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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Absolute throughput calibration of multiple spherical crystals for the Orion High-REsolution X-ray spectrometer (OHREX)

We present absolute throughput analysis of several crystals for the Orion High-REsolution X-ray (OHREX) imaging crystal spectrometer using ray tracing and experimental measurements. The OHREX spectrometer is a high-resolution x-ray spectrometer designed to measure spectral line shapes at the Orion laser facility. The spectrometer is fielded with up to two spherical crystals simultaneously covering two independent spectral ranges. Each crystal has a nominal radius of curvature of R = 67.2 cm and is fielded at a nominal Bragg angle of 51.3°. To cover different bands of interest, several different crystals are available, including Ge (111), KAP, and several cuts of quartz, whose resolving power λ/Δλ exceeds 10 000. The calibrated response of the available crystals has previously been reported from measurements at the EBIT-I electron beam ion trap at Lawrence Livermore National Laboratory. Here, we model the absolute throughput of each crystal using ray tracing and verify the results using experimental data for the quartz $(10\bar{1}1)$ crystal.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

X-ray photoelectron spectroscopy of epitaxial films and heterostructures

X-ray photoelectron spectroscopy is a powerful experimental technique that yields invaluable information on a range of phenomena that occur in solids, liquids, and gasses. The binding energy and shape of a photoemission peak is sensitive not only to the atomic number, valence and orbital from which the electron is ejected, but also to complex many-body effects that accompany photoemission. Provided the influences of these different drivers of spectral line shapes can be disentangled, a great deal can be learned about the electronic structures of specific atoms in the material of interest. In addition to these largely local effects, the long-range electrostatic environment and resulting electric potential at the emitting atom have a direct effect on the measured binding energies. Furthermore, this fact opens the door to extracting information about the dependence of the valence and conduction band minima on depth below the surface, which in turn allows both vertical and lateral electrical transport data to be better understood. One purpose of this Report is to describe how the different physical forces described above impact spectral properties of complex oxide epitaxial films. This class of materials typically incorporates transition metal cations in different valences and of all the elements, these exhibit the most complex core-level spectra. A second purpose is to show how a comprehensive understanding of local physical effects in x-ray photoemission allows one to extract detailed information on internal electric fields and band edge discontinuities in heterostructures involving complex oxides from core-level line shapes.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Extracting doubly excited state lifetimes in helium directly in the time domain with attosecond noncollinear four-wave-mixing spectroscopy

The helium atom, with one nucleus and two electrons, is a prototypical system to study quantum many-body dynamics. Doubly excited states, or quantum states in which both electrons are excited by one photon, showcase electronic-correlation mediated effects. In this paper, the natural lifetimes of the doubly excited 1 P o 2 s n p Rydberg series and the 1 S e 2 p 2 dark state in helium in the 60–65 eV region are measured directly in the time domain with extreme-ultraviolet/near-infrared noncollinear attosecond four-wave-mixing (FWM) spectroscopy. The measured lifetimes agree with lifetimes deduced from spectral linewidths and theoretical predictions, and the roles of specific decay mechanisms are considered. While complex spectral line shapes in the form of Fano resonances are common in absorption spectroscopy of autoionizing states, the background-free and thus homodyned character of noncollinear FWM results exclusively in Lorentzian spectral features in the absence of strong-field effects. The onset of strong-field effects that would affect the extraction of accurate natural lifetimes in helium by FWM is determined to be approximately 0.3 Rabi cycles. This study provides a systematic understanding of the FWM parameters necessary to enable accurate lifetime extractions, which can be utilized in more complex quantum systems in the future. Published by the American Physical Society 2024

Rupprecht, Patrick (ORCID:000000026491793X)↗
DOE OSTI2024

Second-order spectral line shift comparisons

The second-order spectral line width formulae from the projection operator and kinetic theory methods were recently compared. It was shown that a systematic expansion of the projection operator width expression including initial correlations formally agrees with the second-order kinetic theory result. It is now shown that the second-order dynamic shifts are also formally the same. The static shifts, however, differ due to an ad hoc treatment of electron-electron correlations in the projection operator method. The approximation is necessary in order to screen the radiator-electron interactions. The differences, however, are expected to be small. Finally, the results suggest using the rigorous and more compact second-order width and shift expressions from the kinetic theory method as the starting point for spectral line shape calculations. At line center, however, the projection operator second-order expression for the width and shift simplifies and reduces to the kinetic theory result.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Explicit environmental and vibronic effects in simulations of linear and nonlinear optical spectroscopy

Accurately simulating the linear and nonlinear electronic spectra of condensed phase systems and accounting for all physical phenomena contributing to spectral line shapes presents a significant challenge. Vibronic transitions can be captured through a harmonic model generated from the normal modes of a chromophore, but it is challenging to also include the effects of specific chromophore–environment interactions within such a model. We work to overcome this limitation by combining approaches to account for both explicit environment interactions and vibronic couplings for simulating both linear and nonlinear optical spectra. We present and show results for three approaches of varying computational cost for combining ensemble sampling of chromophore–environment configurations with Franck–Condon line shapes for simulating linear spectra. We present two analogous approaches for nonlinear spectra. Simulated absorption spectra and two-dimensional electronic spectra (2DES) are presented for the Nile red chromophore in different solvent environments. Furthermore, employing an average Franck–Condon or 2DES line shape appears to be a promising method for simulating linear and nonlinear spectroscopy for a chromophore in the condensed phase.

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

Temperature and density dependence of Kr L-shell spectrum in hot dense plasmas

Kr L-shell spectroscopy modeling results are discussed in this paper, focusing on the n = 4 to n = 2 line transitions of Be- and Li-like Kr ions. Collisional radiative atomic kinetic and Stark-broadened spectral line shape calculations show electron temperature Te and density ne sensitivity in the spectrum. The combination of the Te dependence due to the relative intensity of Be-like to Li-like line emissions in the range from 1.5 to 3 keV and the ne sensitivity from the Stark broadening effect on the line shapes in the range from 5×1023 to 2×1024/ cc results in a spectrum that can be employed to diagnose Te and ne. Two different collisional radiative atomic kinetic models i.e., Prismspect [J. J. MacFarlane, et al., Int. Fusion Sci. Appl. Conf. Proc. 457 (2003)] and ABAKO [Florido, et al., PRE, 80, 056402 (2009)] produce similar results in level populations and spectra. In x-ray spectroscopy of implosion cores, this Kr L-shell spectrum may prove useful in an intermediate Te range in which Ar is too ionized for its K-shell to be of diagnostic value and Kr is not ionized enough for its K-shell emission to be useful.

Physics↗
DOE OSTI2025

Analysis methodology of coherent oscillations in time- and angle-resolved photoemission spectroscopy

Oscillatory signals from coherently excited phonons are regularly observed in ultrafast pump–probe experiments on condensed matter samples. Electron–phonon coupling implies that coherent phonons also modulate the electronic band structure. These oscillations can be probed with energy and momentum resolution using time- and angle-resolved photoemission spectroscopy (trARPES), which reveals the orbital dependence of the electron–phonon coupling for a specific phonon mode. However, a comprehensive analysis remains challenging when multiple coherent phonon modes couple to multiple electronic bands. Complex spectral line shapes due to strong correlations in quantum materials add to this challenge. In this work, we examine how the frequency domain representation of trARPES data facilitates a quantitative analysis of coherent oscillations of the electronic bands. Here, we investigate the frequency domain representation of the photoemission intensity and the first moment of the energy distribution curves. Both quantities provide complementary information and are able to distinguish oscillations of binding energy, linewidth, and intensity. We analyze a representative trARPES dataset of the transition metal dichalcogenide WTe 2 and construct composite spectra, which intuitively illustrate how much each electronic band is affected by a specific phonon mode. We also show how a linearly chirped probe pulse can generate extrinsic artifacts that are distinct from the intrinsic coherent phonon signal.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Structured light approaches in laser-based plasma diagnostics

There is a growing demand for plasma diagnostics suitable for industrial plasma reactors employed in semiconductor nanofabrication, especially relevant to microelectronics and quantum information systems. Such reactors typically have limited optical access and pose considerable diagnostic challenges, including intense background emission, significant thermal loads, and contamination of optical viewports. In this study, we outline research into structured light techniques (laser beams with tailored spatial, temporal, or phase characteristics) that effectively overcome these issues using laser-induced fluorescence (LIF) as an example. The focus of presented diagnostics is on ion kinetics analysis within an industrial plasma source, although this approach is broadly applicable to other plasma systems and diagnostic contexts. We present a confocal LIF implementation using an axicon-generated Bessel annular beam, achieving spatial resolutions of approximately 5 mm at a focal distance of 300 mm, with potential improvements to about 1 mm. This approach matches conventional orthogonal LIF performance but requires only one optical port. Wavelength-modulation LIF employs nonlinear laser wavelength tuning to measure spectral line derivatives, suppressing background emission and enhancing details of spectral line shape. Additionally, we present new results on applying vortex beams (laser beams carrying orbital angular momentum, OAM) for LIF measurements in an industrial plasma device. These measurements enable simultaneous axial and tangential velocity determination using a single laser beam and have been tested with xenon ion transition. Initial quantification of results was performed. Together, these structured-light approaches provide robust, background-resilient, multi-dimensional diagnostics for complex plasma environments.

Romadanov, Ivan [Princeton Plasma Physics Laborato↗
DOE OSTI2026

Scattering theory of frequency-entangled biphoton states facilitated by cavity polaritons

The use of quantum light to probe exciton properties in semiconductor and molecular nanostructures typically occurs in the low-intensity regime. A substantial enhancement of exciton-photon coupling can be achieved with photonic cavities, where excitons hybridize with cavity modes to form polariton states. Here, to provide a theoretical framework for interpreting emerging experimental efforts in this direction, we develop a scattering theory describing the interaction of frequency-entangled photon pairs with cavity polariton and bipolariton states under various coupling regimes. Employing the Tavis-Cummings model in combination with our scattering approach, we present a quantitative analysis of how the interaction of the entangled photon pair with the polariton or bipolariton modifies its joint spectral amplitude (JSA). Specifically, we examine the effects of the cavity-mode steady-state population, exciton-cavity coupling strength, and different forms of the input photon JSA. Our results show that the entanglement entropy of the scattered photons is highly sensitive to the interplay between the input JSA and the spectral line shapes of the polariton resonances, emphasizing the cavity filtering effects. We suggest that biphoton-scattering quantum light spectroscopy best serves as a sensitive probe of polariton and bipolariton states in the photon-vacuum cavity state. Our approach is not only robust to various regimes of cavity-exciton coupling, but also amenable to extensions beyond the Tavis-Cummings model, enabling the representation of a broad class of molecular systems and solid state quantum materials.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Two-Photon Spontaneous Emission in Atomically Thin Plasmonic Nanostructures

The ability to harness light-matter interactions at the few-photon level plays a pivotal role in quantum technologies. Single photons—the most elementary states of light—can be generated on demand in atomic and solid state emitters. Two-photon states are also key quantum assets, but achieving them in individual emitters is challenging because their generation rate is much slower than competing one-photon processes. We demonstrate that atomically thin plasmonic nanostructures can harness two-photon spontaneous emission, resulting in giant far field two-photon production, a wealth of resonant modes enabling tailored photonic and plasmonic entangled states, and plasmon-assisted single-photon creation orders of magnitude more efficient than standard one-photon emission. We unravel the two-photon spontaneous emission channels and show that their spectral line shapes emerge from an intricate interplay between Fano and Lorentzian resonances. Enhanced two-photon spontaneous emission in two-dimensional nanostructures paves the way to an alternative efficient source of light-matter entanglement for on-chip quantum information processing and free-space quantum communications.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Direct Observation of Coherent Longitudinal and Shear Acoustic Phonons in TaAs Using Ultrafast X-Ray Diffraction

Here, using femtosecond time-resolved x-ray diffraction, we investigated optically excited coherent acoustic phonons in the Weyl semimetal TaAs. The low symmetry of the (112) surface probed in our experiment enables the simultaneous excitation of longitudinal and shear acoustic modes, whose dispersion closely matches our simulations. We observed an asymmetry in the spectral line shape of the longitudinal mode that is notably absent from the shear mode, suggesting a time-dependent frequency chirp that is likely driven by photoinduced carrier diffusion. We argue on the basis of symmetry that these acoustic deformations can transiently alter the electronic structure near the Weyl points and support this with model calculations. Our study underscores the benefit of using off-axis crystal orientations when optically exciting acoustic deformations in topological semimetals, allowing one to transiently change their crystal and electronic structures.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Introductory guide to the application of XPS to epitaxial films and heterostructures

XPS is an important characterization method for epitaxial films and heterostructures. Although standard approaches to XPS data collection and analysis provide useful information such as average composition and the presence of contaminants, more in-depth analysis provides information about film structure, surface termination, built-in electric potentials and band offsets. The high degree of structural order in these materials enables such information to be extracted from spectral data but also adds complications to the analysis. This guide highlights three topics of importance in this field: i) the impacts of crystallinity on XPS signals and quantification, ii) the unexpected spectral line shapes that can occur in unusual or novel materials, and, iii) the ability of XPS to yield information about built-in potentials and band offsets. Concepts are demonstrated using complex oxide heterostructures. Although the topics are highly relevant to epitaxial films and heterostructures, they also apply to signal crystals of complex materials

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2022

Balrog

SAND2022-12602 O Balrog uses mathematical methods to calculate spectral line shapes in high-energy-density plasmas. Line shapes are a result of atomic perturbations by their surrounding plasmas, and this model captures much of the physics and generates model spectrum that can be used in data analysis and as an input for other models. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525.

Gomez, Thomas↗
DOE OSTI2025

Sequential spectral line analysis for accurate density and temperature diagnosis of laboratory opacity measurements

The accuracy of iron opacity calculated in stellar interiors has been questioned since the discovery of the “solar problem” and the discrepancies between the measured and modeled iron opacity reported in 2015. Experimental opacity benchmarks require accurate temperature and density measurements, which were inferred by analyzing tracer magnesium spectra in those experiments. Could the observed discrepancy be explained by insufficient accuracy in the inferred temperature, density, and their uncertainties? Previous analyses may have yielded biased results due to three limitations: (1) simultaneous multi-line fitting, (2) approximations in line-shape models, and (3) exclusion of certain spectral lines due to insufficient background characterization. Notably, the first issue is a common concern for many inversion methods, including Bayesian inferences. We present a refined analysis method that overcomes these limitations, applied to three categories of iron opacity experiments (Anchor 1, 2, and 3). In particular, the sequential fitting method yields unbiased results with more realistic uncertainties by accounting for line inconsistencies in the parameter uncertainties. The average electron temperature and density values are 162 ± 6 eV and (7.0 ± 1.9) × 10 21 cm −3 for six Anchor 1 experiments, 189 ± 7 eV and (3.4 ± 0.3) × 10 22 cm −3 for 21 Anchor 2 experiments, and 201 ± 6 eV and (4.8 ± 1.1) × 10 22 cm −3 for nine Anchor 3 experiments. These results show ∼4% temperature and ∼20% density reproducibility over a decade, which also aligns with the inferred parameter uncertainties. In conclusion, the resulting temperature and density uncertainties lead to a quasi-continuum iron opacity variation of ±4%–7% for wavelengths below 9.5 Å, which is insufficient to explain the significant model-data discrepancies reported in 2015.

Absorption spectroscopy↗
DOE OSTI2020

Isolating the Contributions of Specific Network Sites to the Diffuse Vibrational Spectrum of Interfacial Water with Isotopomer-Selective Spectroscopy of Cold Clusters

Decoding the structural information contained in the interfacial vibrational spectrum of water requires understanding how the spectral signatures of individual water molecules respond to their local hydrogen bonding environments. In this study, we isolated the contributions for the five classes of sites that differ according to the number of donor (D) and acceptor (A) hydrogen bonds that characterize each site. These patterns were measured by exploiting the unique properties of the water cluster cage structures formed in the gas phase upon hydration of a series of cations M+·(H2O)n (M = Li, Na, Cs, NH4, CH3NH3, H3O, and n = 5, 20-22). This selection of ions was chosen to systematically express the A, AD, AAD, ADD, and AADD hydrogen bonding motifs. The spectral signatures of each site were measured using two-color, IR-IR isotopomer-selective photofragmentation vibrational spectroscopy of the cryogenically cooled, mass selected cluster ions in which a single intact H2O is introduced without isotopic scrambling, an important advantage afforded by the cluster regime. The resulting patterns provide an unprecedented picture of the intrinsic line shapes and spectral complexities associated with excitation of the individual OH groups, as well as the correlation between the frequencies of the two OH groups on the same water molecule, as a function of network site. The properties of the surrounding water network that govern this frequency map are evaluated by dissecting electronic structure calculations that explore how changes in the nearby network structures, both within and beyond the first hydration shell, affect the local frequency of an OH oscillator. The qualitative trends are recovered with a simple model that correlates the OH frequency with the network-modulated local electron density in the center of the OH bond.

Yang, Nan↗
DOE OSTI2023

A Quantum-mechanical Treatment of Electron Broadening in Strong Magnetic Fields

Abstract Spectral line-shape fitting is an extremely useful tool in determining the gravity of white dwarf stars. This method is so far limited to nonmagnetic white dwarfs largely because the theory of line broadening in high magnetic fields is not as complete as in the nonmagnetic case. Current Stark+Zeeman models treat plasma particles classically and ignore the motion of the nucleus. We develop the formalism for a quantum-mechanical treatment of the perturbing electrons and include the nuclear motion as part of the broadening and explore their relative importance. The conditions we explore are those found in white dwarf and neutron star atmospheres. We find that, contrary to previous studies, the quantized perturbing electrons create more broadening than perturbers on a straight-path trajectory. Additionally, the quantization of the plasma electrons gives rise to resonances away from the line center. The nuclear motion creates an additional electric field, which also leads to an increase in line broadening; however, this effect in neutron star atmospheres is not as large as previously estimated. This suggests that neutron star spectral lines are sensitive to density and that their mass and radius can be obtained from spectral line fitting, which would help constrain the neutron star equation of state.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Multipole interaction in spectral line broadening by plasmas

A long-standing ambiguity in spectral line broadening theory related to the electric field divergence in the quadrupole term of the screened Coulomb radiator-plasma interaction is examined. This is accomplished with multipole expansions from a Taylor series as well as a partial wave analysis of the screened Coulomb interaction. Here, it is explicitly shown that the two approaches agree up to the octupole term for an effective radiator size small compared to the plasma screening length. Furthermore, the ambigous corrections are confirmed appearing naturally in both methods. For higher multipoles the agreement is demonstrated numerically with a computer program using exact arithmetic.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗