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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 OSTI2025

Harnessing Ultra-Intense Long-Wave Infrared Lasers: New Frontiers in Fundamental and Applied Research

This review explores two main topics: the state-of-the-art and emerging capabilities of high-peak-power, ultrafast (picosecond and femtosecond) long-wave infrared (LWIR) laser technology based on CO2 gas laser amplifiers, and the current and advanced scientific applications of this laser class. The discussion is grounded in expertise gained at the Accelerator Test Facility (ATF) of Brookhaven National Laboratory (BNL), a leading center for ultrafast, high-power CO2 laser development and a National User Facility with a strong track record in high-intensity physics experiments. We begin by reviewing the status of 9–10 μm CO2 laser technology and its applications, before exploring potential breakthroughs, including the realization of 100 terawatt femtosecond pulses. These advancements will drive ongoing research in electron and ion acceleration in plasma, along with applications in secondary radiation sources and atmospheric energy transport. Throughout the review, we highlight how wavelength scaling of physical effects enhances the capabilities of ultra-intense lasers in the LWIR spectrum, expanding the frontiers of both fundamental and applied science.

43 PARTICLE ACCELERATORS↗
DOE OSTI2019

Adaptive control of laser-wakefield accelerators driven by mid-IR laser pulses

There has been growing interest both in studying high intensity ultrafast laser plasma interactions with adaptive control systems as well as using long wavelength driver beams. We demonstrate the coherent control of the dynamics of laser-wakefield acceleration driven by ultrashort (~ 100 fs) mid-infrared (~ 3.9 μ m) laser pulses. The critical density at this wavelength is 7.3 × 10 19 cm -3 , which is achievable with an ordinary gas target system. Interactions between mid-infrared laser pulses and such near-critical-density plasma may be beneficial due to much higher absorption of laser energy. In addition, the normalized vector potential of the laser field a 0 increases with longer laser wavelength, lowering the required peak laser intensity to drive non-linear laser-wakefield acceleration. Here, MeV level, collimated electron beams with non-thermal, peaked energy spectra are generated. Optimization of electron beam qualities are realized through adaptive control of the laser wavefront. A genetic algorithm controlling a deformable mirror improves the electron total charge, energy spectra, beam pointing and stability at various plasma density profiles. Particle-in-cell simulations reveal that the optimal wavefront causes an earlier injection on the density up-ramp and thus higher energy gain as well as less filamentation during the interaction, which leads to the improvement in electron beam collimation and energy spectra.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Burn parameters affect PAH emissions at conditions relevant for prescribed fires

Wildfire smoke is a health hazard as it contains carcinogenic volatile compounds and fine particulate matter. In particular, exposure to polycyclic aromatic hydrocarbons (PAHs) is a major concern, since these compounds have been recognized as important contributors to the overall carcinogenic risk. In this work, gas and particle-phase PAH emissions from combustion of Eastern White Pine (Pinus strobus) were quantified using time-of-flight mass spectrometry over a range of burn conditions representative of wildfires and prescribed fires, including fuel moisture, heat flux, and oxygen concentration. We found that changing the burn environment lead to a variability of up to 77% in phenanthrene/anthracene emissions. This could explain a large part of the variability in PAH emission factors from biomass combustion reported in the literature. Here, we found that optimal conditions for fuel moisture content of 20–30%, sample heat load of 60 - 70 kW m -2 , and oxygen concentrations of 5–15% can significantly reduce the emissions of heavy molar weight PAHs. Our analysis showed that the relative carcinogenic risk from PAH exposure can be reduced by more than 50% under optimal conditions. In light of the increasing use of prescribed fire for forest management, the relationship between emissions and burn conditions that we have established provides a guidance for assessing the expected health impact from prescription burns, and can inform strategies to reduce PAH emissions from prescribed fire activities.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗
DOE OSTI2024

High-throughput homogenization of a quasi-Gaussian ultrafast laser beam using a combined refractive beam shaper and spatial light modulator

Efficiently shaping femtosecond, transverse Gaussian laser beams to flat-top beams with flat wavefronts is critical for large-scale material processing and manufacturing. Existing beam shaping devices fall short either in final beam homogeneity or efficiency. Here, we present an approach that uses refractive optics to perform the majority of the beam shaping and then uses a fine-tune device (spatial light modulator) to refine the intensity profile. For the beam that we selected, circularly asymmetric with intensity fluctuations, our method achieved a uniformity of 0.055 within 90% of the beam area at 92% efficiency. The optimization involved an iterative beam shaping process that converged to optimum within 10 iterations.

43 PARTICLE ACCELERATORS↗
DOE OSTI2021

A light-induced phononic symmetry switch and giant dissipationless topological photocurrent in ZrTe 5

Dissipationless currents from topologically protected states are promising for disorder-tolerant electronics and quantum computation. In this work, we photogenerate giant anisotropic terahertz nonlinear currents with vanishing scattering, driven by laser-induced coherent phonons of broken inversion symmetry in a centrosymmetric Dirac material ZrTe 5 . Our work suggests that this phononic terahertz symmetry switching leads to formation of Weyl points, whose chirality manifests in a transverse, helicity-dependent current, orthogonal to the dynamical inversion symmetry breaking axis, via circular photogalvanic effect. The temperature-dependent topological photocurrent exhibits several distinct features: Berry curvature dominance, particle–hole reversal near conical points and chirality protection that is responsible for an exceptional ballistic transport length of ~10 μm. These results, together with first-principles modelling, indicate two pairs of Weyl points dynamically created by B 1u phonons of broken inversion symmetry. Such phononic terahertz control breaks ground for coherent manipulation of Weyl nodes and robust quantum transport without application of static electric or magnetic fields.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Strong ionisation in carbon nanowires

Surfaces covered with nanostructures, such as nanowire arrays, are shown to facilitate a significantly higher absorption of laser energy as compared to flat surfaces. Due to the efficient coupling of the laser energy, highly energetic electrons are produced, which in turn can emit intense ultrafast X-ray pulses. Full three dimensional PIC simulations are used to analyse the behaviour of arrays of carbon nanowires 400 nm in diameter, irradiated by a 400-nm laser pulse of 60-fs duration at FWHM and a vector potential of α{sub 0} = 18. We analyse the ionisation dynamics of the nanowires. The difference of the ionisation strength and structure between linearly and circularly polarised laser beam is investigated. The nanowires are found to be fully ionised after about 30 laser cycles. Circularly polarised light reveals a slightly stronger ionisation effect. (extreme laser radiation: physics and fundamental applications)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2018

Effect of modified periodic waveforms on current-induced spin polarization measurements

Applying a voltage to a semiconductor sample generates a current-induced electron spin polarization (CISP). Using an ultrafast mode-locked laser and lock-in detection scheme, we measure CISP on an indium gallium arsenide epilayer via Faraday rotation and extract the spin generation rate. While the measured spin polarization initially increases linearly with electric field as observed in previous work, larger applied voltages lead to a decreasing spin generation rate. Here we show that we can recover the linear dependence of spin generation rate with electric field even at larger applied voltages by modifying the applied voltage waveform to reduce heating and multiplying by an appropriate correction factor. Future CISP studies can utilize this technique to investigate CISP under larger applied electric fields.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2018

A terahertz pump mega-electron-volt ultrafast electron diffraction probe apparatus at the SLAC Accelerator Structure Test Area facility

Here, we describe a new experimental setup capable of measuring structural dynamics following intense terahertz excitation. This system, developed at the SLAC Accelerator Structure Test Area facility, uses a high-energy ultrafast laser to produce intense terahertz pulses and femtosecond electron bunches that are accelerated to mega-electron-volt kinetic energies. The focused terahertz pulses have electric fields in excess of 600 kV/cm, and the resulting structural dynamics can be followed by electron diffraction. We also present some examples demonstrating its implementation where interactions between the THz pulses and the electron bunch are used to characterize the spatial and temporal characteristics of the THz field.

42 ENGINEERING↗
DOE OSTI2018

Evolution of plasma wakes in density up- and down-ramps

The time evolution of plasma wakes in density up- and down-ramps is examined through theory and particle-in-cell simulations. Motivated by observation of the reversal of a linear plasma wake in a plasma density upramp in a recent experiment we have examined the behaviour of wakes in plasma ramps that always accompany any plasma source used for plasma-based acceleration. In the up-ramp case it is found that, after the passage of the drive pulse, the wavnumber/wavelength of the wake starts to decrease/increase with time until it eventually tends to zero/infinity, then the wake reverses its propagation direction and the wavenunber/wavelength of the wake begins to increase/shrink. Here, the evolutions of the wavenumber and the phase velocity of the wake as functions of time are shown to be significantly different in the up-ramp and the down-ramp cases. In the latter case the wavenumber of the wake at a particular position in the ramp increases until the wake is eventually damped. It is also shown that the waveform of the wake at a particular time after being excited can be precisely controlled by tuning the initial plasma density profile, which may enable a new type of plasma-based ultrafast optics.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2018

Imaging electron-density fluctuations by multidimensional X-ray photon-coincidence diffraction

The ultrafast spontaneous electron-density fluctuation dynamics in molecules is studied theoretically by off-resonant multiple X-ray diffraction events. The time- and wavevector-resolved photon-coincidence signals give an image of electron-density fluctuations expressed through the four-point correlation function of the charge density in momentum space. A Fourier transform of the signal provides a real-space image of the multipoint charge-density correlation functions, which reveal snapshots of the evolving electron density in between the diffraction events. The proposed technique is illustrated by ab initio simulations of the momentum- and real-space inelastic scattering signals from a linear cyanotetracetylene molecule.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2016

Identification of the dominant photochemical pathways and mechanistic insights to the ultrafast ligand exchange of Fe(CO) 5 to Fe(CO) 4 EtOH

We utilized femtosecond time-resolved resonant inelastic X-ray scattering and ab initio theory to study the transient electronic structure and the photoinduced molecular dynamics of a model metal carbonyl photocatalyst Fe(CO) 5 in ethanol solution. We propose mechanistic explanation for the parallel ultrafast intra-molecular spin crossover and ligation of the Fe(CO) 4 which are observed following a charge transfer photoexcitation of Fe(CO) 5 as reported in our previous study [Wernet et al., Nature 520, 78 (2015)]. We find that branching of the reaction pathway likely happens in the 1 A 1 state of Fe(CO) 4 . A sub-picosecond time constant of the spin crossover from 1 B 2 to 3 B 2 is rationalized by the proposed 1 B 2 → 1 A 1 → 3 B 2 mechanism. Ultrafast ligation of the 1 B 2 Fe(CO) 4 state is significantly faster than the spin-forbidden and diffusion limited ligation process occurring from the 3 B 2 Fe(CO) 4 ground state that has been observed in the previous studies. We propose that the ultrafast ligation occurs via 1 B 2 → 1 A 1 → 1 A' Fe(CO) 4 EtOH pathway and the time scale of the 1 A 1 Fe(CO) 4 state ligation is governed by the solute-solvent collision frequency. In conclusion, our study emphasizes the importance of understanding the interaction of molecular excited states with the surrounding environment to explain the relaxation pathways of photoexcited metal carbonyls in solution.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Single-Molecule Interfacial Electron Transfer

This project is focused on the use of single-molecule high spatial and temporal resolved techniques to study molecular dynamics in condensed phase and at interfaces, especially, the complex reaction dynamics associated with electron and energy transfer rate processes. The complexity and inhomogeneity of the interfacial ET dynamics often present a major challenge for a molecular level comprehension of the intrinsically complex systems, which calls for both higher spatial and temporal resolutions at ultimate single-molecule and single-particle sensitivities. Combined single-molecule spectroscopy and electrochemical atomic force microscopy approaches are unique for heterogeneous and complex interfacial electron transfer systems because the static and dynamic inhomogeneities can be identified and characterized by studying one molecule at a specific nanoscale surface site at a time. The goal of our project is to integrate and apply these spectroscopic imaging and topographic scanning techniques to measure the energy flow and electron flow between molecules and substrate surfaces as a function of surface site geometry and molecular structure. We have been primarily focusing on studying interfacial electron transfer under ambient condition and electrolyte solution involving both single crystal and colloidal TiO 2 and related substrates. The resulting molecular level understanding of the fundamental interfacial electron transfer processes will be important for developing efficient light harvesting systems and broadly applicable to problems in fundamental chemistry and physics. We have made significant advancement on deciphering the underlying mechanism of the complex and inhomogeneous interfacial electron transfer dynamics in dyesensitized TiO 2 nanoparticle systems that strongly involves with and regulated by molecule-surface interactions. We have studied interfacial electron transfer on TiO 2 nanoparticle surfaces by using ultrafast single-molecule spectroscopy and electrochemical AFM metal tip scanning microscopy, focusing on understanding the interfacial electron transfer dynamics at specific nanoscale electron transfer sites with high-spatially and temporally resolved topographic-and-spectroscopic characterization at individual molecule basis, characterizing single-molecule rate processes, reaction driving force, and molecule-substrate electronic coupling. One of the most significant characteristics of our new approach is that we are able to interrogate the complex interfacial electron transfer dynamics by actively pin-point energetic manipulation of the surface interaction and electronic couplings, beyond the conventional excitation and observation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

X-Ray Sum Frequency Diffraction for Direct Imaging of Ultrafast Electron Dynamics

X-ray diffraction from molecules in the ground state produces an image of their charge density, and time-resolved x-ray diffraction can thus monitor the motion of the nuclei. However, the density change of excited valence electrons upon optical excitation can barely be monitored with regular diffraction techniques due to the overwhelming background contribution of the core electrons. We present a nonlinear x-ray technique made possible by novel free electron laser sources, which provides a spatial electron density image of valence electron excitations. The technique, sum frequency generation carried out with a visible pump and a broadband x-ray diffraction pulse, yields snapshots of the transition charge densities, which represent the electron density variations upon optical excitation. The technique is illustrated by ab initio simulations of transition charge density imaging for the optically induced electronic dynamics in a donor or acceptor substituted stilbene.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

First High-Gradient Results of UED/UEM SRF Gun at Cryogenic Temperatures

Benefiting from the rapid progress on RF photogun technologies in the past two decades, the development of MeV range ultrafast electron diffraction/microscopy (UED and UEM) has been identified as an enabling instrumentation. UEM or UED use low power electron beams with modest energies of a few MeV to study ultrafast phenomena in a variety of novel and exotic materials. SRF photoguns become a promising candidate to produce highly stable electrons for UEM/UED applications because of the ultrahigh shot-to-shot stability compared to room temperature RF photoguns. SRF technology was prohibitively expensive for industrial use until two recent advancements: Nb₃Sn and conduction cooling. The use of Nb₃Sn allows to operate SRF cavities at higher temperatures (4K) with low power dissipation which is within the reach of commercially available closed-cycle cryocoolers. Euclid is developing a continuous wave (CW), 1.5-cell, MeV-scale SRF conduction cooled photogun operating at 1.3 GHz. In this paper, we present first high gradient results of the gun conducted in liquid helium.

43 PARTICLE ACCELERATORS↗
DOE OSTI2023

Measurement of femtosecond dynamics of ultrafast electron beams through terahertz compression and time-stamping

Visualizing ultrafast dynamics at the atomic scale requires time-resolved characterization with femtosecond temporal resolution. For fully relativistic electron bunch probes, existing techniques for single-shot ultrafast electron diffraction (UED) are limited by the achievable electron probe bunch length, charge, and timing jitter. We present the first experimental demonstration of dual-fed THz-driven compression and time-stamping that enables electron probes with improved temporal resolution. This technique utilizes two counter-propagating quasi-single-cycle THz pulses generated from two OH-1 organic crystals coupled into an optimized THz compressor structure. We demonstrate electron bunch compression and time-of-arrival jitter suppression by a factor of 3 paving the way toward unique opportunities for UED time-resolved measurements.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2019

Imaging the Renner–Teller effect using laser-induced electron diffraction

Structural information on electronically excited neutral molecules can be indirectly retrieved, largely through pump–probe and rotational spectroscopy measurements with the aid of calculations. Here, we demonstrate the direct structural retrieval of neutral carbonyl disulfide (CS 2 ) in the B ~ 1 B 2 excited electronic state using laser-induced electron diffraction (LIED). We unambiguously identify the ultrafast symmetric stretching and bending of the field-dressed neutral CS 2 molecule with combined picometer and attosecond resolution using intrapulse pump–probe excitation and measurement. We invoke the Renner–Teller effect to populate the B ~ 1 B 2 excited state in neutral CS 2 , leading to bending and stretching of the molecule. Our results demonstrate the sensitivity of LIED in retrieving the geometric structure of CS 2 , which is known to appear as a two-center scatterer.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Characterizing particle-like charge-migration dynamics with high-order harmonic sideband spectroscopy

Here, we introduce high-order harmonic sideband spectroscopy and show that it can be a robust probe of charge migration (CM) in a halogenated carbon-chain molecule. We simulate both the CM and high-order harmonic generation (HHG) dynamics using ab initio time-dependent density-functional theory. We find that CM dynamics initiated along the molecular backbone induces sidebands in the HHG spectrum driven by a delayed laser pulse that is polarized perpendicular to the molecular axis. Monitoring the spectrum as either the HHG laser frequency or the relative delay is scanned allows for the extraction of detailed information about the time-domain characteristics of the CM process.

74 ATOMIC AND MOLECULAR PHYSICS↗