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At least 559 records · Page 31
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

De Novo Synthesis of Bacteriochlorins Bearing Four Trideuteriomethyl Groups

Site-specific introduction of isotopes in tetrapyrrole macrocycles provides the foundation for probing physicochemical features germane to photosynthetic energy-transduction processes, but has chiefly been done with porphyrins rather than the more biologically relevant hydroporphyrin analogues of native photosynthetic pigments. A prior study incorporated pairwise 13C or 15N atoms in the skeleton of a bacteriochlorin containing a gem-dimethyl group in each pyrroline ring. Here, a complementary effort is reported that installs deuterium atoms in substituents at the perimeter of a bacteriochlorin. Thus, perdeuteriated 3-methyl-2,4-pentanedione was converted in an 8-step synthesis via the intermediacy of tert-butyl 5-formyl-3,4-bis(trideuteriomethyl)pyrrole-2-carboxylate to the 2,3,12,13-tetrakis(trideuteriomethyl)-8,8,18,18-tetramethylbacteriochlorin (BC-2). The fidelity of isotope substitution was maintained throughout the synthesis. Resonance Raman spectroscopy of the copper chelate (CuBC-2) revealed that addition of the four β-pyrrolic substituents alone is not sufficient to account for the vibronic complexity observed for the copper chelate of bacteriochlorophyll a (CuBChl a). The increased vibronic activity exhibited by the natural pigments and CuBChl a must arise from the increased structural complexity of the macrocycle.

Jing, Haoyu (ORCID:0000000178399582)↗
DOE OSTI2022

The Structure of Liquid and Glassy Carbamazepine

To enhance the solubility of orally administered pharmaceuticals, liquid capsules or amorphous tablets are often preferred over crystalline drug products. However, little is known regarding the variation in bonding mechanisms between pharmaceutical molecules in their different disordered forms. In this study, liquid and melt-quenched glassy carbamazepine have been studied using high energy X-ray diffraction and modeled using Empirical Potential Structure Refinement. The results show significant structural differences between the liquid and glassy states. The liquid shows a wide range of structures; from isolated molecules, to aromatic ring correlations and NH-O hydrogen bonding. Upon quenching from the liquid to the glass the number of hydrogen bonds per molecule increases by ~50% at the expense of a ~30% decrease in the close contact (non-bonded) carbon-carbon interactions between aromatic rings. During the cooling process, there is an increase in both singly and doubly hydrogen-bonded adjacent molecules. Although hydrogen-bonded dimers found in the crystalline states persist in the glassy state, the absence of a crystalline lattice also allows small, hydrogen-bonded NH-O trimers and tetramers to form. This proposed model for the structure of glassy carbamazepine is consistent with the results from vibrational spectroscopy and nuclear magnetic resonance.

Benmore, Chris J. (ORCID:0000000170077749)↗
NASA NTRS1986

Far-infrared structure in the nuclear region of M51

Far-infrared (100-micron) scans across the nucleus of M51 are presented. These scans show that much of the far-infrared luminosity of this galaxy comes from a small, sharply bounded region within a 30 arcsec radius (700 pc) of the nucleus. This radius corresponds to the innermost spiral structure, as well as that estimated from dynamical models for the radius of the inner Lindblad resonance. The results of a nonlinear image restoration analysis of the data are presented. This analysis, carried out with two different algorithms, yields information on the spatial structure of star formation near the nucleus that exceeds the diffraction limit of the telescope at this wavelength. This 'superresolution' treatment shows that star formation is enhanced at the outer edge of this region compared to the nucleus, which appears to be relatively devoid of young stars. This ring of active star formation may be produced in the same way as that seen in our own Galaxy at a galactocentric radius of 4-5 kpc and may indicate that the region near the nucleus has been swept clean of material by violent processes.

Lester, D. F.↗
NASA NTRS2014

Rotating Balances Used for Fluid Pump Testing

Marshall Space Flight Center has developed and demonstrated two direct read force and moment balances for sensing and resolving the hydrodynamic loads on rotating fluid machinery. These rotating balances consist of a series of stainless steel flexures instrumented with semiconductor type, unidirectional strain gauges arranged into six bridges, then sealed and waterproofed, for use fully submerged in degassed water at rotational speeds up to six thousand revolutions per minute. The balances are used to measure the forces and moments due to the onset and presence of cavitation or other hydrodynamic phenomena on subscale replicas of rocket engine turbomachinery, principally axial pumps (inducers) designed specifically to operate in a cavitating environment. The balances are inserted into the drive assembly with power to and signal from the sensors routed through the drive shaft and out through an air-cooled twenty-channel slip ring. High frequency data - balance forces and moments as well as extensive, flush-mounted pressures around the rotating component periphery - are acquired via a high-speed analog to digital data acquisition system while the test rig conditions are varied continuously. The data acquisition and correction process is described, including the in-situ verifications that are performed to quantify and correct for known system effects such as mechanical imbalance, "added mass," buoyancy, mechanical resonance, and electrical bias. Examples of four types of cavitation oscillations for two typical inducers are described in the laboratory (pressure) and rotating (force) frames: 1) attached, symmetric cavitation, 2) rotating cavitation, 3) attached, asymmetric cavitation, and 4) cavitation surge. Rotating and asymmetric cavitation generate a corresponding unbalanced radial force on the rotating assembly while cavitation surge generates an axial force. Attached, symmetric cavitation induces no measurable force. The frequency of the forces can be determined a priori from the pressure environment while the magnitude of the hydrodynamic force is proportional to the pressure unsteadiness.

Skelley, Stephen↗
DOE OSTI2026

The Hidden Path to the Resonance-Stabilized Fulvenallenyl Radical (C 7 H 5 ) via the Bimolecular Reaction of Tricarbon (C 3 , X 1 Σ g + ) with 1,3-Butadiene (C 4 H 6 ; X 1 A g )

Here, we report a novel bimolecular reaction pathway forming the resonance-stabilized fulvenallenyl radical (C 7 H 5 ) via the gas-phase reaction of tricarbon (C 3 , X 1 Σ g + ) with 1,3-butadiene (C 4 H 6 , X 1 A g ). Crossed molecular beam experiments combined with high-level electronic structures and statistical calculations reveal a rich potential energy surface. The reaction proceeds via tricarbon addition to a double bond of 1,3-butadiene, overcoming a 30 kJ mol –1 barrier, followed by ring closure, isomerizations (ring opening/closures, hydrogen shifts), and eventual hydrogen atom loss, yielding the fulvenallenyl radical (p1) almost exclusively via two dominant pathways. Considering the entrance barrier, this reaction may occur in high-temperature environments, like circumstellar envelopes of carbon stars, but is suppressed in colder regions such as molecular clouds and Titan’s atmosphere. These findings highlight the unexpected reactivity of small carbon clusters in shaping the molecular complexity of our universe, from the flicker of a flame to the death of a star.

Aromatic compounds↗
DOE OSTI2023

Ultrafast snapshots of terahertz electric potentials across ring-shaped quantum barriers

Probing the time evolution of the terahertz electric field within subwavelength dimensions plays a crucial role in observing the nanoscale lightwave interactions with fundamental excitations in condensed-matter systems and in artificial structures, such as metamaterials. Here, we propose a novel probing method for measuring terahertz electric potentials across nanogaps using a combination of optical and terahertz pulse excitations. To achieve this, we employ ring-shaped nanogaps that enclose a metallic island, allowing us to capture tunneling charges when subjected to terahertz electromagnetic pulse illumination. By controlling and manipulating the terahertz tunneling charges through a focused optical gate pulse, we can obtain the terahertz potential strength as a function of spatial coordinates and time delays between pulses. To accurately quantify the time evolution of terahertz electric potential across quantum barriers, we carefully calibrate the recorded nonlinear tunneling current. Its on-resonance and off-resonance behaviors are also discussed, providing valuable insights into the antenna’s characteristics and performance.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1992

Plasma wave observations at Neptune

Phenomena detected by the plasma wave instrument during the Voyager 2 flyby of Neptune are reviewed. Particular attention given to radio emissions, electron plasma oscillations in the solar wind upstream of the bow shock, electrostatic electron cyclotron waves and upper hybrid resonance (UHR) waves, whistler mode noise, and dust impacts. The radio emissions which occur in a broad range of about 5 to 50 kHz are considered to be generated by mode conversion from UHR waves at the magnetic equator. The inner magnetosphere has relatively low plasma wave intensities (less than 100 microV/m). Many small micron-sized dust particles which were detected striking the spacecraft had the maximum impact rate of about 280 impacts per sec at the bound ring plane crossing, and about 110 impacts per sec at the outbound ring plane crossing. Most of the particles were concentrated in a dense disk, about one thousand km thick, near the equatorial plane.

Gurnett, D. A.↗
NASA NTRS1994

Thermodynamic effect of the ion sound instability in the ionosphere

During geomagnetic disturbances when the ring current interacts intensely with the plasmasphere, the plasma of this region undergoes a strong heating due to an ion cyclotron instability. This is followed by the transfer of heat along geomagnetic field lines from the heating region to the ionosphere. One of the results of this process is the formation of non-isothermal region (in which T(sub e) greater than 3.4 T(sub i) at ionospheric heights) caused by a rapid cooling the H(+) ions due to their resonant charge exchange with neutral hydrogen. Heat transfer from the top of the flux tube to the ionosphere is investigated using a hydrodynamic model for the ionosphere-plasmasphere coupling. Field-aligned currents, present in the topside ionosphere, are often accompanied by ion sound turbulence. The turbulence scatters electrons, increasing the total electron collision frequency through wave-particle effects. The influence of wave-particle interactions introduces an anomalous component to the total collision frequency, which modifies substantially the heat conduction coefficient of the plasma. As a result, the plasma is heated more intensely above than below this region of ion sound turbulence.

Khazanov, G. V.↗
NASA NTRS1975

Measurements of selected psi /3684/ branching ratios from a study of secondary lepton pairs

The measurements considered were made at the electron-positron storage ring at the Stanford Linear Accelerator Center. The apparatus used consists of two identical spectrometers mounted in a collinear configuration about the beam-interaction region. The energies of secondary electrons or positrons are measured with good resolution in large NaI(Tl) total-absorption detectors. Data accumulated without gamma-ray converters were examined for electron-positron pairs. The data taken with gamma-ray converters in place and at center-of-mass energies within 1 MeV of the resonance energy were scanned for evidence of either charged particles or converted gamma rays accompanying the detected muon pairs.

Hilger, E.↗
NASA NTRS2017

High-Resolution IR Absorption Spectroscopy of Polycyclic Aromatic Hydrocarbons in the 3-micrometers Region: Role of Periphery

In this work we report on high-resolution IR absorption studies that provide a detailed view on how the peripheral structure of irregular polycyclic aromatic hydrocarbons (PAHs) affects the shape and position of their 3-micrometers absorption band. To this purpose we present mass-selected, high-resolution absorption spectra of cold and isolated phenanthrene, pyrene, benz[a]antracene, chrysene, triphenylene, and perylene molecules in the 2950-3150 per cm range. The experimental spectra are compared with standard harmonic calculations, and anharmonic calculations using a modified version of the SPECTRO program that incorporates a Fermi resonance treatment utilizing intensity redistribution. We show that the 3-micrometers region is dominated by the effects of anharmonicity, resulting in many more bands than would have been expected in a purely harmonic approximation. Importantly, we find that anharmonic spectra as calculated by SPECTRO are in good agreement with the experimental spectra. Together with previously reported high-resolution spectra of linear acenes, the present spectra provide us with an extensive dataset of spectra of PAHs with a varying number of aromatic rings, with geometries that range from open to highly-condensed structures, and featuring CH groups in all possible edge configurations. We discuss the astrophysical implications of the comparison of these spectra on the interpretation of the appearance of the aromatic infrared 3-micrometers band, and on features such as the two-component emission character of this band and the 3-micrometers emission plateau.

techniques: spectroscopic↗
DOE OSTI2021

Formation of Benzene and Naphthalene through Cyclopentadienyl-Mediated Radical–Radical Reactions

Resonantly stabilized free radicals (RSFRs) have been contemplated as fundamental molecular building blocks and reactive intermediates in molecular mass growth processes leading to polycyclic aromatic hydrocarbons (PAHs) and carbonaceous nanoparticles on Earth and in deep space. Here, by combining molecular beams and computational fluid dynamics simulations, we provide compelling evidence on the formation of benzene via the cyclopentadienyl-methyl reaction and of naphthalene through the cyclopentadienyl self-reaction, respectively. These systems offer benchmarks for the conversion of a five-membered ring to the 6π-aromatic (benzene) and the generation of the simplest 10π-PAH (naphthalene) at elevated temperatures. These results uncover molecular mass growth processes from the “bottom up” via RSFRs in high temperature circumstellar environments and combustion systems expanding our fundamental knowledge of the organic, hydrocarbon chemistry in our universe.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1986

1985 Nuclear Science Symposium, 32nd, and 1985 Symposium on Nuclear Power Systems, 17th, San Francisco, CA, October 23-25, 1985, Proceedings

The present conference ranges over topics in high energy physics instrumentation, detectors, nuclear medical applications, health physics and environmental monitoring, reactor instrumentation, nuclear spacecraft instrumentation, the 'Fastbus' data acquisition system, circuits and systems for nuclear research facilities, and the development status of nuclear power systems. Specific attention is given to CCD high precision detectors, a drift chamber preamplifier, a Cerenkov ring imaging detector, novel scintillation glasses and scintillating fibers, a modular multidrift vertex detector, radial wire drift chambers, liquid argon polarimeters, a multianode photomultiplier, the reliability of planar silicon detectors, the design and manufacture of wedge and strip anodes, ultrafast triode photodetectors, photomultiplier tubes, a barium fluoride plastic scintillator, a fine grained neutron hodoscope, the stability of low leakage silicon photodiodes for crystal calorimeters, and X-ray proportional counters. Also considered are positron emission tomography, single photon emission computed tomography, nuclear magnetic resonance imaging, Geiger-Muller detectors, nuclear plant safeguards, a 32-bit Fastbus computer, an advanced light water reactor, and nuclear plant maintenance.

Source record↗
DOE OSTI2023

Multiquanta flux jumps in superconducting fractal

We study the magnetic field response of millimeter scale fractal Sierpinski gaskets (SG) assembled of superconducting equilateral triangular patches. Directly imaged quantitative induction maps reveal hierarchical periodic filling of enclosed void areas with multiquanta magnetic flux, which jumps inside the voids in repeating bundles of individual flux quanta Φ 0 . The number N s of entering flux quanta in different triangular voids of the SG is proportional to the linear size s of the void, while the field periodicity of flux jumps varies as 1/s. We explain this behavior by modeling the triangular voids in the SG with effective superconducting rings and by calculating their response following the London analysis of persistent currents, J s , induced by the applied field H a and by the entering flux. With changing H a , J s reaches a critical value in the vertex joints that connect the triangular superconducting patches and allows the giant flux jumps into the SG voids through phase slips or multiple Abrikosov vortex transfer across the vertices. The unique flux behavior in superconducting SG patterns, may be used to design tunable low-loss resonators with multi-line high-frequency spectrum for microwave technologies.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Highly Robust and Efficient Blechert-Type Cyclic(alkyl)(amino)carbene Ruthenium Complexes for Olefin Metathesis

The first Blechert-type ruthenium complexes containing cyclic(alkyl)(amino)carbene (CAAC) ligands are reported. Furthermore, these catalysts demonstrate remarkable thermal stability in solution and excellent catalytic performances at low catalytic loading (up to 0.005 mol%) in ring-closing metathesis (RCM), macro-RCM, ring-closing enyne metathesis (RCEYM), cross-metathesis (CM), ethenolysis and ring-opening cross metathesis (ROCM). Moreover, up to 95% ee was obtained in asymmetric ring-opening cross metathesis (AROCM) and 57% ee asymmetric cross-metathesis (ACM)

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1997

Reversal in Spreading of a Tabbed Circular Jet Under Controlled Excitation

Detailed flow field measurements have been carried out for a turbulent circular jet perturbed by tabs and artificial excitation. Two "delta tabs" were placed at the nozzle exit at diametrically opposite locations. The excitation condition involved subharmonic resonance that manifested in a periodic vortex pairing in the near flow field. While the excitation and the tabs independently increased jet spreading, a combination of the two diminished the effect. The jet spreading was most pronounced with the tabs but was reduced when excitation was applied to the tabbed jet. The tabs generated streamwise vortex pairs that caused a lateral spreading of the jet in a direction perpendicular to the plane containing the tabs. The excitation, on the other band, organized the azimuthal vorticity into coherent ring structures whose evolution and pairing also increased entrainment by the jet. In the tabbed case, the excitation produced coherent azimuthal structures that were distorted and asymmetric in shape. The self-induction of these structures produced an effect that opposed the tendency for the lateral spreading of the streamwise vortex pairs. The passage of the distorted vortices, and their pairing, also had a cancellation effect on the time-averaged streamwise vorticity field. These led to the reduction in jet spreading.

Zaman, K. B. M. Q.↗
NASA NTRS1997

Reversal in Spreading of a Tabbed Circular Jet Under Controlled Excitation

Detailed flow field measurements have been carried out for a turbulent circular jet perturbed by tabs and artificial excitation. Two "delta tabs" were placed at the nozzle exit at diametricall opposite y locations. The excitation condition involved subharmonic resonance that manifested in a periodic vortex pairing in the near flow field. While the excitation and the tabs independently increased jet spreading, a combination of the two diminished the effect. The jet spreading was most pronounced with the tabs but was reduced when excitation was applied to the tabbed jet. The tabs generated streamwise vortex pairs that caused a lateral spreading of the jet in a direction perpendicular to the plane containing the tabs. ne excitation, on the other hand, organized the azimuthal vorticity into coherent ring structures whose evolution and pairing also increased entrainment by the jet. In the tabbed case, the excitation produced coherent azimuthal structures that were distorted and asymmetric in shape. The self-induction of these structures produced an effect that opposed the tendency for the lateral spreading of the streamwise vortex pairs. The passage of the distorted vortices, and their pairing, also had a cancellation effect on the time-averaged streamwise vorticity field. These led to the reduction in jet spreading.

Zaman, K. B. M. Q.↗
NASA NTRS2006

Self-Consistent Model of Magnetospheric Ring Current and Propagating Electromagnetic Ion Cyclotron Waves: Waves in Multi Ion Magnetosphere - 1

The further development of a self-consistent theoretical model of interacting ring current ions and electromagnetic ion cyclotron waves [Khazanov et al., 2003] is presented. In order to adequately take into account the wave propagation and refraction in a multi-ion plasmasphere, we explicitly include the ray tracing equations in our previous self-consistent model and use the general form of the wave kinetic equation. This is a major new feature of the present model and, to the best of our knowledge, the ray tracing equations for the first time are explicitly employed on a global magnetospheric scale in order to self-consistently simulate spatial, temporal, and spectral evolutions of the ring current and electromagnetic ion cyclotron waves. To demonstrate the effects of EMIC wave propagation and refraction on the EMIC wave energy distributions and evolution we simulate the May 1998 storm. The main findings of our simulation can be summarized as follows. First, due to the density gradient at the plasmapause, the net wave refraction is suppressed, and He(+)-mode grows preferably at plasmapause. This result is in a total agreement with the previous ray tracing studies, and very clear observed in presented B-field spectrograms. Second, comparison the global wave distributions with the results from other ring current model [Kozyra et al., 1997] reveals that our model provides more intense and higher plasmapause organized distributions during the May, 1998 storm period. Finally, the found He(+)-mode energy distributions are not Gaussian distributions, and most important that wave energy can occupy not only the region of generation, i. e. the region of small wave normal angles, but the entire wave normal angle region and even only the region near 90 degrees. The latter is extremely crucial for energy transfer to thermal plasmaspheric electrons by resonant Landau damping, and subsequent downward heat transport and excitation of stable auroral red arcs.

Khazanov, G. V.↗
NASA NTRS2006

Self-Consistent Model of Magnetospheric Ring Current and Propagating Electromagnetic Ion Cyclotron Waves: Waves, Precipitating Ring Current Ions, and Thermal Electron Heating - 2

This paper is dedicated to further presentations and discussions of the results from our new global self-consistent theoretical model of interacting ring current ions and electromagnetic ion cyclotron waves [Khazanov et al., 2006; here referred to as Paper 1]. In order to adequately take into account the wave propagation and refraction in a multi-ion plasmasphere, we explicitly include the ray tracing equations in our previous self-consistent model and use the general form of the wave kinetic equation [for details see Paper 1]. To demonstrate the effects of the EMIC wave propagation and refraction on the RC proton precipitations and heating of the thermal plasmaspheric electrons we simulate the May 1998 storm. The main findings of our simulation can be summarized as follows. Firstly, the wave induced precipitations have a quite fine structure, and are highly organized by location of the plasmapause gradient. The strongest fluxes of about 4 (raised dot) 10(exp 6) [(cm (raised dot) s (raised dot) sr)(sup -l)] are observed during the main and early recovery phases of the storm. The very interesting and probably more important finding is that in a number of cases the most intense precipitating fluxes are not simply connected to the most intense EMIC waves. The character of the EMIC wave power spectral density distribution over the equatorial wave normal angle is an extremely crucial for the effectiveness of the RC ion scattering. Secondly, comparison of the global proton precipitating patterns with the results from other ring current model [Kozyra et al., 1997] reveals that although we observe a qualitative agreement between localizations of the wave induced fluxes in the models, there is no quantitative agreement between the magnitudes of these fluxes. These differences are mainly due to a qualitative difference between the characters of the EMIC wave power spectral density distributions over the equatorial wave normal angle. Finally, the two energy sources to the plasmaspheric electrons are considered; (i) the heat fluxes caused by the EMIC wave energy absorption due to Landau resonance, and (ii) the heat fluxes due to Coulomb energy degradation of the RC o(+) ions. The heat fluxes caused by the EMIC wave energy absorption due to Landau resonance are observed in the postnoon-premidnight MLT sector, and maximize at the magnitude of 10l1 (eV/(cm(sup 2)(raised dot) s) at L=3.25, MLT=22 at 3400 UT after 1 May, 0000 UT. The greatest Coulomb energy deposition rates are about 2 (raised dot) 10(sup 10)(eV/(cm(sup 2)(raised dot) s) and observed during two periods; 32-48 hours, and 76-86 hours after 1 May, 0000 UT. The theoretically derived spatial structure of the thermal electron heating caused by interaction of the RC with plasmasphere is strongly supported by concurrent and conjugate plasma measurements from the plasmasphere, the RC, and the topside ionosphere [Gurgiolo et al., 20051.

Khazanov, G. V.↗