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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 919 records · Page 51
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Broad Frequency Shift of Parametric Processes in Epsilon-Near-Zero Time-Varying Media

The ultrafast changes of material properties induced by short laser pulses can lead to a frequency shift of reflected and transmitted radiation. Recent reports highlight how such a frequency shift is enhanced in spectral regions where the material features a near-zero real part of the permittivity. Here, we investigate the frequency shift for fields generated by four-wave mixing. In our experiment, we observed a frequency shift of more than 60 nm (compared to the pulse width of ~40 nm) in the phase conjugated radiation generated by a 500 nm aluminium-doped zinc oxide (AZO) film pumped close to the epsilon-near-zero wavelength. Our results indicate applications of time-varying media for nonlinear optics and frequency conversion.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Selected Area Deposition of High Purity Gold for Functional 3D Architectures

Selected area deposition of high purity gold films onto nanoscale 3D architectures is highly desirable as gold is conductive, inert, plasmonically active, and can be functionalized with thiol chemistries, which are useful in many biological applications. Here, we show that high-purity gold coatings can be selectively grown with the Me 2 Au (acac) precursor onto nanoscale 3D architectures via a pulsed laser pyrolytic chemical vapor deposition process. The selected area of deposition is achieved due to the high thermal resistance of the nanoscale geometries. Focused electron beam induced deposits (FEBID) and carbon nanofibers are functionalized with gold coatings, and we demonstrate the effects that laser irradiance, pulse width, and precursor pressure have on the growth rate. Furthermore, we demonstrate selected area deposition with a feature-targeting resolutions of ~100 and 5 µm, using diode lasers coupled to a multimode (915 nm) and single mode (785 nm) fiber optic, respectively. The experimental results are rationalized via finite element thermal modeling.

3-dimensional nanostructures↗
DOE OSTI2023

Near-field terahertz nonlinear optics with blue light

Abstract The coupling of terahertz optical techniques to scattering-type scanning near-field microscopy (s-SNOM) has recently emerged as a valuable new paradigm for probing the properties of semiconductors and other materials on the nanoscale. Researchers have demonstrated a family of related techniques, including terahertz nanoscopy (elastic scattering, based on linear optics), time-resolved methods, and nanoscale terahertz emission spectroscopy. However, as with nearly all examples of s-SNOM since the technique’s inception in the mid-1990s, the wavelength of the optical source coupled to the near-field tip is long, usually at energies of 2.5 eV or less. Challenges in coupling of shorter wavelengths (i.e., blue light) to the nanotip has greatly inhibited the study of nanoscale phenomena in wide bandgap materials such as Si and GaN. Here, we describe the first experimental demonstration of s-SNOM using blue light. With femtosecond pulses at 410 nm, we generate terahertz pulses directly from bulk silicon, spatially resolved with nanoscale resolution, and show that these signals provide spectroscopic information that cannot be obtained using near-infrared excitation. We develop a new theoretical framework to account for this nonlinear interaction, which enables accurate extraction of material parameters. This work establishes a new realm of possibilities for the study of technologically relevant wide-bandgap materials using s-SNOM methods.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Active Cancellation of Servo-Induced Noise on Stabilized Lasers via Feedforward

Many precision laser applications require active frequency stabilization. However, such stabilization loops operate by pushing noise to frequencies outside their bandwidth, leading to large “servo bumps” that can have deleterious effects for certain applications. The prevailing approach to filtering this noise is to pass the laser through a high-finesse optical cavity, which places constraints on the system design. Here, we propose and demonstrate a different approach where a frequency error signal is derived from a beat note between the laser and the light that passes through the reference cavity. The phase noise derived from this beat note is fed forward to an electro-optic modulator after the laser, carefully accounting for relative delay, for real-time frequency correction. With a hertz-line-width laser, we show ≳20 dB noise suppression at the peak of the servo bump (approximately 250 kHz) and a noise-suppression bandwidth of approximately 5 MHz—well beyond the servo bump. By simulating the Rabi dynamics of a two-level atom with our measured data, we demonstrate substantial improvements to the pulse fidelity over a wide range of Rabi frequencies. Here, our approach offers a simple and versatile method for obtaining a clean spectrum of a narrow-line-width laser, as required in many emerging applications of cold atoms, and is readily compatible with commercial systems that may even include wavelength conversion.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Energy-efficient pathway for selectively exciting solute molecules to high vibrational states via solvent vibration-polariton pumping

Abstract Selectively exciting target molecules to high vibrational states is inefficient in the liquid phase, which restricts the use of IR pumping to catalyze ground-state chemical reactions. Here, we demonstrate that this inefficiency can sometimes be solved by confining the liquid to an optical cavity under vibrational strong coupling conditions. For a liquid solution of 13 CO 2 solute in a 12 CO 2 solvent, cavity molecular dynamics simulations show that exciting a polariton (hybrid light-matter state) of the solvent with an intense laser pulse, under suitable resonant conditions, may lead to a very strong (>3 quanta) and ultrafast (<1 ps) excitation of the solute, even though the solvent ends up being barely excited. By contrast, outside a cavity the same input pulse fluence can excite the solute by only half a vibrational quantum and the selectivity of excitation is low. Our finding is robust under different cavity volumes, which may lead to observable cavity enhancement on IR photochemical reactions in Fabry–Pérot cavities.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

Grayscale projection two-photon lithography using sub-diffraction motifs for ultrafast and precise nanoscale 3D printing

Rapid and high-fidelity nanoscale 3D printing is highly desirable, but it is difficult due to the tradeoff between speed and accuracy. Although optical projection techniques can massively scale up printing, fidelity is compromised due to the difficulty in precisely controlling the light dosage over the entire field. This challenge is typically addressed by using multiple projections, but it slows down printing. Here, we present grayscale projection two-photon lithography to overcome this tradeoff. Despite using a binary mask, it enables projecting more than 15,000 focal spots, each with independently tunable intensity. It advantageously leverages constraints imposed by optical diffraction to achieve grayscale tuning over the entire field at once. By directly tuning the focal spot intensities, we demonstrate suppression of proximity effects, compensation of non-uniform illumination, compensation of stitching artefacts, and rapid 3D printing with a single femtosecond pulse per layer. We demonstrate printing of nanowires as thin as 55 nm and achieve rates of 1.7 billion voxels/s and 215 mm 3 /hr.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Spin–orbit torque switching of a ferromagnet with picosecond electrical pulses

The development of approaches that can efficiently control the magnetization of magnetic materials is central to the creation of fast and low-power spintronic devices. Spin transfer torque can be used to electrically manipulate magnetic order in devices, but is typically limited to nanosecond timescales. Alternatively, spin–orbit torque can be employed, and switching with current pulses down to ~200 ps has been demonstrated. However, the upper limit to magnetization switching speed remains unestablished. Here, we show that photoconductive switches can be used to apply 6-ps-wide electrical pulses and deterministically switch the out-of-plane magnetization of a common thin cobalt film via spin–orbit torque. We probe the ultrafast magnetization dynamics due to spin–orbit torques with sub-picosecond resolution using the time-resolved magneto-optical Kerr effect (MOKE). We also estimate that the magnetization switching consumes less than 50 pJ in micrometre-sized devices.

42 ENGINEERING↗
DOE OSTI2025

Scanless laser waveform measurement in the near-infrared

Field-resolved measurements of few-cycle laser waveforms allow access to ultrafast electron dynamics in light–matter interactions and are key to future lightwave electronics. Recently, sub-cycle gating based on nonlinear excitation in active pixel sensors has allowed the first single-shot measurements of mid-infrared optical fields. Extending the techniques to shorter wavelengths, however, is not feasible using silicon-based detectors with bandgaps in the near-infrared. Here, we demonstrate an all-optical sampling technique for near-infrared laser fields, wherein an intense fundamental field generates a sub-cycle gate through nonlinear excitation of a wide-bandgap crystal, in this case, ZnO, which can sample the electric field of a weak perturbing pulse. By using a crossed-beam geometry, the temporal evolution of the perturbing field is mapped onto a transverse spatial axis of the nonlinear medium, and the waveform is captured in a single measurement of the spatially resolved fluorescence emission from the crystal. The technique is demonstrated through field-resolved measurements of the field reshaping during nonlinear propagation in the ZnO detection crystal.

Truong, Tran-Chau (ORCID:0000000348940635)↗
DOE OSTI2025

Enhancing the performance of solvent-borne poly(ethyl methacrylate) coatings for high-power laser applications via low-temperature drying

Organic polymers are a versatile class of materials employed in a broad range of optical coating applications. However, their use as coatings in high-power laser applications, particularly in the UV spectral region, has been limited in scope due to their relatively low laser-induced damage thresholds (LIDTs), which decrease further with exposure to multiple pulses. This study explores the effect of post-deposition drying temperature and residual solvent on the LIDT of solvent-borne polymer coatings. In this work, poly(ethyl methacrylate) (PEMA) coatings were deposited by first spin coating solutions of PEMA (dissolved in 2,2,2-trichloroethanol (TCE)) onto fused silica substrates, then baking at temperatures of either 130°C (soft-bake) or 180°C (hard-bake). Analysis of the two coatings revealed that the soft-bake coating retained a significant amount of TCE within the polymer matrix, which functioned to plasticize the coating and reduce internal stress. The laser-induced damage resistance of the two coatings was evaluated using 351-nm, 1-ns laser pulses. The testing protocols included single-pulse (1-on-1), 1-pulse ramp (R-on-1), and a 1000-pulse ramp (1000R-on-1) test. The results showed that the plasticized, soft-bake coating exhibits a significantly increased LIDT, especially for multipulse irradiation conditions.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Epitaxial growth and characterization of magnesium gallate (MgGa 2 O 4 ) thin films by pulsed laser deposition

To advance high power device application of MgGa 2 O 4 , it is imperative to achieve crystalline epitaxial thin films and to observe its materials’ characteristics within a wide range of growth conditions. However, there is no published work on the growth of this promising ultrawide bandgap material till this day. In this study, we report the crystalline growth of MgGa 2 O 4 thin films on c-plane (006) sapphire substrates using the pulsed laser deposition (PLD) technique in a broad range of temperature and oxygen pressure. The temperature range for this crystalline growth was within the temperature range of 300°C to 700°C and a pressure range of 1x10 -1 to 1x10 -3 Torr. Within this parameter range, the structural, chemical, optical, and surface property of MgGa 2 O 4 thin films have been investigated. Specifically, the acquired XRD patterns confirmed the film growth along the [111] preferential crystal orientation in the lattice. Here, the rocking curve measurement of the prominent (222) plane showed an increasing trend of the crystallinity with growth temperature and pressure. Furthermore, the XRD phi (φ) scan demonstrated the six-fold rotational symmetry of the MgGa 2 O 4 films and the epitaxial relationship of 30° between the film and the sapphire substrate. The XPS spectra confirmed the presence of +2 and +3 oxidation state for Mg and Ga respectively, in the films. The direct bandgap of MgGa 2 O 4 films was obtained ~5.27±0.03 eV by analyzing the UV-Vis absorbance spectra using the Tauc equation. The SEM images exhibited a granular surface morphology of the MgGa 2 O 4 films with an increasing trend in the grain size from low to high temperature and pressure. The refractive index and thickness of these films were in the range of ~1.90±0.02 and ~70±2.0 nm, respectively determined by fitting the spectroscopic ellipsometry data.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Elevated Electron Temperature Coincident with Observed Fusion Reactions in a Sheared-Flow-Stabilized Z Pinch

The sheared-flow-stabilized Z pinch concept has been studied extensively and is able to produce fusion-relevant plasma parameters along with neutron production over several microseconds. In this work, we present elevated electron temperature results spatially and temporally coincident with the plasma neutron source. An optical Thomson scattering apparatus designed for the FuZE device measures temperatures in the range of 1–3 keV on the axis of the device, 20 cm downstream of the nose cone. The 17-fiber system measures the radial profiles of the electron temperature. Scanning the laser time with respect to the neutron pulse time over a series of discharges allows the reconstruction of the T e temporal response, confirming that the electron temperature peaks simultaneously with the neutron output, as well as the pinch current and inductive voltage generated within the plasma. Comparison to spectroscopic ion temperature measurements suggests a plasma in thermal equilibrium. The elevated T e confirms the presence of a plasma assembled on axis, and indicates limited radiative losses, demonstrating a basis for scaling this device toward net gain fusion conditions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Uncovering extreme nonlinear dynamics in solids through time-domain field analysis

Time-domain analysis of harmonic fields with sub-cycle resolution is now experimentally viable due to the emergence of sensitive, on-chip techniques for petahertz-scale optical-field sampling. We demonstrate how such a time-domain, field-resolved analysis uncovers the extreme nonlinear electron dynamics responsible for high-harmonic generation within solids. Time-dependent density functional theory was used to simulate harmonic generation from a solid-state band-gap system driven by near- to mid-infrared waveforms. Particular attention was paid to regimes where both intraband and interband emission mechanisms play a critical role in shaping the nonlinear response. We show that a time-domain analysis of the harmonic radiation fields identifies the interplay between intra- and interband dynamical processes underlying the nonlinear light generation. With further analysis, we show that changes to the dominant emission regime can occur after only slight changes to the peak driving intensity and central driving wavelength. Furthermore, time-domain analysis of harmonic fields also reveals, for the first time, the possibility of rapid changes in the dominant emission mechanism within the temporal window of the driving pulse envelope. Finally, we examine the experimental viability of performing time-domain analysis of harmonic fields with sub-cycle resolution using realistic parameters.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

Bayesian optimization of laser wakefield acceleration via spectral pulse shaping

In this paper, we investigate the effect of spectral pulse shaping of the laser driver on the performance of channel-guided, laser–plasma accelerators. The study was carried out with the assistance of Bayesian optimization using particle-in-cell simulations. We used a realistic plasma profile based on a novel optical-field-ionized channel technique with ionization injection and low, on-axis plasma densities to maximize the energy gain of the electron bunch trailing the laser. Spectral shaping allows us to modify the temporal profile of the laser driver while keeping the laser energy constant, affecting the acceleration and injection processes. In addition, we consider how modifying the plasma channel parameters may affect the target outputs. Given the complexity and breadth of the parameter space in question, we used numerical optimization to identify high-performing configurations. In particular, we found laser profiles with additional spectral content that, when used with optimal plasma channel parameters, result in charge content an order of magnitude higher than the baseline Gaussian case while also increasing the mean energy of the electron bunch.

Physics - Plasma physics↗
DOE OSTI2022

Engineering infinite-range SU($\textit{n}$) interactions with spin-orbit-coupled fermions in an optical lattice

Here, we study multilevel fermions in an optical lattice described by the Hubbard model with on-site SU($\textit{n}$) -symmetric interactions. We show that in an appropriate parameter regime this system can be mapped onto a spin model with all-to-all SU($\textit{n}$)-symmetric couplings. Raman pulses that address internal spin states modify the atomic dispersion relation and induce spin-orbit coupling, which can act as a synthetic inhomogeneous magnetic field that competes with the SU($\textit{n}$) exchange interactions. We investigate the mean-field dynamical phase diagram of the resulting model as a function of $\textit{n}$ and different initial configurations that are accessible with Raman pulses. Consistent with previous studies for $\textit{n}$ = 2 , we find that for some initial states the spin model exhibits two distinct dynamical phases that obey simple scaling relations with $\textit{n}$. Moreover, for $\textit{n}$ > 2 we find that dynamical behavior can be highly sensitive to initial intraspin coherences. Our predictions are readily testable in current experiments with ultracold alkaline-earth-metal(-like) atoms.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Coherent band-edge oscillations and dynamic longitudinal-optical phonon mode splitting as evidence for polarons in perovskites

The coherence of collective modes, such as phonons and polarons, and their modulation of electronic states is long sought in complex systems, which is a crosscutting issue in photovoltaics and quantum electronics. In photovoltaic cells and lasers based on metal halide perovskites, the presence of polarons, i.e., photocarriers dressed by the macroscopic motion of charged lattice, assisted by terahertz (THz) longitudinal-optical (LO) phonons, has been intensely studied yet is still debated. This may be key for explaining the remarkable properties of the perovskite materials, e.g., defect tolerance, long charge lifetimes, and diffusion lengths. In this work we use the intense single-cycle THz pulse with peak electric field up to E THz = 1000 kV/cm to drive coherent polaronic band-edge oscillations at room temperature in CH 3 NH 3 PbI 3 (MAPbI 3 ). We reveal the oscillatory behavior is dominated by a specific quantized lattice vibration mode at $ω$ LO ~ 4 THz, which is both dipole and momentum forbidden. THz-driven coherent polaron dynamics exhibits distinguishing features: room temperature coherent oscillations at ω LO longer than 1 ps in both single crystals and thin films, mode-selective modulation of different band-edge states assisted by electron-phonon interaction, and dynamic mode splitting at low temperature due to entropy and anharmonicity of organic cations. Our results demonstrate intense THz-driven coherent band-edge modulation is a powerful probe of electron-lattice coupling phenomena and polaronic quantum control in perovskites.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Optically Addressable Light Valve Based on a GaN:Mn Photoconductor

Semi-insulating manganese-doped gallium nitride (GaN:Mn) layers epitaxially grown on unintentionally doped GaN substrates were used as photoconductors in optically addressable light valves (OALVs) to withstand higher operational laser fluences compared to current state-of-the-art OALVs where bismuth silicon oxide (BSO; Bi 12 SiO 20 ) layers are used as photoconductors. GaN:Mn promises to be an exciting material for optoelectronic operations due to its large laser fluence handling capability and photoresponsivity near the band edge. The laser damage thresholds for the semi-insulating epitaxial GaN:Mn layer and the n-type substrate layer were measured to be 2.4 and 4.2 J/cm 2 , respectively. These are 6–10 times higher than that of BSO (0.4 J/cm 2 ). These measurements were performed by exposing ~200 sites on the samples to increasing fluence levels from a Gaussian pulsed Nd:YAG laser system (1064 nm) operating at a 5 Hz repetition rate with a 3 ns pulse width. Photoresponsivity of the GaN:Mn material was investigated at discrete wavelengths of 447, 405, and 380 nm. Further, the peak photoresponsivity was observed under an illumination wavelength of 380 nm and is attributed to stronger absorption. The OALV was fabricated by attaching a 110-μm-thick GaN:Mn layer grown on a 280-μm-thick n-GaN layer to a 3-mm-thick BK7 optical window. A twisted nematic E7 liquid crystal was introduced to the 5 μm gap between the two components. Transmission levels of >90% were achieved for the fabricated OALVs for a peak voltage of 40 V, constrained by transmission “bleed-through”.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Discovery of enhanced lattice dynamics in a single-layered hybrid perovskite

Layered hybrid perovskites exhibit emergent physical properties and exceptional functional performances, but the coexistence of lattice order and structural disorder severely hinders our understanding of these materials. One unsolved problem regards how the lattice dynamics are affected by the dimensional engineering of the inorganic frameworks and their interaction with the molecular moieties. Here, we address this question by using a combination of spontaneous Raman scattering, terahertz spectroscopy, and molecular dynamics simulations. This approach reveals the structural dynamics in and out of equilibrium and provides unexpected observables that differentiate single- and double-layered perovskites. While no distinct vibrational coherence is observed in double-layered perovskites, an off-resonant terahertz pulse can drive a long-lived coherent phonon mode in the single-layered system. This difference highlights the dramatic change in the lattice environment as the dimension is reduced, and the findings pave the way for ultrafast structural engineering and high-speed optical modulators based on layered perovskites.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗