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Results for “X-ray stimulated Raman”

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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Resonant Stimulated X-ray Raman Spectroscopy of Mixed-Valence Manganese Complexes

Resonant stimulated X-ray Raman spectroscopy of the bimetallic [Mn III Mn IV (μ-O) 2 (μ-OAC)(tacn) 2 ] 2+ manganese complex is investigated in a simulation study. A pump–probe sequence of resonant X-ray Raman excitations is employed to generate and monitor valence-electron wave packets at selected regions in the molecule, by exploiting element specific core-excited states. A two-color protocol is presented, with pump and probe pulses tuned to the Mn and N K-edges. A natural orbital decomposition allows the visualization of the electron dynamics underlying the signal.

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

Attosecond impulsive stimulated X-ray Raman scattering in liquid water

We report the measurement of impulsive stimulated x-ray Raman scattering in neutral liquid water. An attosecond pulse drives the excitations of an electronic wavepacket in water molecules. The process comprises two steps: a transition to core-excited states near the oxygen atoms accompanied by transition to valence-excited states. Thus, the wavepacket is impulsively created at a specific atomic site within a few hundred attoseconds through a nonlinear interaction between the water and the x-ray pulse. We observe this nonlinear signature in an intensity-dependent Stokes Raman sideband at 526 eV. Our measurements are supported by our state-of-the-art calculations based on the polarization response of water dimers in bulk solvation and propagation of attosecond x-ray pulses at liquid density.

Science & Technology - Other Topics↗
DOE OSTI2025

Super-resolution stimulated X-ray Raman spectroscopy

Propagation of intense X-ray pulses through dense media has led to the observation of phenomena such as atomic X-ray lasing, self-induced transparency and stimulated X-ray Raman scattering (SXRS)4. SXRS has been long predicted as a means to launch and probe valence-electron wavepackets and as a building block for nonlinear X-ray spectroscopies. However, experimental observations of SXRS to date have not provided spectroscopic information, and theoretical modelling has largely implemented hard-to-realize phase-coherent attosecond pulses. Here we demonstrate SXRS with spectroscopic precision, that is, detection of valence-excited states in neon with a near Fourier-limited joint energy–time resolution of 0.1 eV–40 fs. We used a new covariance analysis between statistically spiky broadband incident X-ray and scattered X-ray Raman pulses. Using 18,000 single shots, we beat not only the incident (about 8 eV) bandwidth but also the approximately 0.2 eV instrumental energy resolution, thus creating super-resolution conditions, in analogy to super-resolved fluorescence microscopy. Our experimental results, supported by ab initio propagation simulations, reveal the competition between lasing in the ion and stimulated Raman scattering in the neutral. We demonstrate enhanced signal collection efficiency and a broad excitation window, surpassing spontaneous Raman efficiencies by orders of magnitude. This stochastic SXRS approach represents a first step towards tracking elementary events that determine chemical outcomes.

nonlinear x-ray spectroscopy↗
DOE OSTI2025

High gas-pressure apparatus for nonlinear X-ray propagation and reshaping via stimulated X-ray Raman scattering

Abstract We describe an experimental setup for non-linear interaction and propagation of ultrashort and intense x-ray free-electron laser (XFEL) pulses in a dense gas. It allows one to provide high, but adjustable, target-gas pressures of up to 6 bar within a vacuum environment of 3∙10 − 3 mbar or better. The setup enables investigation of intense x-ray propagation in an optically thick medium with minimal absorption loss of the unfocused beam outside of the target. As an application, we demonstrate the amplification of spectrally-resolved stimulated x-ray Raman scattering (SXRS) in dense neon gas, where the most intense inner part of the beam is almost completely absorbed. As a result, in the inner part of the beam, the SXRS signal exceeds the residual XFEL pulse by a factor of around two. In principle, this reshaping effect allows for a spatial separation of the two spectral components, i.e., the driving pulse and the SXRS signal.

Magunia, Alexander↗
DOE OSTI2021

Site-specific generation of excited state wavepackets with high-intensity attosecond x rays

High-intensity attosecond x rays can produce coherent superpositions of valence-excited states through two-photon Raman transitions. The broad-bandwidth, high-field nature of the pulses results in a multitude of accessible excited states. Multiconfigurational quantum chemistry with the time-dependent Schrödinger equation is used to examine population transfer dynamics in stimulated x-ray Raman scattering of the nitric oxide oxygen and nitrogen K-edges. Two pulse schemes initiate wavepackets of different characters and demonstrate how chemical differences between core-excitation pathways affect the dynamics. The population transfer to valence-excited states is found to be sensitive to the electronic structure and pulse conditions, highlighting complexities attributed to the Rabi frequency. The orthogonally polarized two- color-pulse setup has increased selectivity while facilitating longer, less intense pulses than the one-pulse setup. Population transfer in the 1s → Rydberg region is more effective but less selective at the nitrogen K-edge; the selectivity is reduced by double core-excited states. Result interpretation is aided by resonant inelastic x-ray scattering maps.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Conical Intersection Passages of Molecules Probed by X-ray Diffraction and Stimulated Raman Spectroscopy

Conical intersections (CoIns) play an important role in ultrafast relaxation channels. Their monitoring remains a formidable experimental challenge. We theoretically compare the probing of the S 2 → S 1 CoIn passage in 4-thiouracil by monitoring its vibronic coherences, using off-resonant X-ray-stimulated Raman spectroscopy (TRUECARS) and time resolved X-ray diffraction (TRXD). The quantum nuclear wavepacket (WP) dynamics provides an accurate picture of the photoinduced dynamics. Upon photoexcitation, the WP oscillates among the Franck–Condon point, the S2 minimum, and the CoIn with a 70 fs period. A vibronic coherence first emerges at 20 fs and can be observed until the S 2 state is fully depopulated. The distribution of the vibronic frequencies involved in the coherence is recorded by the TRUECARS spectrogram. Here, the TRXD signal provides spatial images of electron densities associated with the CoIn. In combination, the two signals provide a complementary picture of the nonadiabatic passage, which helps in the study of the underlying photophysics in thiobases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Photoisomerization transition state manipulation by entangled two-photon absorption

Significance Entangled two-photon absorption has attracted considerable interest due to its potential applications for low–photon flux spectroscopy and microscopy. The entanglement parameters in the twin-photon state can be exploited to control two-photon excitation processes. Here we demonstrate that photon entanglement provides a powerful novel control knob for the nuclear wave packets in an optically dark electronic state. We show that the transition states in the trans–cis photoisomerization of azobenzene, initiated by an entangled two-photon absorption process, can be manipulated significantly by entangled light. These effects can be monitored experimentally by coherent stimulated X-ray Raman signals which reveal electronic coherences during the passage through conical intersections.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Selective Enhancement of Spectroscopic Features by Quantum Optimal Control

Tailored light can be used to steer atomic motions into selected quantum pathways. In optimal control theory (OCT), the target is usually expressed in terms of the molecular wave function, a quantity that is not directly observable in experiment. In this study, we present simulations using OCT that optimize the spectroscopic signal itself. By shaping the optical pump, the x-ray stimulated Raman signal, which occurs solely during the passage through conical intersections, is temporally controlled and amplified by up to 2 orders of magnitude. This enhancement can be crucial in order to bring small coherence-based signatures above the detectable threshold. Our approach is applicable to any signal that depends on the expectation value of a positive definite operator.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Core-excited states of SF 6 probed with soft-x-ray femtosecond transient absorption of vibrational wave packets

A vibrational wavepacket in SF 6 is created by impulsive stimulated Raman scattering with a few-cycle infrared pulse and mapped simultaneously onto five sulfur core-excited states using table-top soft x-ray transient absorption spectroscopy between 170 to 200 eV. The femtosecond vibrations induce real-time energy shifts of the x-ray absorption, whose amplitude depend strongly on the nature of the core-excited state. The pump laser intensity is used to control the number of vibrational states in the superposition, thereby accessing core-excited levels for various extensions of the S-F stretching motion. This enables the determination of the relative core-level potential energy gradients for the symmetric stretching mode, in good agreement with TDDFT calculations. This experiment demonstrates a new means of characterizing core-excited potential energy curves.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Low mode implosion symmetry sensitivity in low gas-fill NIF cylindrical hohlraums

Achieving an efficient capsule implosion in National Ignition Facility indirect-drive target experiments requires symmetric hohlraum x-ray drive for the duration of the laser pulse. This is commonly achieved using two-sided two-cone laser irradiation of cylindrical hohlraums that, in principle, can zero the time average of all spherical harmonic asymmetry modes <6 as well as the time dependence of the usually dominant mode 2. In practice, experimental evidence indicates that maintaining symmetric drive becomes limited late in the pulse due to the inward expansion of the hohlraum wall and outward expansion of the capsule ablator plasmas impairing the propagation of the inner-cone laser beams. This effect is enhanced in hohlraums employing low gas-fill, now used almost exclusively as these provide the highest performing implosions and reduce Stimulated Brillouin and Raman backscatter losses, since the gas plasma provides less back pressure to limit blow-in of the hohlraum wall and capsule ablator plasmas. In order to understand this dynamic behavior, we combined multi-keV X-ray imaging of the wall and imploded fuel plasmas as we changed a single parameter at a time: hohlraum gas-fill, laser outer cone picket energy, radius of high density carbon capsules used, and laser beam polar and azimuthal pointing geometry. In this work, we developed a physics-based multi-parameter experimental scaling to explain the results that extend prior scalings and compare those to radiation hydrodynamic simulations to develop a more complete picture of how hohlraum, capsule, and laser parameters affect pole vs equator drive symmetry.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Element- and enantiomer-selective visualization of molecular motion in real-time

Ultrafast optical-domain spectroscopies allow to monitor in real time the motion of nuclei in molecules. Achieving element-selectivity had to await the advent of time resolved X-ray spectroscopy, which is now commonly carried at X-ray free electron lasers. However, detecting light element that are commonly encountered in organic molecules, remained elusive due to the need to work under vacuum. Here, we present an impulsive stimulated Raman scattering (ISRS) pump/carbon K-edge absorption probe investigation, which allowed observation of the low-frequency vibrational modes involving specific selected carbon atoms in the Ibuprofen RS dimer. Remarkably, by controlling the probe light polarization we can preferentially access the enantiomer of the dimer to which the carbon atoms belong.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Evolution and hot electron generation of laser–plasma instabilities in direct-drive inertial confinement fusion

A series of 2D in-plane plane wave particle-in-cell simulations find distinctive paths of laser-plasma instability evolution in OMEGA-scale implosions, depending on the initial electron temperature. At low temperatures, two-plasmon decay (TPD) dominates in both initial growth and the steady state. At high temperatures, the initial dominant modes switch to stimulated Raman scattering, but TPD still dominates a steady state characterized by cavitation and Langmuir turbulence. A hot electron scaling is also obtained from the simulations that, when combined with laser/plasma conditions from hydro simulations, can predict hot electron generation in implosions that do not employ smoothing-by-spectral-dispersion (SSD). It also shows that under the same laser/plasma conditions, SSD can reduce hot electron generation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2026

2D in-Plane Ordered MXene Nanosheets Derived from (Mo 2/3 Er 1/3 ) 2 AlC Rare-Earth i-MAX for Energy Storage Applications

MXenes have become one of the most versatile families of two-dimensional (2D) materials due to their high conductivity, hydrophilicity, and remarkable electrochemical performance. This has stimulated intense efforts to design and synthesize MXenes, including structurally unique in-plane ordered 2D MXenes called i-MXenes. Here, we have synthesized the quaternary rare earth (RE)-based i-MAX phase (Mo 2/3 Er 1/3 ) 2 AlC using an arc melting method, and the corresponding 2D i-MXene was then obtained through a LiF/HCl soft etching process. Literature studies have shown that Al and the RE element are etched out during the etching process, leading to the formation of pure vacancy-ordered Mo1.33C 2D i-MXene. However, our investigation reveals that upon exposure to a fluorine solution, the i-MAX phase forms RE fluoride impurities, which are challenging to remove through HCl−DI water washing and persist in the final product, resulting in impure Mo 1.33 C@Er i-MXene. These results were confirmed by various characterizations such as X-ray diffraction, Raman spectroscopy, X-ray photoelectron spectroscopy, and scanning transmission electron microscopy. Although the Mo 1.33 C@Er electrode showed a 24-fold increase in specific capacitance compared to its parent i-MAX phase, it still exhibited a high charge-transfer resistance arising from the insulating nature of RE fluoride byproducts, which adversely influence the overall capacitance behavior of the synthesized 2D Mo 1.33 C@Er i-MXenes. This study contributes to identifying pathways for the preparation of pure 2D i-MXenes from RE-based i-MAX phases and developing improved synthesis methods. With additional process optimization, the 2D i-MXene holds a strong potential for electrochemical energy storage applications. Additionally, the electronic structures of Mo 1.33 C were theoretically studied using first-principles density functional theory calculations, which revealed that pristine Mo 1.33 C is metallic, and this metallic nature is preserved even with −O, −F, and mixed functionalization.

chemical structure↗
DOE OSTI2023

Hot electron preheat in hydrodynamically scaled direct-drive inertial confinement fusion implosions on the NIF and OMEGA

Hot electron preheat has been quantified in warm, directly driven inertial confinement fusion implosions on OMEGA and the National Ignition Facility (NIF), to support hydrodynamic scaling studies. These CH-shell experiments were designed to be hydrodynamically equivalent, spanning a factor of 40 in laser energy and a factor of 3.4 in spatial and temporal scales, while preserving the incident laser intensity of 10 15 W/cm 2 . Experiments with similarly low levels of beam smoothing on OMEGA and NIF show a similar fraction (~0.2%) of laser energy deposited as hot electron preheat in the unablated shell on both OMEGA and NIF and similar preheat per mass (~2 kJ/mg), despite the NIF experiments generating a factor of three more hot electrons (~1.5% of laser energy) than on OMEGA (~0.5% of laser energy). This is plausibly explained by more absorption of hot electron energy in the ablated CH plasma on NIF due to larger areal density, as well as a smaller solid angle of the imploding shell as viewed from the hot electron generating region due to the hot electrons being produced at a larger standoff distance in lower-density regions by stimulated Raman scattering, in contrast to in higher-density regions by two-plasmon decay on OMEGA. Finally, the results indicate that for warm implosions at intensities of around 10 15 W/cm 2 , hydrodynamic equivalence is not violated by hot electron preheat, though for cryogenic implosions, the reduced attenuation of hot electrons in deuterium–tritium plasma will have to be considered.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗