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NASA NTRS2014

Magnetite as Possible Template for the Synthesis of Chiral Organics in Carbonaceous Chondrites

The main goal of the Japanese Aerospace Ex-ploration Agency (JAXA) Hayabusa-2 mission is to visit and return to Earth samples of a C-type asteroid (162173) 1999 JU3 in order to understand the origin and nature of organic materials in the Solar System. Life on Earth shows preference towards the set of organics with particular spatial arrangements, this 'selectivity' is a crucial criterion for life. With only rare exceptions, life 'determines' to use the left- (L-) form over the right- (D-) form of amino acids, resulting in a L-enantiomeric excess (ee). Recent studies have shown that L-ee is found within the alpha-methyl amino acids in meteorites [1, 2], which are amino acids with rare terrestrial occurrence, and thus point towards a plausible abiotic origin for ee. One of the proposed origins of chiral asymmetry of amino acids in meteorites is their formation with the presence of asymmetric catalysts [3]. The catalytic mineral grains acted as a surface at which nebular gases (CO, H2 and NH3) were allowed to condense and react through Fisher Tropsch type (FTT) syntheses to form the organics observed in meteorites [4]. Magnetite is shown to be an effective catalyst of the synthesis of amino acids that are commonly found in meteorites [5]. It has also taken the form as spiral magnetites (a.k.a. 'plaquettes'), which were found in various carbonaceous chondrites (CCs), including C2s Tagish Lake and Esseibi, CI Orgueil, and CR chondrites [e.g., 6, 7, 8]. In addition, L-ee for amino acids are common in the aqueously altered CCs, as opposed to the unaltered CCs [1]. It seems possible that the synthesis of amino acids with chiral preferences is correlated to the alteration process experienced by the asteroid parent body, and related to the configuration of spiral magnetite catalysts. Since C-type asteroids are considered to be enriched in organic matter, and the spectral data of 1999 JU3 indicates a certain de-gree of aqueous alteration [9], the Hayabusa-2 mission serves as a perfect chance to attest this argument. In order to understand the distribution of spiral magnetites among different meteorite classes, as well as to investigate their spiral configurations and correlation to molecular asymmetry, we observed polished thin sections of CCs using scanning electron microscope (SEM) imaging. Individual magnetite grains were picked, embedded in epoxy, thin-sectioned using an ultra-microtome, and studied with electron backscatter diffraction (EBSD) in order to reconstruct the crystal orientation along the stack of magnetite disks.

Chan, Q. H. S.↗

NASA NTRS2004

Structure and Dynamics of Freely Suspended Liquid Crystals

Smectic liquid crystals are phases of rod shaped molecules organized into one dimensionally (1 D) periodic arrays of layers, each layer being between one and two molecular lengths thick. In the least ordered smectic phases, the smectics A and C, each layer is a two dimensional (2D) liquid. Additionally there are a variety of more ordered smectic phases having hexatic short range translational order or 2D crystalline or quasi long range translational order within the layers. The inherent fluid-layer structure and low vapor pressure of smectic liquid crystals enables the long term stabilization of freely suspended, single component, layered fluid films as thin as 30A, a single molecular layer. The layering forces the films to be an integral number of smectic layers thick, quantizing their thickness in layer units and forcing a film of a particular number of layers to be physically homogeneous with respect to its layer structure over its entire area. Optical reflectivity enables the precise determination of the number of layers. These ultrathin freely suspended liquid crystal films are structures of fundamental interest in condensed matter and fluid physics. They are the thinnest known stable fluid structures and have the largest surface-to-volume ratio of any stable fluid preparation, making them ideal for the study of the effects of reduced dimensionality on phase behavior and on fluctuation and interface phenomena. Their low vapor pressure and quantized thickness enable the effective use of microgravity to extend the study of basic capillary phenomena to ultrathin fluid films. Freely suspended films have been a wellspring of new LC physics. They have been used to provide unique experimental conditions for the study of condensed phase transitions in two dimensions. They are the only system in which the hexatic has been unambiguously identified as a phase of matter, and the only physical system in which fluctuations of a 2D XY system and Kosterlitz Thouless phase transition has been observed and 2D XY quasi long range order verified. Smectic films have enabled the precise determination of smectic layer electron density and positional fluctuation profiles and have been used to show that the interlayer interactions in antiferroelectric tilted smectics do not extend significantly beyond nearest neighbors. Freely suspended films played a pivotal role in the recent discovery of macroscopic chiral-polar ordering in fluids of achiral molecules. The interactions which are operative in liquid crystals are generally weak in comparison to those in crystalline phases, leading to the facile manipulation of the order in liquid crystals by external agents such as applied fields and surfaces. Effects arising from weak ordering are significantly enhanced in ultrathin free films and filaments, in which the intermolecular coupling is effectively further reduced by loss of neighbors. Over the past four years this research, which we now detail, has produced a host of exciting new discoveries and unexpected results, maintaining the study of freely suspended liquid crystal structures as one of most exciting and fruitful areas of complex fluid physics. In addition, a class of experiments on the behavior of 1D interfaces in 2D films have been pursued with results that point to potentially quite interesting effects in microgravity.

Clark, Noel A.↗

NASA NTRS1984

On the stereoselective aminoacylation of RNA

Gabbay and Kleinman (1970) have found that stereospecific complex formation (noncovalent) occurs between nucleic acids and a number of derivatives of amino acids. However, until recently, chiral selection in any nonenzymatic RNA-aminoacylation reaction was unknown. Profy and Usher (1984) reported that aminoacylation of the 'internal' 2-prime-ester occurred with a significant amount of stereoselection. Profy and Usher (1984) have also observed that aminoacylation of the 'internal' 2-prime-hydroxyl groups of polyribonucleotides by the imidazolide of N-3,5-dinitrobenzoylalanine occurs with chiral selection. In order to obtain further information regarding the considered phenomena, a systematic investigation was initiated of the factors which contribute to the observed stereoselectivity of the aminoacylation reaction. In the present paper, the effect of a change in the amino acid from alanine to leucine is considered along with an investigation of the D- and L-alanyl internal' 2-prime esters of the dinucleoside monophosphate of 3-prime,5-prime-ApA.

Usher, D. A.↗

NASA NTRS1999

Electro-mechanical Properties of Carbon Nanotubes: Effect of Small Tensile and Torsional Strains

We present a simple picture to calculate the bandgap ($E_g$) of carbon nanotubes (CNT) in the presence of uniform torsional and tensile strain ($\sigma$). We find that under tensile strain, $ absolute value of dE_g/d\sigma$ of zig-zag tubes is approximately equal to $3t_0$, where $t_0$ is the hopping parameter. Further, $ absolute value of dE_g/d\sigma$ decreases as the chirality changes to armchair, where it takes the value zero. The sign of $dE_g/d\sigma$ follows the $(N_x-N_y) *mod 3$(equal to - 1, 0 and +1) rule. In contrast to the above, we show that under torsional strain, $absolute value of dE_g/d\sigma$ of armchair tubes is approximately equal to $3t_0$ and continually decreases as the chirality changes to zig-zag, where is takes a small value. The sign of $dE_g/d\sigma$ again follows the $(N_x-N_y)*mod 3$ rule. Finally, we predict a change in the sign of $dE_g/d\sigma$ as function of strain, corresponding to a change in the value of $q$ that corresponds to the bandgap minimum.

Anantram, M. P.↗

NASA NTRS1973

Experiments on the origin of molecular chirality by parity non-conservation during beta-decay

Experiments are described to test a theory for the origin of optical activity wherein the longitudinally polarized electrons resulting from parity violation during radioactive beta decay, and their resulting circularly polarized Bremsstrahlung, might interact asymmetrically with organic matter to yield optically active products. Experiments involve subjecting a number of racemic and optically active amino acid samples to irradiation in a 61700 Ci90SR-90Y beta radiation source for a period of 1.34 years, then examining them for any asymmetric effects by means of optical rotatory dispersion and analytical gas chromatography. In the cases of D,L-leucine, norleucine, norvaline and proline as solids, of D,L-leucine in solution and of D,L-tyrosine in alkaline solution no optical rotation was observed during CRD measurements in the 250-630 nm spectral region. While slight differences were noted in the percent radiolysis of solid D- (12.7%) and L-leucine (16.2%) as determined by GC, no enrichment of either enantiomer was found.

Bonner, W. A.↗

NASA NTRS1974

Experiments on the origin of molecular chirality by parity non-conservation during beta-decay

Bonner, W. A.↗

NASA NTRS1989

Observational physics of mirror world

The existence of the whole world of shadow particles, interacting with each other and having no mutual interactions with ordinary particles except gravity is a specific feature of modern superstring models, being considered as models of the theory of everything. The presence of shadow particles is the necessary condition in the superstring models, providing compensation of the asymmetry of left and right chirality states of ordinary particles. If compactification of additional dimensions retains the symmetry of left and right states, shadow world turns to be the mirror one, with particles and fields having properties strictly symmetrical to the ones of corresponding ordinary particles and fields. Owing to the strict symmetry of physical laws for ordinary and mirror particles, the analysis of cosmological evolution of mirror matter provides rather definite conclusions on possible effects of mirror particles in the universe. A general qualitative discussion of possible astronomical impact of mirror matter is given, in order to make as wide as possible astronomical observational searches for the effects of mirror world, being the unique way to test the existence of mirror partners of ordinary particles in the Nature.

Khlopov, M. YA.↗

NASA NTRS1992

The Prebiotic Synthesis of Ethylenediamine Monoacetic Acid, The Repeating Unit of Peptide Nucleic Acids

The polymerization of ribonucleic acids or their precursors constitutes an important event in prebiotic chemistry. The various problems using ribonucleotides to make RNA suggest that there may have been a precursor. An attractive possibility are the peptide nucleic acids (PNA). PNAs are nucleotide analogs that make use of a polymer of ethylenediamine monoacetic acid (EDMA or 2-amninoethyl glycine) with the bases attached by an acetic acid. EDMA is an especially attractive alternative to the ribose phosphate or deoxyribose phosphate backbone because it contains no chiral centers and is potentially prebiotic, but there is no reported prebiotic synthesis. We have synthesized both EDMA and ethylenediamine diacetic acid (EDDA) from the prebiotic compounds ethylenediamine, formaldehyde, and hydrogen cyanide. The yields of EDMA range from 11 to 79% along with some sEDDA and uEDDA. These reactions work with concentrations of 10(exp -1)M and as low as 10(exp -4)M, and the reaction is likely to be effective at even lower concentrations. Ethylenediamine is a likely prebiotic compound, but it has not yet been demonstrated, although compounds such as ethanolamine and cysteamine have been proven to be prebiotic. Under neutral pH and heating at l00 C, EDMA is converted to the lactam, monoketopiperazine (MKP). The cyclization occurs and has an approximate ratio of MKP/EDMA = 3 at equilibrium. We have measured the solubilities of EDMA center dot H20 as 6.4 m, EDMA center dot HCl center dot H20 as 13.7 m, and EDMA center dot 2HCl center dot H20 as 3.4 m. These syntheses together with the high solubility of EDMA suggest that EDMA would concentrate in drying lagoons and might efficiently form polymers. Given the instability of ribose and the poor polymerizability of nucleotides, the prebiotic presence of EDMA and the possibility of its polymerization raises the possibility that PNAs are the progenitors of present day nucleic acids. A pre-RNA world may have existed in which PNAs or polymers with related peptide backbones were the dominant information macromolecules.

Nelson, Kevin E.↗

NASA NTRS1995

Vertical bloch line memory

A new read gate design for the vertical Bloch line (VBL) memory is disclosed which offers larger operating margin than the existing read gate designs. In the existing read gate designs, a current is applied to all the stripes. The stripes that contain a VBL pair are chopped, while the stripes that do not contain a VBL pair are not chopped. The information is then detected by inspecting the presence or absence of the bubble. The margin of the chopping current amplitude is very small, and sometimes non-existent. A new method of reading Vertical Bloch Line memory is also disclosed. Instead of using the wall chirality to separate the two binary states, the spatial deflection of the stripe head is used. Also disclosed herein is a compact memory which uses vertical Bloch line (VBL) memory technology for providing data storage. A three-dimensional arrangement in the form of stacks of VBL memory layers is used to achieve high volumetric storage density. High data transfer rate is achieved by operating all the layers in parallel. Using Hall effect sensing, and optical sensing via the Faraday effect to access the data from within the three-dimensional packages, an even higher data transfer rate can be achieved due to parallel operation within each layer.

Katti, Romney R.↗

NASA NTRS1995

ISSOL Meeting, Barcelona, Spain, 1993

Topics in a conference on the origins of life and the evolution of the biosphere include the origin of chirality, prebiotic chemistry of small biomolecules, primitive polymer formation, RNA regulation and control. Early origins of life and the ecology of hydrothermal systems such as ocean floor vents and their simple organisms are examined. The process of mineral catalysis in Montmorillonite as a model for early metabolism is used. The origin of the genetic code and the development of branching in molecular structures of amino acids is described. Studies are reported of the effects of meteorite impact on early Earth life.

Ferris, James P.↗

NASA NTRS1994

Helicity charging and eruption of magnetic flux from the Sun

The ejection of helical toroidal fields from the solar atmosphere and their detection in interplanetary space are described. The discovery that solar magnetic fields are twisted and that they are segregated by hemisphere according to their chirality has important implications for the escape process. The roles played by erupting prominences, coronal mass ejections (CME's) and active region (AR) loops in expressing the escape of magnetic flux and helicity are discussed. Sporadic flux escape associated with filament eruptions accounts for less than one-tenth the flux loss. Azimuthal flux loss by CME's could account for more, but the major contributor to flux escape may be AR loop expansion. It is shown how the transfer of magnetic helicity from the sun's interior into emerged loops ('helicity charging') could be the effective driver of solar eruptions and of flux loss from the sun.

Rust, David M.↗

NASA NTRS2004

Kinematic Treatment of CME Evolution in the Solar Wind

We present a kinematic study of the evolution of coronal mass ejections (CMEs) in the solar wind. Specifically, we consider the effects of: (1) spherical expansion; and (2) uniform expansion due to pressure gradients between the Interplanetary CME (ICME) and the ambient solar wind. We compare these results with an MHD model, which allows us to isolate these effects from the combined kinematic and dynamical effects, which are included in MHD models. They also provide compelling evidence that the fundamental cross section of so-called "force-free" flux ropes (or magnetic clouds) is neither circular or elliptical, but rather a convex-outward, "pancake" shape. We apply a force-free fitting to the magnetic vectors from the MHD simulation to assess how the distortion of the flux rope affects the fitting. In spite of these limitations, force-free fittings, which are straightforward to apply, do provide an important description of a number of parameters, including the radial dimension, orientation and chirality of the ICME.

Riley, Pete↗

NASA NTRS2004

KINEMATIC TREATMENT OF CORONAL MASS EJECTION EVOLUTION IN THE SOLAR WIND

We present a kinematic study of the evolution of coronal mass ejections (CMEs) in the solar wind. Specifically, we consider the effects of (1) spherical expansion and (2) uniform expansion due to pressure gradients between the interplanetary CME (ICME) and the ambient solar wind. We compare these results with an MHD model that allows us to isolate these effects h m the combined kinematic and dynamical effects, which are included in MHD models. They also provide compelling evidence that the fundamental cross section of so-called "force-free" flux ropes (or magnetic clouds) is neither circular or elliptical, but rather a convex-outward, "pancake" shape. We apply a force-free fit to the magnetic vectors from the MHD simulation to assess how the distortion of the flux rope affects the fit. In spite of these limitations, force-free fits, which are straightforward to apply, do provide an important description of a number of parameters, including the radial dimension, orientation, and chirality of the ICME. Subject headings: MHD - solar wind - Sun: activity - Sun: corona - Sun: coronal mass ejections (CMEs) - On-line material color figures Sun: magnetic fields

Riley, Pete↗

NASA NTRS2001

Which nanowire couples better electrically to a metal contact: Armchair or zigzag nanotube?

The fundamental question of how chirality affects tile electronic coupling of a nanotube to metal contacts is important for tile application of nanotubes as nanowires. We show that metallic-zigzag nanotubes are superior to armchair nanotubes as nanowires, by modeling the metal-nanotube interface. More specifically, we show that as a function of coupling strength, the total electron transmission of armchair nanotubes increases and tends to be pinned close to unity for a metal with Fermi wave vector close to that of gold. In contrast, the transmission probability of zigzag nanotubes increases to the maximum possible value of two. The origin of these effects lies in the details of the wave function, which is explained.

Anantram, M. P.↗

NASA NTRS2009

Control of the Diameter and Chiral Angle Distributions during Production of Single-Wall Carbon Nanotubes

Many applications of single wall carbon nanotubes (SWCNT), especially in microelectronics, will benefit from use of certain (n,m) nanotube types (metallic, small gap semiconductor, etc.) Especially fascinating is the possibility of quantum conductors that require metallic armchair nanotubes. However, as produced SWCNT samples are polydisperse, with many (n,m) types present and typical approx.1:2 metal/semiconductor ratio. Nanotube nucleation models predict that armchair nuclei are energetically preferential due to formation of partial triple bonds along the armchair edge. However, nuclei can not reach any meaningful thermal equilibrium in a rapidly expanding and cooling plume of carbon clusters, leading to polydispersity. In the present work, SWCNTs were produced by a pulsed laser vaporization (PLV) technique. The carbon vapor plume cooling rate was either increased by change in the oven temperature (expansion into colder gas), or decreased via "warm-up" with a laser pulse at the moment of nucleation. The effect of oven temperature and "warm-up" on nanotube type population was studied via photoluminescence, UV-Vis-NIR absorption and Raman spectroscopy. It was found that reduced temperatures leads to smaller average diameters, progressively narrower diameter distributions, and some preference toward armchair structures. "Warm-up" shifts nanotube population towards arm-chair structures as well, but the effect is small. Possible improvement of the "warm-up" approach to produce armchair SWCNTs will be discussed. These results demonstrate that PLV production technique can provide at least partial control over the nanotube (n,m) population. In addition, these results have implications for the understanding the nanotube nucleation mechanism in the laser oven.

Nikolaev, Pavel↗

NASA NTRSDate not supplied

Does Chirality Influence the Stability of Amino Acid –Cu Complexes in the Salt-Induced Peptide Formation Reaction? Insights from Density Functional Theory Calculations

The polymerization of amino acids into peptides and ultimately proteins is critical to evolution of life. Ribosomally-synthesized proteins are homochiral, composed entirely of L-amino acids. Abiotic syntheses of amino acids, however, produce racemic mixtures(equal amounts of L and D enantiomers), meaning that the pool of monomers available for abiotic protein synthesis would be racemic or nearly so. There are no prebiotically plausible mechanisms known to yield homochiral peptides from racemic pools of amino acids. While some mechanisms capable of producing or amplifying enantiomeric excesses have been observed, these excesses are small or not applicable to all biologically relevant amino acids. As a result, a prebiotically-feasible mechanism to create enantiopure pools of amino acids has not been identified. However, it is not clear that these enantio-enriched or enantiopure pools are necessary to produce homochiral peptides. Steric and electronic effects, or a combination of both, may influence how different enantiomers interact with each other, potentially leading to homochiral peptides from racemic mixtures. Here, we use density functional theory (DFT) calculations to assess the stability of homochiral and heterochiral reactive complexes produced during polymerization via the salt-induced peptide formation (SIPF) reaction. Experimental studies of the SIPF reaction have shown that it enables the formation of peptides under diverse environmental conditions, making it a plausible pathway to peptide formation on early Earth. In the SIPF reaction, NaCl acts as a condensation reagent while a divalent metal cation, primarily Cu2+, facilitates polymerization by complexing and activating amino acids forming a monochlorocuprate complex. To assess if hetero-or homochiral monochlorocuprate complexes were energetically favored, we compared the stability of LL, DD, and LD enantiomers of Cu2+–(alanine)2and Cu2+–(valine) 2 complexes. Gaussian 09 density DFT energy-minimization calculations were made for each Cu –amino acid complex in the cis and trans configuration. Models were energy minimized using the BH and HLYP/6-31++G(d,p) level of theory and free energies were compared to determine the most stable configuration.

A C Fox↗

NASA NTRS2009

Methods Reduce Cost, Enhance Quality of Nanotubes

For all the challenges posed by the microgravity conditions of space, weight is actually one of the more significant problems NASA faces in the development of the next generation of U.S. space vehicles. For the Agency s Constellation Program, engineers at NASA centers are designing and testing new vessels as safe, practical, and cost-effective means of space travel following the eventual retirement of the space shuttle. Program components like the Orion Crew Exploration Vehicle, intended to carry astronauts to the International Space Station and the Moon, must be designed to specific weight requirements to manage fuel consumption and match launch rocket capabilities; Orion s gross liftoff weight target is about 63,789 pounds. Future space vehicles will require even greater attention to lightweight construction to help conserve fuel for long-range missions to Mars and beyond. In order to reduce spacecraft weight without sacrificing structural integrity, NASA is pursuing the development of materials that promise to revolutionize not only spacecraft construction, but also a host of potential applications on Earth. Single-walled carbon nanotubes are one material of particular interest. These tubular, single-layer carbon molecules - 100,000 of them braided together would be no thicker than a human hair - display a range of remarkable characteristics. Possessing greater tensile strength than steel at a fraction of the weight, the nanotubes are efficient heat conductors with metallic or semiconductor electrical properties depending on their diameter and chirality (the pattern of each nanotube s hexagonal lattice structure). All of these properties make the nanotubes an appealing material for spacecraft construction, with the potential for nanotube composites to reduce spacecraft weight by 50 percent or more. The nanotubes may also feature in a number of other space exploration applications, including life support, energy storage, and sensor technologies. NASA s various efforts with carbon nanotubes have made it a global leader in this field. Among the many examples are Johnson Space Center s Carbon Nanotube Project, which focuses on bulk nanotube production, purification, and application, and Goddard Space Flight Center s improved arc discharge method of nanotube production, developed under the direction of Jeannette Benavides (featured in Spinoff 2007 and 2008). While the Agency continues its own research, it partners with private companies to advance this unique technology for use on Earth as well as among the stars.

Source record↗

NASA NTRS2004

Numerical Simulation of Nanostructure Growth

Nanoscale structures, such as nanowires and carbon nanotubes (CNTs), are often grown in gaseous or plasma environments. Successful growth of these structures is defined by achieving a specified crystallinity or chirality, size or diameter, alignment, etc., which in turn depend on gas mixture ratios. pressure, flow rate, substrate temperature, and other operating conditions. To date, there has not been a rigorous growth model that addresses the specific concerns of crystalline nanowire growth, while demonstrating the correct trends of the processing conditions on growth rates. Most crystal growth models are based on the Burton, Cabrera, and Frank (BCF) method, where adatoms are incorporated into a growing crystal at surface steps or spirals. When the supersaturation of the vapor is high, islands nucleate to form steps, and these steps subsequently spread (grow). The overall bulk growth rate is determined by solving for the evolving motion of the steps. Our approach is to use a phase field model to simulate the growth of finite sized nanowire crystals, linking the free energy equation with the diffusion equation of the adatoms. The phase field method solves for an order parameter that defines the evolving steps in a concentration field. This eliminates the need for explicit front tracking/location, or complicated shadowing routines, both of which can be computationally expensive, particularly in higher dimensions. We will present results demonstrating the effect of process conditions, such as substrate temperature, vapor supersaturation, etc. on the evolving morphologies and overall growth rates of the nanostructures.

Hwang, Helen H.↗