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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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465 records · Page 26
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Imaging the dynamics of initial laser-driven shocks and blowoff plasmas in polystyrene under laser-direct-drive fusion conditions

The dynamics of laser-driven shock propagation in solid ablator material, along with the concomitant processes of shinethrough and blowoff plasma plume expansion, at conditions relevant to laser-direct-drive fusion are measured using a tabletop system capable of supporting rapid dataset development with significantly higher resolution compared to existing methods. The experimental results are directly compared with current radiation-hydrodynamic simulations using the two-dimensional code . Discrepancies between experiments and simulations are evidenced and attributed to limitation of simulation to account for important processes involved in the solid-to-plasma transition. Published by the American Physical Society 2024

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Direct Observation of Enhanced Electron-Phonon Coupling in Copper Nanoparticles in the Warm-Dense Matter Regime

Warm-dense matter (WDM) is a highly-excited state that lies at the confluence of solids, plasmas, and liquids and that cannot be described by equilibrium theories. The transient nature of this state when created in a laboratory, as well as the difficulties in probing the strongly-coupled interactions between the electrons and the ions, make it challenging to develop a complete understanding of matter in this regime. Here in this work, by exciting isolated ~8 nm nanoparticles with a femtosecond laser below the ablation threshold, we create uniformly-excited WDM. We then use photoelectron spectroscopy to track the instantaneous electron temperature and directly extract the strongest electron-ion coupling observed experimentally to date. By directly comparing with state-of-the-art theories, we confirm that the superheated nanoparticles lie at the boundary between hot solids and plasmas, with associated strong electron-ion coupling. This is evidenced both by the fast energy loss of electrons to ions, as well as a strong modulation of the electron temperature by acoustic oscillations in the nanoparticle. This work demonstrates a new route for experimental exploration and theoretical validation of the exotic properties of WDM.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Role of dipole-forbidden autoionizing resonances in nonresonant one-color two-photon single ionization of N 2

We present an experimental and theoretical energy- and angle-resolved study on the photoionization dynamics of non-resonant one-color two-photon single valence ionization of neutral N$_2$ molecules. Using 9.3 eV photons produced via high harmonic generation and a 3-D momentum imaging spectrometer, we detect the photoelectrons and ions produced from one-color two-photon ionization in coincidence. Photoionization of N$_2$ populates the X $^2\Sigma^+_g$, A $^2\Pi_u$, and B $^2\Sigma^+_u$ ionic states of N$_2^+$, where the photoelectron angular distributions associated with the X $^2\Sigma^+_g$ and A $^2\Pi_u$ states both vary with changes in photoelectron kinetic energy of only a few hundred meV. We attribute the rapid evolution in the photoelectron angular distributions to the excitation and decay of dipole-forbidden autoionizing resonances that belong to series of different symmetries, all of which are members of the Hopfield series, and compete with the direct two-photon single ionization.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Coherence in Chemistry: Foundations and Frontiers

Coherence refers to correlations in waves. Because matter has a wave-particle nature, it is unsurprising that coherence has deep connections with the most contemporary issues in chemistry research (e.g., energy harvesting, femtosecond spectroscopy, molecular qubits and more). But what does the word "coherence" really mean in the context of molecules and other quantum systems? We provide a review of key concepts, definitions, and methodologies, surrounding coherence phenomena in chemistry, and we describe how the terms "coherence" and "quantum coherence" refer to many different phenomena in chemistry. Moreover, we show how these notions are related to the concept of an interference pattern. Coherence phenomena are indeed complex, and ambiguous definitions may spawn confusion. By describing the many definitions and contexts for coherence in the molecular sciences, we aim to enhance understanding and communication in this broad and active area of chemistry.

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

Transient absorption measurements of excitonic dynamics in 3 R -MoS 2

The excitonic dynamics in MoS 2 monolayer, bilayer, and bulk flakes with different stacking orders, namely 3R and 2H, are investigated through transient absorption spectroscopy at room temperature. Samples are obtained by the mechanical exfoliation of bulk MoS 2 crystals with 3R and 2H stacking orders. Photoluminescence spectroscopy is performed to characterize and compare the samples. Time-resolved differential reflection measurements reveal that monolayer flakes exfoliated from the 3R and 2H crystals exhibit similar exciton lifetimes of a few picoseconds. However, the exciton lifetime in the 3R bilayer flake is approximately 85 ps, about twice as long as that in the 2H bilayer. This prolonged exciton lifetime is attributed to the reduction of the electron-hole wavefunction overlap in the 3R bilayer due to the built-in polarization. Similarly, in bulk 3R MoS 2 , the exciton lifetime is around 220 ps, approximately twice as long as those in bulk 2H MoS 2 . The extension of the exciton lifetime in 3R transition metal dichalcogenides could be advantageous for their applications in optoelectronic devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Ferricyanide photo-aquation pathway revealed by combined femtosecond Kβ main line and valence-to-core x-ray emission spectroscopy

Reliably identifying short-lived chemical reaction intermediates is crucial to elucidate reaction mechanisms but becomes particularly challenging when multiple transient species occur simultaneously. Here, we report a femtosecond x-ray emission spectroscopy and scattering study of the aqueous ferricyanide photochemistry, utilizing the combined Fe Kβ main and valence-to-core emission lines. Following UV-excitation, we observe a ligand-to-metal charge transfer excited state that decays within 0.5 ps. On this timescale, we also detect a hitherto unobserved short-lived species that we assign to a ferric penta-coordinate intermediate of the photo-aquation reaction. We provide evidence that bond photolysis occurs from reactive metal-centered excited states that are populated through relaxation of the charge transfer excited state. Beyond illuminating the elusive ferricyanide photochemistry, these results show how current limitations of Kβ main line analysis in assigning ultrafast reaction intermediates can be circumvented by simultaneously using the valence-to-core spectral range.

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

Ultrafast nonlinear absorption of TMDC quantum dots

Here, we study theoretically absorption properties of MoS 2 quantum dots placed in an ultrashort and strong optical pulse with the duration of a few femtoseconds and the amplitude up to 1.5 V/Å. While the monolayer of MoS 2 has a bandgap of ≈ 1.8 eV, the quantum dots of MoS 2 have in-gap edge states, which open additional absorption channels. The absorbance of the system strongly depends on the amplitude of the pulse. At small amplitude, less than 0.5 V/Å, the absorbance varies by more than 20% with the frequency of the pulse. The system shows saturable absorption if the frequency of the pulse is larger than the bulk bandgap and reverse saturable absorption if the frequency of the pulse is in the bandgap. At large amplitudes, > 0.5 V/Å, of the pulse, the ultrafast absorbance of a quantum dot has a weak dependence on the pulse frequency. If the frequency of the pulse is less than the corresponding bulk bandgap, the absorbance has a nonmonotonic dependence on the pulse amplitude with the maximum at ≈ 0.5 V/Å. We also present the results for QDs of different TMDC materials, which show that at large field amplitude, > 0.5 V/Å, the absorbance is universal and has weak dependence on the type of TMDC.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Direct structural retrieval from gas-phase ultrafast diffraction data using a genetic algorithm

Ultrafast scattering techniques such as ultrafast electron diffraction and ultrafast x-ray diffraction have been utilized to elucidate the structural dynamics, reaction intermediates, and final products in molecular reactions following photoexcitation. The time-dependent structures are typically not directly retrieved from the experimental data, but they rely on comparison with calculations. The genetic algorithm (GA), a global optimization strategy, can be used to retrieve the molecular structures directly from diffraction patterns without any theoretical input. However, the robustness of the GA with respect to real experimental conditions such as a limited momentum transfer range, noise, and artifacts has not been studied in detail. In this work, we characterize the performance of the GA with simulated data that mimic realistic experimental conditions. We have developed and implemented a variant of the GA specific to diffraction measurements which performs better in the presence of imperfect data compared to the standard implementation of the GA. We demonstrate this method with both synthetic data and experimental ultrafast electron diffraction data on the UV-induced photodissociation of trifluoroiodomethane (C⁢F 3⁡ I) molecules.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Hard x-ray – optical four-wave mixing using a split-and-delay line

New, hard x-ray free electron lasers (FEL) produce intense femtosecond-to-attosecond pulses at angstrom wavelengths, giving access to the fundamental spatial and temporal scales of matter. These revolutionary light sources open the door to applying the suite of nonlinear, optical spectroscopy methods at hard x-ray photon energies. Nonlinear spectroscopy with hard x-rays can allow for measuring the coherence properties of short wavelength excitations with atomic specificity and for understanding how high energy excitations couple to other degrees of freedom in atomic, molecular or condensed-phase systems. As a step in this direction, here we present hard x-ray, optical four-wave mixing (4WM) measurements done at 9.8 keV at the split-and-delay line at the x-ray correlation spectroscopy (XCS) hutch of the Linac Coherent Light Source (LCLS). In this work, we create an x-ray transient grating (TG) from a pair of crossing x-ray beams and diffract optical laser pulses at 400 nm from the TG. The key technical advance here is being able to independently vary the delays of the x-ray pulses. Measurements were made in 3 different solid samples: bismuth germinate (BGO), zinc oxide (ZnO) and yttrium aluminum garnet (YAG). The resulting phase-matched, 4WM signal is measured in two different ways: by varying the x-ray, x-ray pulse delay which can reveal both material and light source coherence properties and also by varying the optical laser delay with respect to the x-ray TG to study how the x-ray excitation couples to the optical properties. Although no coherent 4WM signal was seen in these measurements, the absence of this signal gives important information on experimental requirements for detecting this in future work. Also, our laser-delay scans, although not a new measurement, were applied to different materials than in past work and reveal new examples x-ray induced lattice dynamics in solids. This work represents a key step towards extending nonlinear optics and time-resolved spectroscopy into the hard x-ray regime.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Observation of polarization density waves in SrTiO 3

The nature of the incipient ferroelectric transition in SrTiO 3 has been a long-standing puzzle in condensed matter physics. One explanation involves the competition between ferroelectricity and an instability characterized by the mesoscopic modulation of the polarization. These polarization density waves, which should intensify near the quantum critical point, break local inversion symmetry and are difficult to characterize with conventional X-ray scattering methods. Here, in this study, we probe inversion symmetry breaking at finite momenta and visualize the instability of the polarization at the nanometre scale in SrTiO3 by combining a femtosecond X-ray free-electron laser with terahertz coherent control methods. We found polar-acoustic collective modes that are soft, particularly at the tens of nanometre scale. These precursor collective excitations provide evidence for the conjectured mesoscopic-modulated phase in SrTiO 3 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Simultaneous imaging of vibrational, rotational, and electronic wave-packet dynamics in a triatomic molecule

Light-induced molecular dynamics often involve the excitation of several electronic, vibrational, and rotational states. Since the ensuing electronic and nuclear motion determines the pathways and outcomes of photoinduced reactions, our ability to monitor and understand these dynamics is crucial for molecular physics, physical chemistry, and photobiology. However, characterizing this complex motion represents a significant challenge when different degrees of freedom are strongly coupled. In this Letter, we demonstrate how the interplay between vibrational, rotational, and electronic degrees of freedom governs the evolution of molecular wave packets in the low-lying states of strong-field-ionized sulfur dioxide. Using time-resolved Coulomb explosion imaging (CEI) and quantum mechanical wave packet simulations, we directly map the bending vibrations of the molecule, show how the vibrational wave packet is influenced by molecular alignment, and elucidate the consequences of nuclear motion for the coupling between the two lowest electronic states of the cation. Furthermore, our results demonstrate that multicoincident CEI can be an efficient experimental tool for characterizing coupled electronic and nuclear motion in polyatomic molecules.

Atomic & molecular processes in external fields↗
DOE OSTI2022

UV-induced dissociation of CH 2 BrI probed by intense femtosecond XUV pulses

The ultraviolet (UV)-induced dissociation and photofragmentation of gas-phase CH 2 BrI molecules induced by intense femtosecond extreme ultraviolet (XUV) pulses at three different photon energies are studied by multi-mass ion imaging. Using a UV-pump–XUV-probe scheme, charge transfer between highly charged iodine ions and neutral CH 2 Br radicals produced by C–I bond cleavage is investigated. In earlier charge-transfer studies, the center of mass of the molecules was located along the axis of the bond cleaved by the pump pulse. In the present case of CH 2 BrI, this is not the case, thus inducing a rotation of the fragment. We discuss the influence of the rotation on the charge transfer process using a classical over-the-barrier model. Our modeling suggests that, despite the fact that the dissociation is slower due to the rotational excitation, the critical interatomic distance for charge transfer is reached faster. Furthermore, we suggest that charge transfer during molecular fragmentation may be modulated in a complex way.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Temperature Measurements in Hypersonic Wind Tunnels via Femtosecond Coherent Anti-Stokes Raman Scattering

A femtosecond coherent anti-Stokes Raman scattering (fs CARS) instrument is developed to perform gas-phase thermometry in cold-flow hypersonic wind tunnels. Measurements are reported for Mach 8 and 14 pure-nitrogen flows. The fs CARS instrument includes a 100 fs pump/Stokes pulse and a spectrally narrow probe pulse from a second harmonic bandwidth compressor. Important experimental considerations such as limits on the pump/Stokes pulse energy are discussed. The fs CARS focusing and collimating optics are mounted on a two-axis translation stage system to scan the measurement location during a 30 second wind tunnel run. Single-laser-shot rotational CARS spectra are recorded at the laser repetition rate of 1 kHz in the wind tunnel freestream and near simple cone models. Spectral fitting is used to determine quantitative gas temperatures. Freestream temperatures at Mach 8 and 14 spanned ranges of 40–75 and 35–50 K, respectively, depending on tunnel operating conditions. Temperature variations across the central 100 mm span of the wind tunnel were quantified. Measured temperature jumps across conical bow shocks from various models varied by less than 1% from predicted values. Hypersonic boundary layer measurements were demonstrated. In conclusion, these measurements illustrate the utility and robustness of this instrument for the study of complex fluid flow phenomena in challenging ground test facilities.

Aerodynamics↗
DOE OSTI2025

Experimental Generation of Extreme Electron Beams for Advanced Accelerator Applications

In this Letter, we report on the experimental generation of high energy (10 GeV), ultrashort (femtosecond-duration), ultrahigh current (∼ 0.1 MA), petawatt peak power electron beams in a particle accelerator. These extreme beams enable the exploration of a new frontier of high-intensity beam-light and beam-matter interactions broadly relevant across fields ranging from laboratory astrophysics to strong field quantum electrodynamics and ultrafast quantum chemistry. We demonstrate our ability to generate and control the properties of these electron beams by means of a laser-electron beam shaping technique. In conclusion, this experimental demonstration opens the door to on-the-fly customization of extreme beam current profiles for desired experiments and is poised to benefit a broad swath of cross-cutting applications of relativistic electron beams.

43 PARTICLE ACCELERATORS↗
DOE OSTI2026

Structural Mechanism of an Efficacy Photoswitch Targeting the β 2 ‐adrenergic Receptor

The field of photopharmacology develops light-responsive drugs that can modulate protein activity, enabling precise and dynamic investigations of their roles in health and disease. Adrenergic receptors are prominent targets for this approach because they are prototypical G protein-coupled receptors with high clinical relevance in bronchial and cardiovascular diseases. Here, we employed the azobenzene-based compound photoazolol-1 in combination with time-resolved serial crystallography at X-ray free-electron lasers to resolve the molecular mechanisms by which photoswitchable β-blockers modulate activity of the β 2 -adrenoceptor (β 2 AR). Time-resolved structures of the receptor bound to trans-photoazolol-1 (pre-photoconversion), a strained intermediate in the nanosecond range, and the fully photoisomerized cis-photoazolol-1 reveal how isomerization of the azobenzene moiety induces distinct conformational changes within the orthosteric ligand binding pocket. Within seconds, light-excited photoazolol-1 adopts a new binding pose, altering interactions with extracellular loop 2 and shifting the positions of transmembrane helices 5, 6, and 7. Functional assays of β 2 AR in cellular membranes show that photoazolol-1 acts as an efficacy photoswitch, changing from an inverse agonist to a neutral antagonist upon isomerization without leaving the binding pocket. In combination, these findings suggest a molecular mechanism for activity modulation via efficacy photoswitches and provide a framework for designing ligands that exploit light-driven transitions within the binding pocket to achieve spatiotemporal control of receptor function.

G protein-coupled receptors↗