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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 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Sub-threshold ultrafast one-photon photoemission from a Cu(111) photocathode

Single-photon photoemission of electrons for incident photon energies below the surface work function is reported for a single-crystal Cu(111) photocathode. Spectral characterization of the quantum efficiency and mean transverse energy of the emitted electrons is shown to be consistent with emission from a thermalized hot electron distribution photoexcited on sub-picosecond time scales into an upper conduction band at the L-point of the Brillouin zone of copper. To our knowledge, this is the first time that such excited-state thermionic emission has been observed from a planar metal photocathode, and then from a commonly used photocathode material. The results, therefore, indicate the potential importance of such band structure dependent sub-threshold photoemission mechanisms on the performance of photocathodes employed for the generation of short electron pulses using sub-picosecond laser pulses. Consequently, the combined experimental and theoretical work presented in this paper contributes to solid-state photocathode-based research aimed at our understanding and selection (or discovery) of high brightness photo-electron sources required for many electron-based diffraction, imaging, and accelerator applications.

43 PARTICLE ACCELERATORS↗
DOE OSTI2022

Low Repetition-Rate, High-Resolution Femtosecond Transmission Electron Microscopy

Spatial and energy resolutions of state-of-the-art transmission electron microscopes (TEMs) have surpassed 50 pm and 5 meV. However, with respect to the time domain, even the fastest detectors combined with the brightest sources may only be able to reach the microsecond timescale. Thus, conventional methods are incapable of resolving myriad fundamental ultrafast (i.e., attosecond to picosecond) atomic-scale dynamics. The successful demonstration of femtosecond (fs) laser-based (LB) ultrafast transmission electron microscopy (UEM) nearly 20 years ago provided a means to span this nearly 10-order-of-magnitude temporal gap. While nanometer-picosecond UEM studies of dynamics are now well established, ultrafast Å-scale imaging has gone largely unrealized. Further, while instrument development has rightly been an emphasis, and while new modalities and uses of pulsed-beam TEM continue to emerge, the overall chemical and materials application space has been only modestly explored to date. In this Perspectives article, we argue that these apparent shortfalls can be attributed to a simple lack of data and detail. We speculate that present work and continued growth of the field will ultimately lead to the realization that Å-scale fs dynamics can indeed be imaged with minimally modified UEM instrumentation and with repetition rates (f rep ) below - and perhaps even well below - 1 MHz. We further argue that use of low f rep , whether for LB UEM or for chopped/bunched beams, significantly expands the accessible application space. Furthermore, this calls for systematically establishing modality-specific limits so that especially promising technologies can be pursued, thus ultimately facilitating broader adoption as individual instrument capabilities expand.

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

Ultrafast time-resolved 2D imaging of laser-driven fast electron transport in solid density matter using an x-ray free electron laser

High-power, short-pulse laser-driven fast electrons can rapidly heat and ionize a high-density target before it hydrodynamically expands. The transport of such electrons within a solid target has been studied using two-dimensional (2D) imaging of electron-induced Kα radiation. However, it is currently limited to no or picosecond scale temporal resolutions. Here, we demonstrate femtosecond time-resolved 2D imaging of fast electron transport in a solid copper foil using the SACLA x-ray free electron laser (XFEL). An unfocused collimated x-ray beam produced transmission images with sub-micron and ~10 fs resolutions. The XFEL beam, tuned to its photon energy slightly above the Cu K-edge, enabled 2D imaging of transmission changes induced by electron isochoric heating. Time-resolved measurements obtained by varying the time delay between the x-ray probe and the optical laser show that the signature of the electron-heated region expands at ~25% of the speed of light in a picosecond duration. Time-integrated Cu Kα images support the electron energy and propagation distance observed with the transmission imaging. The x-ray near-edge transmission imaging with a tunable XFEL beam could be broadly applicable for imaging isochorically heated targets by laser-driven relativistic electrons, energetic protons, or an intense x-ray beam.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Prediction of photodynamics of 200 nm excited cyclobutanone with linear response electronic structure and ab initio multiple spawning

Simulations of photochemical reaction dynamics have been a challenge to the theoretical chemistry community for some time. In an effort to determine the predictive character of current approaches, we predict the results of an upcoming ultrafast diffraction experiment on the photodynamics of cyclobutanone after excitation to the lowest lying Rydberg state (S 2 ). A picosecond of nonadiabatic dynamics is described with ab initio multiple spawning. Herein we use both time dependent density functional theory (TDDFT) and equation-of-motion coupled cluster singles and doubles (EOM-CCSD) theory for the underlying electronic structure theory. We find that the lifetime of the S 2 state is more than a picosecond (with both TDDFT and EOM-CCSD). The predicted ultrafast electron diffraction spectrum exhibits numerous structural features, but weak time dependence over the course of the simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Thermal Weibel instability induced magnetic fields co-exist with linear wakes in laser-ionized plasmas

When a moderately intense, few-picosecond-long laser pulse ionizes gas to produce an underdense plasma column, a linear relativistic plasma wave or wake can be excited by the self-modulation instability that may prove useful for multi-bunch acceleration of externally injected electrons or positrons to high energies in a short distance. At the same time, due to the anisotropic temperature distributions of the ionized plasma electrons, the Weibel instability can self-generate magnetic fields throughout such a plasma on a few picoseconds timescale that can persist even longer than the lifetime of the wake. In the present paper, we first show using simulations that both these effects do indeed co-exist in space and time in the plasma. Using our simulations, we make preliminary estimates of the contribution to the transverse emittance growth of an externally injected beam due to the Weibel magnetic fields in a few-millimeter-long plasma. We then present the results of an experiment that has allowed us to measure the spatiotemporal evolution of the magnetic fields using an ultrashort relativistic electron probe beam. Both the topology and the lifetime of the Weibel instability induced magnetic fields in the experiment are in reasonable agreement with the fields induced by the Weibel instability in the simulations.

43 PARTICLE ACCELERATORS↗
DOE OSTI2026

Fit-free optical determination of electronic thermalization time in nematic iron-based superconductors

We present a nematic response function model (NRFM) for fit-free direct extraction of the characteristic time of ultrafast electronic thermalization in iron-based superconductors, materials with electronic nematicity. By combining the NRFM for polarization-dependent pump–probe measurements of electronic nematic response with the two-temperature model (TTM) for sub-picosecond quasiparticle relaxation, we quantify the electronic thermalization timescales and their anisotropy. The nematic response function is modeled as the difference in normalized reflectivity signals, revealing a pronounced sub-picosecond extremum in signal evolution that directly yields the characteristic electronic thermalization time. This method demonstrates that the NRFM is consistent with TTM fits of transient optical response, yielding electronic thermalization time constants on the order of 110–230 fs for the FeSe 1−x Te x and Ba(Fe 0.92 Co 0.08 ) 2 As 2 thin films. Here, the proposed approach can be applied to any material that exhibits electronic nematicity, providing a powerful tool for direct mapping of the relaxation time in nematic materials, avoiding complex experimental data-fitting procedures.

Bartenev, Alexander [University of Puerto Rico, Ma↗
DOE OSTI2022

Mapping the self-generated magnetic fields due to thermal Weibel instability

The origin of the seed magnetic field that is amplified by the galactic dynamo is an open question in plasma astrophysics. Aside from primordial sources and the Biermann battery mechanism, plasma instabilities have also been proposed as a possible source of seed magnetic fields. Among them, thermal Weibel instability driven by temperature anisotropy has attracted broad interests due to its ubiquity in both laboratory and astrophysical plasmas. However, this instability has been challenging to measure in a stationary terrestrial plasma because of the difficulty in preparing such a velocity distribution. Here, we use picosecond laser ionization of hydrogen gas to initialize such an electron distribution function. We record the 2D evolution of the magnetic field associated with the Weibel instability by imaging the deflections of a relativistic electron beam with a picosecond temporal duration and show that the measured k -resolved growth rates of the instability validate kinetic theory. Concurrently, self-organization of microscopic plasma currents is observed to amplify the current modulation magnitude that converts up to ~1% of the plasma thermal energy into magnetic energy, thus supporting the notion that the magnetic field induced by the Weibel instability may be able to provide a seed for the galactic dynamo.

42 ENGINEERING↗
DOE OSTI2023

Real-time imaging of acoustic waves in bulk materials with X-ray microscopy

The dynamics of lattice vibrations govern many material processes, such as acoustic wave propagation, displacive phase transitions, and ballistic thermal transport. The maximum velocity of these processes and their effects is determined by the speed of sound, which therefore defines the temporal resolution (picoseconds) needed to resolve these phenomena on their characteristic length scales (nanometers). Here, we present an X-ray microscope capable of imaging acoustic waves with subpicosecond resolution within mm-sized crystals. We directly visualize the generation, propagation, branching, and energy dissipation of longitudinal and transverse acoustic waves in diamond, demonstrating how mechanical energy thermalizes from picosecond to microsecond timescales. Bulk characterization techniques capable of resolving this level of structural detail have previously been available on millisecond time scales—orders of magnitude too slow to capture these fundamental phenomena in solid-state physics and geoscience. As such, the reported results provide broad insights into the interaction of acoustic waves with the structure of materials, and the availability of ultrafast time-resolved dark-field X-ray microscopy opens a vista of new opportunities for 3D imaging of materials dynamics on their intrinsic submicrosecond time scales.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Measurements of the Growth and Saturation of Electron Weibel Instability in Optical-Field Ionized Plasmas

The temporal evolution of the magnetic field associated with electron thermal Weibel instability in optical-field ionized plasmas is measured using ultrashort (1.8 ps), relativistic (45 MeV) electron bunches from a linear accelerator. The self-generated magnetic fields are found to self-organize into a quasistatic structure consistent with a helicoid topology within a few picoseconds and such a structure lasts for tens of picoseconds in underdense plasmas. Here, the measured growth rate agrees well with that predicted by the kinetic theory of plasmas taking into account collisions. Magnetic trapping is identified as the dominant saturation mechanism.

Electric & magnetic plasma measurements↗
DOE OSTI2021

Ultrafast Adsorbate Excitation Probed with Subpicosecond-Resolution X-Ray Absorption Spectroscopy

We use a pump-probe scheme to measure the time evolution of the C K-edge x-ray absorption spectrum from CO/Ru(0001) after excitation by an ultrashort high-intensity optical laser pulse. Because of the short duration of the x-ray probe pulse and precise control of the pulse delay, the excitation-induced dynamics during the first picosecond after the pump can be resolved with unprecedented time resolution. By comparing with density functional theory spectrum calculations, we find high excitation of the internal stretch and frustrated rotation modes occurring within 200 fs of laser excitation, as well as thermalization of the system in the picosecond regime. The ~100 fs initial excitation of these CO vibrational modes is not readily rationalized by traditional theories of nonadiabatic coupling of adsorbates to metal surfaces, e.g., electronic frictions based on first order electron-phonon coupling or transient population of adsorbate resonances. Finally, we suggest that coupling of the adsorbate to nonthermalized electron-hole pairs is responsible for the ultrafast initial excitation of the modes.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Ultrafast measurements of the interfacial spin Seebeck effect in Au and rare-earth iron-garnet bilayers

We investigate picosecond spin-currents across Au/iron-garnet interfaces in response to ultrafast laser heating of the electrons in the Au film. In the picoseconds after optical heating, interfacial spin currents occur due to an interfacial temperature difference between electrons in the metal and magnons in the insulator. We report measurements of this interfacial longitudinal spin Seebeck effect between Au and rare-earth iron-garnet insulators, i.e. RE 3 Fe 5 O 12 , where RE is Y, Eu, Tb, Tm. By systematically varying the rare-earth element, we modify the total magnetic moment of the iron-garnet. We use time domain thermoreflectance (TDTR) measurements to characterize the thermal response of the bilayer to ultrafast optical heating. We use time-resolved magneto-optic Kerr effect (TR-MOKE) measurements of the Au layer to measure the time-evolution of spin accumulation in the Au film. Replacing Y with other rare-earths enhances the electron-magnon conductance G e-m at the Au iron-garnet interface by as much as a factor of three. The electron-magnon conductance does not follow the trend of either the total magnetization of the iron garnet or the magnetic moment of the rare-earth.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Pulsed laser induced atomic layer etching of silicon

Here, we demonstrate the laser mediated atomic layer etching (ALEt) of silicon. Using a nanosecond pulsed 266 nm laser focused loosely over and in a parallel configuration to the surface of the silicon, we dissociate Cl 2 gas to induce chlorination. Then, we use pulsed picosecond irradiation to remove the chlorinated layer. Subsequently, we perform continuous wave (CW) laser annealing to eliminate amorphization caused by the picosecond laser etching. Based on atomic force microscopy (AFM) and X-ray photoelectron spectroscopy (XPS), we observed strong evidence of chlorination and digital etching at 0.85 nm etching per cycle with good uniformity.

42 ENGINEERING↗
DOE OSTI2024

Squeezed Light Stimulated Raman Scattering (SRS) Microscopy for Bioenergy Applications

Stimulated Raman scattering (SRS) microscopy using picosecond near-IR pulses have provided a great penetration depth with reduced fluorescence interference when imaging biological samples for bioenergy applications. These tools have provided insight into 1) tracking the degradation of chemical composites in biomass feedstocks to investigate the recalcitrant factors during the deconstruction processes, 2) monitoring the production of chemicals in photosynthetic plants and wood-digesting microorganisms, and 3) probing plant-bacteria interactions. However, the above processes are usually slow and require continuous imaging for an extended period. This is challenging for classic SRS because the laser power needed to achieve enough sensitivity causes photodamage in the samples during such long experiments. Quantum-squeezed light with reduced noise in the intensity quadrature can improve the sensitivity of classic SRS microscopy beyond the shot noise limit. The successful squeezing of one of the picosecond pulses in the above SRS will improve sensitivity and reduce photodamage, greatly expanding the range of studies available to SRS microscopy.

BIOMASS FUELS↗
DOE OSTI2020

Direct visualization of electromagnetic wave dynamics by laser-free ultrafast electron microscopy

Integrating femtosecond lasers with electron microscopies has enabled direct imaging of transient structures and morphologies of materials in real time and space. Here, we report the development of a laser-free ultrafast electron microscopy (UEM) offering the same capability but without requiring femtosecond lasers and intricate instrumental modifications. We create picosecond electron pulses for probing dynamic events by chopping a continuous beam with a radio frequency (RF)–driven pulser with the pulse repetition rate tunable from 100 MHz to 12 GHz. As a first application, we studied gigahertz electromagnetic wave propagation dynamics in an interdigitated comb structure. We reveal, on nanometer space and picosecond time scales, the transient oscillating electromagnetic field around the tines of the combs with time-resolved polarization, amplitude, and local field enhancement. This study demonstrates the feasibility of laser-free UEM in real-space visualization of dynamics for many research fields, especially the electrodynamics in devices associated with information processing technology.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Direct observation of strong momentum-dependent electron-phonon coupling in a metal

Phonon scattering in metals is one of the most fundamental processes in materials science. However, understanding such processes has remained challenging and requires detailed information on interactions between phonons and electrons. We use an ultrafast electron diffuse scattering technique to resolve the nonequilibrium phonon dynamics in femtosecond–laser-excited tungsten in both time and momentum. We determine transient populations of phonon modes which show strong momentum dependence initiated by electron-phonon coupling. For phonons near Brillouin zone border, we observe a transient rise in their population on a timescale of approximately 1 picosecond driven by the strong electron-phonon coupling, followed by a slow decay on a timescale of approximately 8 picosecond governed by the weaker phonon-phonon relaxation process. We find that the exceptional harmonicity of tungsten is needed for isolating the two processes, resulting in long-lived nonequilibrium phonons in a pure metal. Our finding highlights that electron-phonon scattering can be the determinant factor in the phonon thermal transport of metals.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Intermolecular vibrational energy transfer enabled by microcavity strong light–matter coupling

Selective vibrational energy transfer between molecules in the liquid phase, a difficult process hampered by weak intermolecular forces, is achieved through polaritons formed by strong coupling between cavity photon modes and donor and acceptor molecules. Using pump-probe and two-dimensional infrared spectroscopy, we found that the excitation of the upper polariton, which is composed mostly of donors, can efficiently relax to the acceptors within ~5 picoseconds. The energy-transfer efficiency can be further enhanced by increasing the cavity lifetime, suggesting that the energy transfer is a polaritonic process. This vibrational energy-transfer pathway opens doors for applications in remote chemistry, sensing mechanisms, and vibrational polariton condensation.

Science & Technology - Other Topics↗
DOE OSTI2025

Plasma Assisted Combustion and Chemical Processing: Chapter 9 - Plasma Diagnostics

Plasma dynamics and chemistry have a broad range of timescales from picoseconds to milliseconds. In addition, it involves nonequilibrium energy transfer between electrons, ions, electronically and vibrationally excited states, radicals, intermediate species, and reactants and products as well as surface charges and chemistry. To understand plasma physics and chemistry, it is essential to conduct time and space resolved, quantitative detection of nonequilibrium temperature distributions, electron energy and number density, electric field, and species concentrations. There are enormous publications and review articles on this subject. The focus of this chapter is to be placed on the most recent progress in gas phase plasma properties and chemistry, especially on optical emission spectroscopy, laser absorption spectroscopy, Faraday rotational spectroscopy, Raman and Thompson scattering, femtosecond and picosecond (fs/ps) coherent anti-Stokes Raman scattering (CARS) spectroscopy, and electric field-induced second harmonic generation methods.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Ultrafast carrier dynamics in terahertz photoconductors and photomixers: beyond short-carrier-lifetime semiconductors

Abstract Efficient terahertz generation and detection are a key prerequisite for high performance terahertz systems. Major advancements in realizing efficient terahertz emitters and detectors were enabled through photonics-driven semiconductor devices, thanks to the extremely wide bandwidth available at optical frequencies. Through the efficient generation and ultrafast transport of charge carriers within a photo-absorbing semiconductor material, terahertz frequency components are created from the mixing products of the optical frequency components that drive the terahertz device – a process usually referred to as photomixing. The created terahertz frequency components, which are in the physical form of oscillating carrier concentrations, can feed a terahertz antenna and get radiated in case of a terahertz emitter, or mix with an incoming terahertz wave to down-convert to DC or to a low frequency photocurrent in case of a terahertz detector. Realizing terahertz photoconductors typically relies on short-carrier-lifetime semiconductors as the photo-absorbing material, where photocarriers are quickly trapped within one picosecond or less after generation, leading to ultrafast carrier dynamics that facilitates high-frequency device operation. However, while enabling broadband operation, a sub-picosecond lifetime of the photocarriers results in a substantial loss of photoconductive gain and optical responsivity. In addition, growth of short-carrier-lifetime semiconductors in many cases relies on the use of rare elements and non-standard processes with limited accessibility. Therefore, there is a strong motivation to explore and develop alternative techniques for realizing terahertz photomixers that do not rely on these defect-introduced short-carrier-lifetime semiconductors. This review will provide an overview of several promising approaches to realize terahertz emitters and detectors without short-carrier-lifetime semiconductors. These novel approaches utilize p-i-n diode junctions, plasmonic nanostructures, ultrafast spintronics, and low-dimensional materials to offer ultrafast carrier response. These innovative directions have great potentials for extending the applicability and accessibility of the terahertz spectrum for a wide range of applications.

36 MATERIALS SCIENCE↗