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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 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
NASA NTRS2012

Frequency Correction for MIRO Chirp Transformation Spectroscopy Spectrum

This software processes the flyby spectra of the Chirp Transform Spectrometer (CTS) of the Microwave Instrument for Rosetta Orbiter (MIRO). The tool corrects the effect of Doppler shift and local-oscillator (LO) frequency shift during the flyby mode of MIRO operations. The frequency correction for CTS flyby spectra is performed and is integrated with multiple spectra into a high signal-to-noise averaged spectrum at the rest-frame RF frequency. This innovation also generates the 8 molecular line spectra by dividing continuous 4,096-channel CTS spectra. The 8 line spectra can then be readily used for scientific investigations. A spectral line that is at its rest frequency in the frame of the Earth or an asteroid will be observed with a time-varying Doppler shift as seen by MIRO. The frequency shift is toward the higher RF frequencies on approach, and toward lower RF frequencies on departure. The magnitude of the shift depends on the flyby velocity. The result of time-varying Doppler shift is that of an observed spectral line will be seen to move from channel to channel in the CTS spectrometer. The direction (higher or lower frequency) in the spectrometer depends on the spectral line frequency under consideration. In order to analyze the flyby spectra, two steps are required. First, individual spectra must be corrected for the Doppler shift so that individual spectra can be superimposed at the same rest frequency for integration purposes. Second, a correction needs to be applied to the CTS spectra to account for the LO frequency shifts that are applied to asteroid mode.

Lee, Seungwon↗
NASA NTRS1997

Bromine Dioxide, OBrO: The Rotational Spectrum and Molecular Properties

The spectra are well descrie by Hamiltonian which included centrifugal distortion efects for fine and hyperfine terms. The molecular structure and the harmonic force field have been derived, and they as well as fine and hyperfine structure constants, are compared with data of related molecules and ESR data from OBrO isolated in cryogenic salt matrices.

Bromine Dioxide Rotational Spectrum↗
NASA NTRS1977

Photoabsorption in formaldehyde

Theoretical studies of the vertical electronic dipole excitation and ionization spectra in molecular formaldehyde are reported. The investigations relied on configuration-interaction calculations and moment-theory techniques. A double-zeta basis of contracted Gaussian-lobe functions supplemented with appropriate polarization and bond functions was used to construct Fock spectra in C(2 nu) symmetry for certain states near the ground state equilibrium geometry. The ionization energies, discrete vertical transition frequencies, and oscillator strengths for occupied and vertical Fock orbitals are in general accord with experimental determinations and other theoretical calculations. Stieltjes and Chebyshev vertical electronic photoionization profiles were calculated and found to be in good agreement with appropriately averaged photoionization-mass spectrometric measurements of the cross section for parent H2CO(+) ion production.

Langhoff, P. W.↗
NASA NTRS2005

Differential Cross Sections for the Electron Impact Excitation of the A(sup 3)(Sigma)(sub u)(sup +), B(sup 3)Pi(sub g), W(sup 3)(Delta)(sub u), B'(sup 3)(Sigma)(sub u)(sup -), a'(sup 1)Sigma(sub u)(sup -), a(sup 1)Pi(sub g), w(sup 1)Delta(sub u), and C(sup 3)Pi(sub u) States of N(sub 2)

Measurements of differential cross sections for the electron-impact excitation of molecular nitrogen from the ground X(sup 1)(Sigma)(sub g)(sup +)(v''=0)level to the A(sup 3)(Sigma)(sub u)(sup +)(v'), B(sup 3)Pi(sub g)(v'), W(sup 3)(Delta)(sub u)(v'),B'(sup 3)(Sigma)(sub u)(sup -)(v'), a(sup 1)(Pi)(sub g)(v'), w(sup 1)(Delta)(sub u)(v'), and C(sup 3)(Pi)(sub u)(v') levels are presented. The data are obtained at the incident energies of 10, 12.5, 15, 17.5, 20, 30, 50, and 100 eV over the angular range of 5(deg)-130(deg) in 5(deg) intervals. The individual electronic state excitation differential cross sections are obtained by unfolding electron energy-loss spectra of molecular nitrogen using available semiempirical Frank-Condon factors. The data are compared to previous measurements and to available theory. We also make several important suggestions regarding future work that, like the present, relies on the unfolding of electron energy-loss spectra for obtaining differential cross sections.

electron impact↗
DOE OSTI2026

Photoabsorption and photoionization of N2 near the first ionization threshold

The photoabsorption and photoionization spectra of molecular nitrogen, N2, near the first ionisation threshold display numerous intense resonances that have not been satisfactorily assigned to date. Principal among these is a pair of broad resonances between 126,200 and 126,600 cm−1 commonly referred to as the ”cathedral” bands. Here, we present new double-resonance photoionization spectra in this region recorded via the 𝑎′′ 1Σ+ 𝑔,𝑣′=0 intermediate state as well as new high-resolution, vacuum-ultraviolet photoabsorption spectra of 14N2,14N15N, and 15N2 to provide additional insight into the assignment of these features. Progress towards a fully consistent interpretation of the existing data on these bands is discussed, and a route towards a comprehensive description of the N2 absorption spectrum up to the 𝐵 2Σ+ 𝑢 state of N+ 2 is proposed.

Nitrogen, vacuum ultraviolet absorption, photoioni↗
NASA NTRS2013

Absorption and Scattering by Molecules and Particles

The Earth's atmosphere absorbs, scatters, and emits electromagnetic radiation. Although air molecules are the primary actors in these processes, aerosol particles are also present ubiquitously and modify the radiation field. In fact, this modification constitutes the very physical basis of aerosol remote sensing. Whenever clouds are present, they have a much larger influence on radiation which largely overshadows the aerosol impact. Therefore, in aerosol remote sensing, one often has to limit observations to cloudless conditions and screen cloudy pixels. In the solar part of the spectrum, molecular absorption is mostly limited to ultraviolet (UV; ozone) and near-infrared (near-IR; carbon dioxide, water vapor) wavelengths and is characterized by strong and narrow oxygen bands. A brief description of atmospheric molecular absorption is presented in Section 2.2. Shortwave aerosol remote sensing is usually performed outside the absorption bands, but some instruments also have channels capturing absorption bands with the objective of quantifying gaseous components.

remote sensing↗
DOE OSTI2021

Two-dimensional electronic–vibrational spectroscopy: Exploring the interplay of electrons and nuclei in excited state molecular dynamics

Two-dimensional electronic-vibrational spectroscopy (2DEVS) is an emerging spectroscopic technique which exploits two different frequency ranges for the excitation (visible) and detection (infrared) axes of a 2D spectrum. In contrast to degenerate 2D techniques, such as 2D electronic or 2D infrared spectroscopy, the spectral features of a 2DEV spectrum report cross correlations between fluctuating electronic and vibrational energy gaps rather than autocorrelations as in the degenerate spectroscopies. The center line slope of the spectral features reports on this cross correlation function directly and can reveal specific electronic-vibrational couplings and rapid changes in the electronic structure, for example. The involvement of the two types of transition moments, visible and infrared, makes 2DEVS very sensitive to electronic and vibronic mixing. 2DEV spectra also feature improved spectral resolution, making the method valuable for unraveling the highly congested spectra of molecular complexes. The unique features of 2DEVS are illustrated in this paper with specific examples and their origin described at an intuitive level with references to formal derivations provided. Although early in its development and far from fully explored, 2DEVS has already proven to be a valuable addition to the tool box of ultrafast nonlinear optical spectroscopy and is of promising potential in future efforts to explore the intricate connection between electronic and vibrational nuclear degrees of freedom in energy and charge transport applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Predicting High‐Resolution Spatial and Spectral Features in Mass Spectrometry Imaging with Machine Learning and Multimodal Data Fusion

Recent advancements in molecular Mass Spectrometry Imaging have sparked interest in integrating high spatial resolution methods with molecular mass-spectrometry-based chemical imaging. Fusion-based algorithms have proven effective in generating high spatial-resolution molecular mass spectra. However, a significant challenge stems from the differing physical mechanisms underlying image generation and data upsampling techniques, potentially leading to discrepancies in integrated information channels. Integrating physical constraints into data processing workflows is essential to tackle this issue. In this study, we propose an innovative approach that merges data from Fourier transform ion cyclotron resonance (FTICR), time-of-flight matrix-assisted laser desorption/ionization, and time-of-flight secondary ion mass spectrometry imaging techniques. By leveraging FT-ICR's unparalleled spectral resolution and ToF-SIMS's exceptional spatial resolution, we achieve submicron spatial resolution, enabling the observation of intact molecular species with remarkable spectral precision. Canonical correlation analysis is employed to incorporate physical constraints. Through sophisticated image processing and machine learning techniques, the results of this fusion hold significant promise for advancing our comprehension of complex systems and unveiling concealed molecular intricacies.

canonical correlation analysis↗
DOE OSTI2020

Vibrational spectroscopy of shock compressed condensed phase nitrous oxide: Frequency shifts in the ν 1 mode

Over many years, we have published vibrational spectra of molecular materials at extreme pressure and temperature obtained using shock compression and coherent Raman spectroscopy methods. For diatomic molecules, we were able to extract vibrational temperatures from the intensities of spectrally resolved vibrational hot bands. Larger molecules in the condensed phase suffer band broadening effects that obscure the vibrational hot bands as the anharmonicities are typically smaller than the widths of the bands. This inability to resolve the hot bands inhibits the extraction of vibrational temperature and the measurement of the vibrational frequency of the fundamental. Here, we use a hot band model based on gas-phase anharmonic coupling coefficients to fit coherent anti-Stokes Raman spectra of the ν 1 vibrational mode of shock compressed condensed phase N 2 O with shock pressures and temperatures estimated from literature equations of state and compare to fits from a model using a single Gaussian peak. We report the resulting vibrational frequency shifts with shock pressure.

36 MATERIALS SCIENCE↗
NASA NTRS1994

Pre- and postperihelon abundances of gas and dust in comet Halley

Photometrically calibrated spectra of comet P/Halley (1986 III) were recorded between 1985 September 12-1986 June 10 using the Ohio State University Image Dissector Scanner on the Perkins 72 inch telescope at the Lowell Observatory. Column densities of CN, C3, CH, C2, and NH2 were calculated from measured fluxes in these spectra, and molecular scale lengths were deduced from the radial distribution of CN, C3, C2, and NH2. Production rates were computed using the new scale lengths and a Haser model analysis. Continuum emission at 4260 A was used to derive gas-to-dust ratios. The data indicate than comet Halley was approximately 2-5 times more abundant in gas and dust at postperihelion than preperihelion. On 1986 June 8 we observed the onset of a cometary ourburst which appeared very strong in dust production. The gas-to-dust ratios appeared to be subject to changes as a result of short-term outbursts but otherwise did not exhibit any systematic dependence on heliocentric distance. Reflectivity gradients of the continuum were also measured from the spectra. While most of the continua were red, blue continua were also observed which may be correlated with dust outbursts.

Womack, Maria↗
NASA NTRS1995

The Ultraviolet Spectrum of the Jovian Dayglow

The ultraviolet spectra of molecular hydrogen H2 and HD due to solar fluorescence and photoelectron excitation are calculated and compared with the Jovian equatorial dayglow spectrum measured at 3 A resolution at solar maximum. The dayglow emission is accounted for in both brightness and spectral shape by the solar fluorescence and photoelectron excitation and requires no additional energy source. The emission is characterized by an atmospheric temperature of 530 K and an H2 column density of 10(exp 20) cm(exp -2). The dayglow spectrum contains a cascade contribution to the Lyman band emission from high-lying E and F states. Its relative weakness at short wavelengths is due to both self-absorption by H2 and absorption by CH4. Strong wavelength coincidences of solar emission lines and absorption lines of H2 and HD produce unique line spectra which can be identified in the dayglow spectrum. The strongest fluorescence is due to absorption of the solar Lyman-beta line at 1025.72 A by the P(1) line of the (6, 0) Lyman band of H2 at 1025.93 A. The fluorescence lines due to absorption of the solar O 6 line at 1031.91 A by vibrationally excited H2 via the Q(3) line of the (1, 1) Werner band at 1031.86 A are identified. The fluorescence lines provide a sensitive measure of the atmospheric temperature. There occurs an exact coincidence of the solar O 6 line at 1031.91 A and the R(0) line of the (6, 0) Lyman band of HD at 1031-91 A, but HD on Jupiter is difficult to detect due to the dominance of the H2 emission where the HD emission is particularly strong. Higher spectral resolution and higher sensitivity may make possible such a detection. The high resolution (0.3 A) spectra of H2 and HD are presented to stimulate search for the HD on Jupiter with the Hubble Space Telescope.

Liu, Weihong↗
DOE OSTI2024

Exploring the exact limits of the real-time equation-of-motion coupled cluster cumulant Green’s functions

In this paper, we analyze the properties of the recently proposed real-time equation-of-motion coupled-cluster (RT-EOM-CC) cumulant Green’s function approach [Rehr et al., J. Chem. Phys. 152, 174113 (2020)]. We specifically focus on identifying the limitations of the original time-dependent coupled cluster (TDCC) ansatz and propose an enhanced double TDCC ansatz, ensuring the exactness in the expansion limit. In addition, we introduce a practical cluster-analysis-based approach for characterizing the peaks in the computed spectral function from the RT-EOM-CC cumulant Green’s function approach, which is particularly useful for the assignments of satellite peaks when many-body effects dominate the spectra. Our preliminary numerical tests focus on reproducing, approximating, and characterizing the exact impurity Green’s function of the three-site and four-site single impurity Anderson models using the RT-EOM-CC cumulant Green’s function approach. The numerical tests allow us to have a direct comparison between the RT-EOM-CC cumulant Green’s function approach and other Green’s function approaches in the numerical exact limit.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Toward the origins of binding energy shifts and “satellites” formation during plasma-XPS measurements

In-plasma x-ray photoelectron spectroscopy (plasma-XPS) emerges as a powerful platform for real-time, in situ chemical analysis under conditions relevant to semiconductor processing and other plasma-enabled technologies. This study investigates the origins of binding energy (BE) shifts and the formation of “satellite” peaks observed during plasma-XPS measurements across conductive, dielectric, and gas-phase systems. Using a standard laboratory-based ambient pressure XPS apparatus coupled with an alternating current (AC)-driven capacitively coupled plasma source, we demonstrate that metastable surface species, such as transient Au oxides, can be detected during plasma exposure, revealing chemical states that are hardly accessible using conventional ultrahigh vacuum (UHV) XPS. In dielectric samples (e.g., undoped diamond, sapphire), we observe pressure- and plasma-type-dependent BE shifts of more than 50 eV, attributed to x-ray-induced and plasma-mediated surface charging. These shifts are mitigated at higher pressures/plasmas or in electronegative plasmas (e.g., O 2 ), the latter due to enhanced charge compensation mechanisms involving slow negative ions. For gas-phase species, AC-plasma excitation leads to spectral broadening and the emergence of “satellite” peaks with energy separations of a few electron volts, linked to oscillating local plasma potentials in the probing volume. Furthermore, these findings highlight the complex and important interplay between plasma parameters, surface charging, and local electric fields in shaping XPS spectra. Overall, plasma-XPS emerges as a critical metrological tool for probing transient surface chemistry, with implications for semiconductor processing, material synthesis, and plasma diagnostics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Twin Polaritons: Classical versus Quantum Features in Polaritonic Spectra

Understanding whether a polaritonic phenomenon is fundamentally quantum or classical is essential for building accurate theoretical models and guiding experimental design. Here, in this work, we address this question in the context of polaritonic spectra and report an intriguing new feature: the twin polariton, an additional splitting beyond the primary resonant polariton splitting originating from vacuum field fluctuations. We show that the twin polariton persists in the many-molecule limit under permutationally symmetrical initial-state constraint and that it follows the same linear dependence on coupling strength as the primary polariton splitting. This establishes a novel mechanism by which a quantum feature (the twin polariton) can be tuned through a classical one (the primary polariton), offering new opportunities to probe and control the fundamental nature of polaritonic systems.

classical optics↗
DOE OSTI2021

Particle transport constraints via Bayesian spectral fitting of multiple atomic lines

Optimized operation of fusion devices demands detailed understanding of plasma transport, a problem that must be addressed with advances in both measurement and data analysis techniques. In this work, we adopt Bayesian inference methods to determine experimental particle transport, leveraging opportunities from high-resolution He-like ion spectra in a tokamak plasma. The Bayesian spectral fitting code is used to analyze resonance (w), forbidden (z), intercombination (x, y), and satellite (k, j) lines of He-like Ca following laser blow-off injections on Alcator C-Mod. This offers powerful transport constraints since these lines depend differently on electron temperature and density, but also differ in their relation to Li-like, He-like, and H-like ion densities, often the dominant Ca charge states over most of the C-Mod plasma radius. Using synthetic diagnostics based on the AURORA package, we demonstrate improved effectiveness of impurity transport inferences when spectroscopic data from a progressively larger number of lines are included.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Evaluation of the excitation spectra with diffusion Monte Carlo on an auxiliary bosonic ground state

We aim to improve upon the variational Monte Carlo (VMC) approach for excitations replacing the Jastrow factor by an auxiliary bosonic (AB) ground state and multiplying it by a fermionic component factor. The instantaneous change in imaginary time of an arbitrary excitation in the original interacting fermionic system is obtained by measuring observables via the ground-state distribution of walkers of an AB system that is subject to an auxiliary effective potential. The effective potential is used to (i) drive the AB system’s ground-state configuration space toward the configuration space of the excitations of the original fermionic system and (ii) subtract from a diffusion Monte Carlo (DMC) calculation contributions that can be included in conventional approximations, such as mean-field and configuration interaction (CI) methods. In this novel approach, the AB ground state is treated statistically in DMC, whereas the fermionic component of the original system is expanded in a basis. The excitation energies of the fermionic eigenstates are obtained by sampling a fermion–boson coupling term on the AB ground state. We show that this approach can take advantage of and correct for approximate eigenstates obtained via mean-field calculations or truncated interactions. We demonstrate that the AB ground-state factor incorporates the correlations missed by standard Jastrow factors, further reducing basis truncation errors. Relevant parts of the theory have been tested in soluble model systems and exhibit excellent agreement with exact analytical data and CI and VMC approaches. In particular, for limited basis set expansions and sufficient statistics, AB approaches outperform CI and VMC in terms of basis size for the same systems. The implementation of this method in current codes, despite being demanding, will be facilitated by reusing procedures already developed for calculating ground-state properties with DMC and excitations with VMC.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗