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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 541 records · Page 30
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Time domain probabilistic seismic risk analysis using ground motion prediction equations of Fourier amplitude spectra

Modeling of Fourier amplitude spectra (FAS) of seismic motions has gained much attention in engineering seismology. In the past few years, several ground motion prediction equations (GMPEs) and inter-frequency correlation structure of FAS have been established. Due to many preferable characteristics of FAS, probabilistic seismic hazard/risk analysis is rapidly changing from ergodic, spectrum acceleration Sa(T 0 )-based approach to non-ergodic, site-specific, FAS-based approach. This paper presents time domain intrusive framework for probabilistic seismic risk analysis using GMPE of FAS. Herein, methodology for time domain stochastic ground motion modeling based on GMPEs of FAS is presented in some detail. The simulated uncertain motions are modeled as a random process and represented by polynomial chaos Karhunen-Loève expansion. The random process excitations are further propagated into the uncertain structural system using Galerkin stochastic finite element method (SFEM). Probabilistic evolution of structural response is solved, and such solution is used to develop seismic risk for any damage state. The presented framework is illustrated through seismic risk analysis of a four-story building subjected to possible earthquakes from two strike slip faults. The influences of the epistemic uncertainties in source stress drop Δσ and site attenuation κ0 on seismic risk are investigated. The need for non-ergodic seismic risk analysis with source-specific and site specific characterizations is emphasized.

58 GEOSCIENCES↗
DOE OSTI2022

Ab initio calculation of X-ray and related core-level spectroscopies: Green's function approaches

X-Ray and related spectroscopies are powerful probes of atomic, vibrational, and electronic structure. In order to unlock the full potential of such experimental techniques, accurate and efficient theoretical and computational approaches are essential. Here we review the status of a variety of first-principles and nearly first principles techniques for X-ray spectroscopies such as X-ray absorption, X-ray emission, and X-ray photoemission, with a focus on Green's function based methods. In particular, we describe the current state of multiple scattering Green's function techniques available in the FEFF10 code and cumulant Green's function techniques for including the effects of many-body electronic excitations. Furthermore, illustrative examples are shown for a variety of materials and compared with other theoretical and experimental results.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Isoenergetic two-photon excitation enhances solvent-to-solute excited-state proton transfer

Two-photon excitation (TPE) is an attractive means for controlling chemistry in both space and time. Since isoenergetic one- and twophoton excitations (OPE and TPE) in non-centrosymmetric molecules are allowed to reach the same excited state, it is usually assumed that they produce similar excited-state reactivity. We compare the solvent-to-solute excited-state proton transfer of the super photobase FR0-SB following isoenergetic OPE and TPE. We find up to 62% increased reactivity following TPE compared to OPE. From steady-state spectroscopy, we rule out the involvement of different excited states and find that OPE and TPE spectra are identical in non-polar solvents but not in polar ones. We propose that differences in the matrix elements that contribute to the two-photon absorption cross sections lead to the observed enhanced isoenergetic reactivity, consistent with the predictions of our high-level coupledcluster-based computational protocol. We find that polar solvent configurations favor greater dipole moment change between ground and excited states, which enters the probability for TPE as the absolute value squared. This, in turn, causes a difference in the Franck– Condon region reached via TPE compared to OPE. We conclude that a new method has been found for controlling chemical reactivity via the matrix elements that affect two-photon cross sections, which may be of great utility for spatial and temporal precision chemistry.

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

Using a multistate mapping approach to surface hopping to predict the ultrafast electron diffraction signal of gas-phase cyclobutanone

Using the recently developed multistate mapping approach to surface hopping (multistate MASH) method combined with SA(3)-CASSCF(12,12)/aug-cc-pVDZ electronic structure calculations, the gas-phase isotropic ultrafast electron diffraction (UED) of cyclobutanone is predicted and analyzed. After excitation into the n-3s Rydberg state (S2), cyclobutanone can relax through two S2/S1 conical intersections, one characterized by compression of the CO bond and the other by dissociation of the α–CC bond. Subsequent transfer into the ground state (S0) is then achieved via two additional S1/S0 conical intersections that lead to three reaction pathways: α ring-opening, ethene/ketene production, and CO liberation. The isotropic gas-phase UED signal is predicted from the multistate MASH simulations, allowing for a direct comparison to the experimental data. This work, which is a contribution to the cyclobutanone prediction challenge, facilitates the identification of the main photoproducts in the UED signal and thereby emphasizes the importance of dynamics simulations for the interpretation of ultrafast experiments.

Chemistry↗
NASA NTRS1977

Application of system identification to analytic rotor modeling from simulated and wind tunnel dynamic test data, part 2

An introduction to aircraft state and parameter identification methods is presented. A simplified form of the maximum likelihood method is selected to extract analytical aeroelastic rotor models from simulated and dynamic wind tunnel test results for accelerated cyclic pitch stirring excitation. The dynamic inflow characteristics for forward flight conditions from the blade flapping responses without direct inflow measurements were examined. The rotor blades are essentially rigid for inplane bending and for torsion within the frequency range of study, but flexible in out-of-plane bending. Reverse flow effects are considered for high rotor advance ratios. Two inflow models are studied; the first is based on an equivalent blade Lock number, the second is based on a time delayed momentum inflow. In addition to the inflow parameters, basic rotor parameters like the blade natural frequency and the actual blade Lock number are identified together with measurement bias values. The effect of the theoretical dynamic inflow on the rotor eigenvalues is evaluated.

Hohenemser, K. H.↗
NASA NTRS1981

Substructure program for analysis of helicopter vibrations

A substructure vibration analysis which was developed as a design tool for predicting helicopter vibrations is described. The substructure assembly method and the composition of the transformation matrix are analyzed. The procedure for obtaining solutions to the equations of motion is illustrated for the steady-state forced response solution mode, and rotor hub load excitation and impedance are analyzed. Calculation of the mass, damping, and stiffness matrices, as well as the forcing function vectors of physical components resident in the base program code, are discussed in detail. Refinement of the model is achieved by exercising modules which interface with the external program to represent rotor induced variable inflow and fuselage induced variable inflow at the rotor. The calculation of various flow fields is discussed, and base program applications are detailed.

Sopher, R.↗
NASA NTRS1990

An approximate method for the calculation of nonequilibrium radiative heat transfer

A simplified method for the calculation of radiative heat transfer in hypersonic reentry flows where local thermal nonequilibrium (LTNE) conditions exist is presented. This method has been incorporated into the computer code RADMC (RADiation/Modified Corrections), which utilizes an approximate 'two-state' model of the electronic levels of atoms and molecules in the determination of the populations of the excited states for both LTNE and local thermal equilibrium (LTE) conditions for each of the relevant chemical species. The population data are used to calculate a correction factor to the radiative cross sections in an eight-step nongray radiative heat-transfer model. Results have been obtained for various points along the proposed trajectory of the Aeroassist Flight Experiment and the Fire II trajectory, and compared with results obtained for the same flowfields from the NEQAIR radiative heat-transfer code.

Greendyke, Robert B.↗
NASA NTRS1995

The Heat of Formation of HNO

The HNO molecule is of interest in both combustion and atmospheric chemistry. For example, Guadagnini et al. have recently presented ab initio potential energy surfaces for the three lowest lying electronic states of HNO and then used these in examining several chemical reactions that take place in the combustion of nitrogen containing fuels and in the oxidation of atmospheric nitrogen. We have previously studied the ground state potential energy surface (i.e., stationary points along the HNO rev. reaction HON path), vibrational spectrum (using an accurate quartic force field), zero-point energy, and bonding of HNO using coupled-cluster ab initio methods. HNO is also very interesting because of the unique nature of its bonding characteristics. That is, the potential energy surface is very flat along the H-N bonding coordinate thereby giving unusual harmonic and fundamental vibrational frequencies, and the H-N bond energy is rather weak in comparison to other H-N bond energies. In fact, using experimental heats of formation for HO, H, and NO, the H- bond energy is computed to be only 49.9 kcal/ mol (298 K). However, ab initio calculations of isodesmic reaction energies involving HNO, FNO, ClNO, and several other molecules have shown that there is an inconsistency in the experimental heats of formation of the XNO (X=H, F, and Cl) species. Hence the motivation for this study was to determine a very accurate(DELTA)H(sup o)(sub f) value for HNO using state of-the-art ab initio methods. Based on many recent studies it is evident that the singles and doubles coupled-cluster method that includes a perturbational estimate of the effects of connected triple excitations, denoted CCSD(T), in conjunction with large one-particle basis sets should be reliable to better than +0.8 kcal/mol for this quantity. The computational methodology is described in the next section followed by our results and discussion. Conclusions are presented in the final section.

Lee, Timothy J.↗
NASA NTRS2000

Scientific Objectives of the Mars Surveyor 2001 Gamma-Ray Spectrometer

The Gamma-Ray Spectrometer (GRS) is one of the instruments on the Mars Surveyor 2001 Orbiter, which is part of NASA's Mars-Surveyor program. The GRS is really an instrument suite consisting of the GRS, a neutron spectrometer (NS), and a high-energy neutron detector (FIEND). Each of these instruments/sensors are remotely mounted at different locations on the spacecraft and connect to a central electronics box. The GRS will achieve global mapping of the elemental composition of the surface and the abundance of hydrogen in the shallow subsurface. It is an updated design using the same technology as the lost Mars Observer mission. The Martian surface is continuously bombarded by cosmic ray particles; their interactions with the constituents of the soil produces nuclear reaction cascades with fast neutrons being the main secondaries. Those neutrons interact in turn with the nuclei of the elements that make up the soil and they eventually get slowed to thermal energies. In this process they leave the nuclei in an excited state that decays via the emission of characteristic gamma rays. All these processes are precisely known and have been simulated by means of numerical models. Thus, remote gamma-ray spectroscopy is a useful method for quantitatively measuring the geochemical composition of the surface down to a few tens of g/sq cm. Additional information is contained in original extended abstract.

Boynton, W. V.↗
NASA NTRS2007

Electron-Molecule Col1isions: Quantitative Approaches, and the Legacy of Aaron Temkin

This article, on electron-molecule collisions, is dedicated to the legacy of my good friend and sometime collaborator, Aaron Temkin on his retirement from the NASA-Goddard Space Flight Center after many years of work at the highest intellectual level in the theoretical treatment of electron-atom and electron-molecule scattering. Aaron's contributions to the manner in which we think about electron-molecule collisions is clear to all of us who have worked in this field. I doubt that the great progress that has occurred in the computational treatment of such complex collision problems could have happened without these contributions. For a brief historical account, see the discussion of Temkin's contribution to electron-molecule scattering in the first article of this volume by Dr. A. K. Bhatia. In this article, I will concentrate on the application of the so called, non-adiabatic R-matrix theory, to vibrational excitation and dissociative attachment, although I will also present some results applying the Linear Algebraic and Kohn-Variational methods to vibrational excitation. As a starting point for almost all computationally effective approaches to electron-molecule collisions, is the fixed nuclei approximation. That is, one recognizes, just as one does with molecular bound states, that there is a separation of electronic(fast) and nuclear(s1ow) degrees of freedom. This separation makes it possible to "freeze" the nuclei in space, calculate the collision parameters for the frozen molecule and then, somehow to add back the vibrations and rotations. The manner in which this is done, depends on the details of the collision problem. It is the work of Aaron and a number of other researchers that has provided the guidance necessary to resolve these issues.

Schneider, B.I.↗
DOE OSTI2020

Core excitations with excited state mean field and perturbation theory

In this work, we test the efficacy of excited state mean field theory and its excited-state-specific perturbation theory on the prediction of K-edge positions and x-ray peak separations. We find that the mean field theory is surprisingly accurate, even though it contains no accounting of differential electron correlation effects. In the perturbation theory, we test multiple core-valence separation schemes and find that, with the mean field theory already so accurate, electron-counting biases in one popular separation scheme become a dominant error when predicting K-edges. Happily, these appear to be relatively easy to correct for, leading to a perturbation theory for K-edge positions that is lower scaling and more accurate than coupled cluster theory and competitive in accuracy with recent high-accuracy results from restricted open-shell Kohn-Sham theory. For peak separations, our preliminary data show excited state mean field theory to be exceptionally accurate, but more extensive testing will be needed to see how it and its perturbation theory compare to coupled cluster peak separations more broadly.

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

Coherent photoexcitation of entangled triplet pair states

The functional properties of organic semiconductors are defined by the interplay between optically bright and dark states. Organic devices require rapid conversion between these bright and dark manifolds for maximum efficiency, and one way to achieve this is through multiexciton generation (S 1 → 1 TT). Here, the dark state 1 TT is typically generated from bright S 1 after optical excitation; however, the mechanistic details are hotly debated. Here we report a 1 TT generation pathway in which it can be coherently photoexcited, without any involvement of bright S 1 . Using <10-fs transient absorption spectroscopy and pumping sub-resonantly, 1 TT is directly generated from the ground state. Applying this method to a range of pentacene dimers and thin films of various aggregation types, we determine the critical material properties that enable this forbidden pathway. Through a strikingly simple technique, this result opens the door for new mechanistic insights into 1 TT and other dark states in organic materials.

14 SOLAR ENERGY↗
DOE OSTI2023

Self-tuning wave energy converter (WEC) controller for changing sea states

Systems and methods for a WEC controller that uses a self-tuning proportional-integral control law prescribing motor torques to maximize electrical power generation and automatically tune the controller to maximize power absorption. In an embodiment, the controller may be part of any resonant WEC system. The control law relies upon an identified model of device intrinsic impedance to generate a frequency-domain estimate of the wave-induced excitation force and measurements of device velocities. The control law was tested in irregular sea-states that evolved over hours (a rapid, but realistic time-scale) and that changed instantly (an unrealistic scenario to evaluate controller response).

Bacelli, Giorgio↗
DOE OSTI2021

Double photoionization of atomic oxygen: Feshbach resonances in the two-electron continuum

In this work, we describe a joint experimental and theoretical investigation on oxygen double photoionization—the emission of two electrons from atomic oxygen following single photon absorption. High-resolution experimental measurements were performed at the Advanced Light Source, revealing sharp resonance structure superimposed on the more familiar Wannier-like, nearly-linear background. These resonance features are attributed to ionization-plus-excitation Feshbach resonances embedded in the double ionization continuum, doubly-excited states that lie above the double-ionization threshold. Such features are absent in the double photoionization cross section of He, or other quasi-two-electron systems, for which the doubly-ionized atomic core remains inert. For a corresponding theoretical analysis, the R-matrix with pseudostates (RMPS) method was invoked by calculating final-state, two-electron resonances-plus-continua wavefunctions and corresponding single-photon absorption cross sections. Overall agreement is found in the direct, background double photoionization cross section. However, the RMPS method, using a small basis due to practical computational limitations, was unable to reproduce quantitatively the smooth background or the sharper resonance features observed in the measurements, showing instead large-scale oscillations about the experimental background, and characteristic pseudoresonance jitter, associated with an insufficient convergence of the pseudostate representation to the true two-electron infinite series of Feshbach resonances embedded in the two-electron continuum. The prominent resonance structure observed highlights the need to consider multiple excitation processes in atoms more complex than He or quasi-two-electron systems.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS2021

Synthesis and Characterization of Fe(III)-Fe(II)- Mg- Al Smectite Solid Solutions and Implications for Planetary Science

This study demonstrates the synergies and limits of multiple measurement types for the detection of smectite chemistry and oxidation state on planetary surfaces to infer past geochemical conditions. Smectite clay minerals are common products of water-rock interactions throughout the solar system, and their detection and characterization provides important clues about geochemical conditions and past environments if sufficient information about their composition can be discerned. Here, we synthesize and report on the spectroscopic properties of a suite of smectite samples that span the intermediate compositional range between Fe(II), Fe(III), Mg, and Al end-member species using bulk chemical analyses, X-ray diffraction, Vis/IR reflectance spectroscopy, UV and green-laser Raman spectroscopy, and Mössbauer spectroscopy. Our data show that smectite composition and the oxidation state of octahedral Fe can be reliably identified in the near infrared on the basis of combination and fundamental metal-OH stretching modes between 2.1–2.9 μm, which vary systematically with chemistry. Smectites dominated by Mg or Fe(III) have spectrally distinct fundamental and combination stretches, whereas Al-rich and Fe(II)-rich smectites have similar fundamental minima near 2.76 μm, but have distinct combination M-OH features between 2.24 and 2.36 μm. We show that with expanded spectral libraries that include intermediate composition smectites and both Fe(III) and Fe(II) oxidation states, more refined characterization of smectites from MIR data is now possible, as the position of the 450 cm–1 absorption shifts systematically with octahedral Fe content, although detailed analysis is best accomplished in concert with other characterization methods. Our data also provide the first Raman spectral libraries of smectite clays as a function of chemistry, and we demonstrate that Raman spectroscopy at multiple excitation wavelengths can qualitatively distinguish smectite clays of different structures and can enhance interpretation by other types of analyses. Our sample set demonstrates how X-ray diffraction can distinguish between dioctahedral and trioctahedral smectites using either the (02,11) or (06,33) peaks, but auxiliary information about chemistry and oxidation state aids in specific identifications. Finally, the temperature-dependent isomer shift and quadrupole splitting in Mössbauer data are insensitive to changes in Fe content but reliability differentiates Fe within the smectite mineral structure.

Valerie K Fox↗
DOE OSTI2023

Resolving Electron Injection from Singlet Fission-Borne Triplets into Mesoporous Transparent Conducting Oxides

Photoinduced electron transfer from a molecular chromophore into mesoporous metal oxide substrates occurs efficiently from both singlet and triplet excited states for traditional metal-to-ligand charge transfer (MLCT) dyes. All organic molecules that undergo singlet fission (SF), the process of generating two triplet excitons with photoexcitation of one singlet exciton, offers a promising method of generating two charges per one absorbed photon. However, the singlet-triplet energy balance required to drive SF often places the driving force for triplet electron injection into metal oxides too low. As such, the dynamics of singlet vs. triplet electron transfer for SF in dye-sensitized solar cell configurations has not been elucidated. Here, we use applied bias transient absorption spectroscopy to modulate the driving force for triplet electron transfer from an anthradithiophene-based SF chromophore (ADT-COOH) adsorbed to mesoporous indium tin oxide (nanoITO).

CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SU↗
DOE OSTI2023

Improved temperature dependence of rate coefficients for rotational state-to-state transitions in H 2 O + H 2 O collisions

Aims. We present an improved database of temperature-dependent rate coefficients for rotational state-to-state transitions in H 2 O + H 2 O collisions. The database includes 231 transitions between the lower para-states of H 2 O and 210 transitions between its lower ortho-states (up toj= 7) and can be employed in cometary and planetary applications up to the temperature of 1000 K. Methods. We developed and applied a new general method that allows the generation of rate coefficients for excitation and quenching processes that automatically satisfy the principle of microscopic reversibility and also helps to cover the range of low collision energies by interpolation of cross sections between the process threshold and the computed data points. Results. We find that in the range of intermediate temperatures, 150

Astronomy & Astrophysics↗
DOE OSTI2023

Lifetime measurement of excited states in 116 Xe

Lifetimes of excited states in 116 Xe were measured using the recoil-distance Doppler-shift technique. Excited 116 Xe nuclei were populated in the fusion-evaporation reaction 102 Pd( 16 O,2n) 116 Xe. Lifetimes of the $2^{+}_{1}$ and $4^{+}_{1}$ states were evaluated using the differential decay-curve method with $\gamma$-$\gamma$-coincidence data as well as lifetimes of the $6^{+}_{1}$ and $7^{-}_{1}$ states using simulations of spectra considering Doppler-shift attenuation effects.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗