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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 217 records · Page 12
All sourcesNASA NTRSDOE OSTI
NASA NTRS2005

CARS Temperature and Species Measurements For Air Vehicle Propulsion Systems

The coherent anti-Stokes Raman spectroscopy (CARS) method has recently been used in the United States and Europe to probe several different types of propulsion systems for air vehicles. At NASA Langley Research Center in the United States, CARS has been used to simultaneously measure temperature and the mole fractions of N2, O2 and H2 in a supersonic combustor, representative of a scramjet engine. At Wright- Patterson Air Force Base in the United States, CARS has been used to simultaneously measure temperature and mole fractions of N2, O2 and CO2, in the exhaust stream of a liquid-fueled, gas-turbine combustor. At ONERA in France and the DLR in Germany researchers have used CARS to measure temperature and species concentrations in cryogenic LOX-H2 rocket combustion chambers. The primary aim of these measurements has been to provide detailed flowfield information for computational fluid dynamics (CFD) code validation.

Danehy, Paul M.↗
NASA NTRS2010

Advancements in Dual-Pump Broadband CARS for Supersonic Combustion Measurements

Space- and time-resolved measurements of temperature and species mole fractions of nitrogen, oxygen, and hydrogen were obtained with a dual-pump coherent anti-Stokes Raman spectroscopy (CARS) system in hydrogen-fueled supersonic combustion free jet flows. These measurements were taken to provide time-resolved fluid properties of turbulent supersonic combustion for use in the creation and verification of computational fluid dynamic (CFD) models. CFD models of turbulent supersonic combustion flow currently facilitate the design of air-breathing supersonic combustion ramjet (scramjet) engines. Measurements were made in supersonic axi-symmetric free jets of two scales. First, the measurement system was tested in a laboratory environment using a laboratory-scale burner (approx.10 mm at nozzle exit). The flow structures of the laboratory-burner were too small to be resolved with the CARS measurements volume, but the composition and temperature of the jet allowed the performance of the system to be evaluated. Subsequently, the system was tested in a burner that was approximately 6 times larger, whose length scales are better resolved by the CARS measurement volume. During both these measurements, weaknesses of the CARS system, such as sensitivity to vibrations and beam steering and inability to measure temperature or species concentrations in hydrogen fuel injection regions were indentified. Solutions were then implemented in improved CARS systems. One of these improved systems is a dual-pump broadband CARS technique called, Width Increased Dual-pump Enhanced CARS (WIDECARS). The two lowest rotational energy levels of hydrogen detectable by WIDECARS are H2 S(3) and H2 S(4). The detection of these lines gives the system the capability to measure temperature and species concentrations in regions of the flow containing pure hydrogen fuel at room temperature. WIDECARS is also designed for measurements of all the major species (except water) in supersonic combustion flows fueled with hydrogen and hydrogen/ethylene mixtures (N2, O2, H2, C2H4, CO, and CO2). This instrument can characterize supersonic combustion fueled with surrogate fuel mixtures of hydrogen and ethylene. This information can lead to a better understanding of the chemistry and performance of supersonic combustion fueled with cracked jet propulsion (JP)-type fuel.

Tedder, Sarah Augusta Umberger↗
NASA NTRS2012

Large-Eddy / Reynolds-Averaged Navier-Stokes Simulations of a Dual-Mode Scramjet Combustor

Numerical simulations of reacting and non-reacting flows within a scramjet combustor configuration experimentally mapped at the University of Virginia s Scramjet Combustion Facility (operating with Configuration A ) are described in this paper. Reynolds-Averaged Navier-Stokes (RANS) and hybrid Large Eddy Simulation / Reynolds-Averaged Navier-Stokes (LES / RANS) methods are utilized, with the intent of comparing essentially blind predictions with results from non-intrusive flow-field measurement methods including coherent anti-Stokes Raman spectroscopy (CARS), hydroxyl radical planar laser-induced fluorescence (OH-PLIF), stereoscopic particle image velocimetry (SPIV), wavelength modulation spectroscopy (WMS), and focusing Schlieren. NC State's REACTMB solver was used both for RANS and LES / RANS, along with a 9-species, 19- reaction H2-air kinetics mechanism by Jachimowski. Inviscid fluxes were evaluated using Edwards LDFSS flux-splitting scheme, and the Menter BSL turbulence model was utilized in both full-domain RANS simulations and as the unsteady RANS portion of the LES / RANS closure. Simulations were executed and compared with experiment at two equivalence ratios, PHI = 0.17 and PHI = 0.34. Results show that the PHI = 0.17 flame is hotter near the injector while the PHI = 0.34 flame is displaced further downstream in the combustor, though it is still anchored to the injector. Reactant mixing was predicted to be much better at the lower equivalence ratio. The LES / RANS model appears to predict lower overall heat release compared to RANS (at least for PHI = 0.17), and its capability to capture the direct effects of larger turbulent eddies leads to much better predictions of reactant mixing and combustion in the flame stabilization region downstream of the fuel injector. Numerical results from the LES/RANS model also show very good agreement with OH-PLIF and SPIV measurements. An un-damped long-wave oscillation of the pre-combustion shock train, which caused convergence problems in some RANS simulations, was also captured in LES / RANS simulations, which were able to accommodate its effects accurately.

Fulton, Jesse A.↗
NASA NTRS2012

Dual-Pump CARS Development and Application to Supersonic Combustion

A dual-pump Coherent Anti-Stokes Raman Spectroscopy (CARS) instrument has been developed to obtain simultaneous measurements of temperature and absolute mole fractions of N2, O2 and H2 in supersonic combustion and generate databases for validation and development of CFD codes. Issues that compromised previous attempts, such as beam steering and high irradiance perturbation effects, have been alleviated or avoided. Improvements in instrument precision and accuracy have been achieved. An axis-symmetric supersonic combusting coaxial jet facility has been developed to provide a simple, yet suitable flow to CFD modelers. Approximately one million dual-pump CARS single shots have been collected in the supersonic jet for varying values of flight and exit Mach numbers at several locations. Data have been acquired with a H2 co-flow (combustion case) or a N2 co-flow (mixing case). Results are presented and the effects of the compressibility and of the heat release are discussed.

Magnotti, Gaetano↗
NASA NTRS2016

OH PLIF Visualization of a Premixed Ethylene-fueled Dual-Mode Scramjet Combustor

Hydroxyl radical (OH) planar induced laser fluorescence (PLIF) measurements have been performed in a small-scale scramjet combustor at the University of Virginia Aerospace Research Laboratory at nominal simulated Mach 5 enthalpy. OH lines were carefully chosen to have fluorescent signal that is independent of pressure and temperature but linear with mole fraction. The OH PLIF signal was imaged in planes orthogonal to and parallel to the freestream flow at different equivalence ratios. Flameout limits were tested and identified. Instantaneous planar images were recorded and analyzed to compare the results with width increased dual-pump enhanced coherent anti-Stokes Raman spectroscopy (WIDECARS) measurements in the same facility and large eddy simulation/Reynolds average Navier-Stokes (LES/RANS) numerical simulation. The flame angle was found to be approximately 10 degrees for several different conditions, which is in agreement with numerical predictions and measurements using WIDECARS. Finally, a comparison between NO PLIF non-combustion cases and OH PLIF combustion cases is provided: the comparison reveals that the dominant effect of flame propagation is freestream turbulence rather than heat release and concentration gradients.

Cantu, Luca M. L.↗
DOE OSTI2025

Tracing Long-Lived Atomic Coherences Generated via Molecular Conical Intersections

Accessing coherences is key to fully understand and control ultrafast dynamics of complex quantum systems like molecules. Most photochemical processes are mediated by conical intersections, which generate coherences between electronic states in molecules. We show with accurate calculations performed on gas-phase methyl iodide that electronic coherences of spin-orbit-split states persist in atomic iodine after dissociation. Our simulation predicts a maximum magnitude of vibronic coherence in the molecular regime of 0.75% of the initially photoexcited state population. Upon dissociation, one-third of this coherence magnitude is transferred to a long-lived atomic coherence where vibrational decoherence can no longer occur. To trace these dynamics, we propose a tabletop experimental approach—heterodyned attosecond four-wave-mixing spectroscopy. This technique can temporally resolve small electronic coherence magnitudes and reconstruct the full complex coherence function via phase cycling. Hence, heterodyned attosecond four-wave-mixing spectroscopy leads the way to a complete understanding and optimal control of spin-orbit-coupled electronic states in photochemistry.

Chemical Physics↗
DOE OSTI2025

Distinct Optical Excitation Mechanisms of a Coherent Magnon in a van der Waals Antiferromagnet

The control of antiferromagnets with ultrashort optical pulses has emerged as a prominent field of research. Tailored laser excitation can launch coherent spin waves at terahertz frequencies, yet a comprehensive description of their generation mechanisms is still lacking despite extensive efforts. Using terahertz emission spectroscopy, we investigate the generation of a coherent magnon mode in the van der Waals antiferromagnet NiPS 3 under a range of photoexcitation conditions. By tuning the pump photon energy from transparency to resonant with a 𝑑−𝑑 transition, we reveal a striking change in the coherent magnon’s dependence on the pump polarization, indicating two distinct excitation mechanisms. Furthermore, our findings provide a strategy for the manipulation of magnetic modes via photoexcitation around subgap electronic states.

Light-induced magnetic effects↗
DOE OSTI2024

The role of the dopant in the electronic structure of erbium-doped TiO 2 for quantum emitters

Erbium-doped TiO 2 materials are promising candidates for advancing quantum technologies, necessitating a thorough understanding of their electronic and crystal structures to tailor their properties and enhance coherence times. This study explored epitaxial erbium-doped rutile TiO 2 films deposited on r-sapphire substrates using molecular beam epitaxy. Photoluminescence excitation spectroscopy demonstrated decreasing photoluminescence lifetimes with erbium doping, indicating limited optical coherence times. Lattice distortions associated with Er 3+ were probed by x-ray absorption spectroscopy, indicating that erbium primarily occupies Ti 4+ sites and influences oxygen vacancies. Significant lattice distortions in the higher-order shells and apparent full coordination around erbium suggest that additional defects are likely prevalent in these regions. These findings indicate that defects contribute to limited coherence times by introducing alternative decay pathways, leading to shorter photoluminescence lifetimes.

Crystallographic defects↗
DOE OSTI2022

Ultrafast branching in intersystem crossing dynamics revealed by coherent vibrational wavepacket motions in a bimetallic Pt($\mathrm{II}$) complex

Ultrafast excited-state processes of transition metal complexes (TMCs) are governed by complicated interplays between electronic and nuclear dynamics, which demand a detailed understanding to achieve optimal functionalities of photoactive TMC-based materials for many applications. Here, in this work, we investigated a cyclometalated platinum(II) dimer known to undergo a Pt-Pt bond contraction in metal-metal-to-ligand-charge-transfer (MMLCT) excited state using femtosecond broadband transient absorption (fs-BBTA) spectroscopy in combination with geometry optimization and normal mode calculations. Using sub-20 fs pump and broadband probe pulses in fs-BBTA spectroscopy, we are able to correlate coherent vibrational wavepacket (CVWP) evolution with stimulated emission (SE) dynamics of the 1 MMLCT state. The results demonstrated that the 145 cm -1 CVWP motions with the damping times of ~ 0.9 ps and ~ 2 ps originate from coherent Pt-Pt stretching vibrations in the singlet and triplet MMLCT states, respectively. On the basis of excited-state potential energy surface calculations in our previous work, we rationalized that the CVWP transfer from Franck-Condon (FC) state to the 3 MMLCT state was mediated by a triplet ligand-centered ( 3 LC) intermediate state through two step intersystem crossing (ISC) on a time scale shorter than a period of the Pt-Pt stretching wavepacket motions. Moreover, it was found that the CVWP motion with 110 cm-1 frequency decays with the damping time of ~ 0.2 ps, well matching the time constant of 0.253 ps corresponding to a redshift in the SE feature at early time. This observation indicates that the Pt-Pt bond contraction changes the stretching frequency from 110 to 145 cm -1 and stabilize the 1 MMLCT state relative to the 3 LC state with the ~ 0.2 ps time scale. Thus, the ultrafast ISC from the 1 MMLCT to the 3 LC states occurs before the Pt-Pt bond shortening. The findings herein provide insight into understanding the impact of Pt-Pt bond contraction on ultrafast branching of the 1 MMLCT population into the direct ( 1 MMLCT → 3 MMLCT) and indirect ISC pathways ( 1 MMLCT → 3 LC → 3 MMLCT) in the Pt(II) dimer. These results revealed intricate excited state electronic and nuclear motions that could steer the reaction pathways with levels of details that have not achieved before

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

Coherent diffractive imaging with twisted X-rays: Principles, applications, and outlook

Recent technological breakthroughs in synchrotron and x-ray free electron laser facilities have revolutionized nanoscale structural and dynamic analyses in condensed matter systems. This review provides a comprehensive overview of the advancements in coherent scattering and diffractive imaging techniques, which are now at the forefront of exploring materials science complexities. These techniques, notably Bragg coherent diffractive imaging and x-ray photon correlation spectroscopy, x-ray magnetic dichroism, and x-ray correlation analysis leverage beam coherence to achieve volumetric three-dimensional imaging at unprecedented sub-nanometer resolutions and explore dynamic phenomena within sub-millisecond timeframes. Such capabilities are critical in understanding and developing advanced materials and technologies. Simultaneously, the emergence of chiral crystals—characterized by their unique absence of standard inversion, mirror, or other roto-inversion symmetries—presents both challenges and opportunities. These materials exhibit distinctive interactions with light, leading to phenomena such as molecular optical activity, chiral photonic waveguides, and valley-specific light emissions, which are pivotal in the burgeoning fields of photonic and spintronic devices. This review elucidates how novel x-ray probes can be leveraged to unravel these properties and their implications for future technological applications. A significant focus of this review is the exploration of new avenues in research, particularly the shift from conventional methods to more innovative approaches in studying these chiral materials. Inspired by structured optical beams, the potential of coherent scattering techniques utilizing twisted x-ray beams is examined. This promising direction not only offers higher spatial resolution but also opens the door to previously unattainable insights in materials science. By contextualizing these advancements within the broader scientific landscape and highlighting their practical applications, this review aims to chart a course for future research in this rapidly evolving field.

Physics↗
DOE OSTI2023

Trapping-induced quantum beats in a van-der-Waals heterostructure microcavity observed by two-dimensional micro-spectroscopy

Spatial confinement has been frequently engineered to control the flow and relaxation dynamics of exciton polaritons. While widely investigated in GaAs microcavities, exciton-polariton coupling between discretized polariton modes arising from spatially confined 2D crystals been has been less exhaustively studied. Here, we use coherent 2D photoluminescence-detected micro-spectroscopy to detect oscillating 2D peaks exclusively from a spatial trap in a microcavity with an embedded van-der-Waals heterostructure at room temperature. We observe a wide variation of oscillatory phases as a function of spectral position within the 2D spectrum, which suggests the existence of a coupling between the discretized polariton modes. The latter is accompanied by the generation of coherent phonons.

Materials Science↗
DOE OSTI2021

Quasiparticle coherence in the nematic state of FeSe

We report electronic nematicity is a ubiquitous phenomenon in iron-based superconductors but its origin is still debated. Most models consider either spin or orbital degrees of freedom as the driving force but typically do not take electronic correlations into account. However, mass enhancements, coherent-incoherent crossovers, and the strong orbital differentiation can only be understood using correlations in a Hund's metal framework. Here, we study the influence of nematicity on the quasiparticle coherence in detwinned FeSe using angle-resolved photoemission spectroscopy (ARPES). We compare photoemission spectral weight from d xz and d yz orbitals in the coherent quasiparticle peak and in the incoherent Hubbard band and find an anisotropy between the two orbitals. We interpret our observation in terms of a more coherent d xz orbital compared to the d yz orbital inside the nematic phase. This result is in contrast to earlier predictions of an incoherent d xz orbital and highlights the importance of electronic correlations in the description of nematicity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

A Contrast Calibration Protocol for X-ray Speckle Visibility Spectroscopy

X-ray free electron lasers, with their ultrashort highly coherent pulses, opened up the opportunity of probing ultrafast nano- and atomic-scale dynamics in amorphous and disordered material systems via speckle visibility spectroscopy. However, the anticipated count rate in a typical experiment is usually low. Therefore, visibility needs to be extracted via photon statistics analysis, i.e., by estimating the probabilities of multiple photons per pixel events using pixelated detectors. Considering the realistic X-ray detector responses including charge cloud sharing between pixels, pixel readout noise, and gain non-uniformity, speckle visibility extraction relying on photon assignment algorithms are often computationally demanding and suffer from systematic errors. In this paper, we present a systematic study of the commonly-used algorithms by applying them to an experimental data set containing small-angle coherent scattering with visibility levels ranging from below 1% to ∼60%. We also propose a contrast calibration protocol and show that a computationally lightweight algorithm can be implemented for high-speed correlation evaluation.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

Theoretical framework for soft X-ray Fourier transform spectroscopy using the Wigner function

This work presents a theoretical framework for the propagation of partially coherent Gaussian radiation in a modified Mach–Zehnder interferometer designed for Fourier transform spectroscopy (FTS) applications. Using the Wigner function formalism, we analytically propagate the radiation through the system and benchmark our approach by comparing the resulting interference pattern and interferogram with previous works in the diffraction limit. Our analysis reveals that the transverse coherence length requirement of the incident light field for detectable modulation is less stringent than previously assumed. Additionally, we provide theoretical demonstrations of FTS performance across various wavelengths using the proposed setup. These findings underscore the potential of this interferometer to achieve high-resolution FTS in the soft X-ray regime.

Fourier transform spectroscopy↗
DOE OSTI2021

Transparent window 2D IR spectroscopy of proteins

Proteins are complex, heterogeneous macromolecules that exist as ensembles of interconverting states on a complex energy landscape. A complete, molecular-level understanding of their function requires experimental tools to characterize them with high spatial and temporal precision. Infrared (IR) spectroscopy has an inherently fast time scale that can capture all states and their dynamics with, in principle, bond-specific spatial resolution. Two-dimensional (2D) IR methods that provide richer information are becoming more routine but remain challenging to apply to proteins. Spectral congestion typically prevents selective investigation of native vibrations; however, the problem can be overcome by site-specific introduction of amino acid side chains that have vibrational groups with frequencies in the “transparent window” of protein spectra. This Perspective provides an overview of the history and recent progress in the development of transparent window 2D IR of proteins.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2004

The Role of Coherent Detection

Many interesting astronomical objects, such as galaxies, molecular clouds, PDRs, star - forming regions, protostars, evolved stars, planets, and comets, have rich submillimeter spectra. In order to avoid line blending, and to be able to resolve the line shape, it is often necessary to measure these spectra at high resolution. This paper discusses the relative advantages and limitations of coherent and direct detection for high resolution spectroscopy in the submillimeter and far - infrared. In principle, direct detection has a fundamental sensitivity advantage. In practice, it is di.cult to realize this advantage given the sensitivities of existing detectors and reasonable constraints on the instrument volume. Thus, coherent detection can be expected to play an important role in submillimeter and far - infrared astrophysics well into the future.

Zmuidzinas, J.↗
DOE OSTI2024

Ultrafast all-optical coherence of molecular electron spins in room-temperature water solution

The tunability and spatial precision of paramagnetic molecules makes them attractive for quantum sensing. However, usual microwave-based detection methods have poor temporal and spatial resolution, and optical methods compatible with room-temperature solutions have remained elusive. In this study, we utilized pump-probe polarization spectroscopy to initialize and track electron spin coherence in a molecule. Designed to efficiently couple spins to light, aqueous potassium hexachloroiridate(IV) enabled detection of few-picosecond free-induction decay at room temperature and micromolar concentrations. Viscosity was found to strongly vary decoherence lifetimes. This approach has improved the experimental time resolution by up to five orders of magnitude, making it possible to observe molecular electron spin coherence in a system that only exhibits coherence below 25 kelvin with traditional techniques.

74 ATOMIC AND MOLECULAR PHYSICS↗