate that the electron impact ionization in the sheaths is largely ineffective, due to the low electron density. The reduction of the electric field in the plasma by the self-shielding in the sheaths is moderate, such that the energy is coupled to the plasma by the below-breakdown RF field. The peak RF field in the plasma is in the range of 15–25 Td, indicating the efficient vibrational excitation of N 2 by electron impact. The modeling predictions suggest that the targeted vibrational excitation of molecular species in a non-self-sustained RF discharge with external ionization is scalable to high pressures, electron densities, and discharge powers. The present approach can be extended to the vibrational excitation of other molecular species where the vibrational relaxation is relatively slow, such as CO, CO 2 , and H 2 .

Physics↗
NASA NTRS1995

Growth of single crystals of organic salts with large second-order optical nonlinearities by solution processes for devices

Data obtained from the electric field induced second harmonic generation (EFISH) and Kurtz Powder Methods will be provided to MSFC for further refinement of their method. A theoretical model for predicting the second-order nonlinearities of organic salts is being worked on. Another task is the synthesis of a number of salts with various counterions. Several salts with promising SHG activities and new salts will be tested for the presence of two crystalline forms. The materials will be recrystallized from dry and wet solvents and compared for SHG efficiency. Salts that have a high SHG efficiency and no tendency to form hydrates will be documented. The synthesis of these materials are included in this report. A third task involves method to aid in the growth of large, high quality single crystals by solution processes. These crystals will be characterized for their applicability in the fabrication of devices that will be incorporated into optical computers in future programs. Single crystals of optimum quality may be obtained by crystal growth in low-gravity. The final task is the design of a temperature lowering single crystal growth apparatus for ground based work. At least one prototype will be built.

Leslie, Thomas M.↗
DOE OSTI2024

High-efficiency, single-stage tunable optical parametric amplifier for visible photocathode applications

In this work we present a single-stage optical parametric amplifier (OPA) with an average conversion efficiency up to 38%, tunable between 1.01 and 1.18 µm. The OPA seed is produced by a gain-managed nonlinear fiber amplifier. Numerical modeling of the seed pulse generation shows a linear chirp, a smoothly broadened redshifted spectrum, and a high spectral energy density. When up-converted to the visible through second-harmonic generation, the signal pulses are suitable for visible photocathode excitation.

14 SOLAR ENERGY↗