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PubMed1997

A high deuterium abundance at redshift z = 0.7.

Of the light elements, the primordial abundance of deuterium relative to hydrogen, (D/H)p, provides the most sensitive diagnostic for the cosmological mass density parameter, omegaB. Recent high-redshift D/H measurements are highly discrepant, although this may reflect observational uncertainties. The larger primordial D/H values imply a low omegaB (requiring the Universe to be dominated by non-baryonic matter), and cause problems for galactic chemical evolution models, which have difficulty in reproducing the steep decline in D/H to the present-day values. Conversely, the lower D/H values measured at high redshift imply an omegaB greater than that derived from 7Li and 4He abundance measurements, and may require a deuterium-abundance evolution that is too low to easily explain. Here we report the first measurement of D/H at intermediate redshift (z = 0.7010), in a gas cloud selected to minimize observational uncertainties. Our analysis yields a value of D/H ((2.0 +/- 0.5) x 10[-4]) which is at the upper end of the range of values measured at high redshifts. This finding, together with other independent observations, suggests that there may be inhomogeneity in (D/H)p of at least a factor of ten.

Astronomical Phenomena↗
PubMed1999

Accretion of low-metallicity gas by the Milky Way.

Models of the chemical evolution of the Milky Way suggest that the observed abundances of elements heavier than helium ('metals') require a continuous infall of gas with metallicity (metal abundance) about 0.1 times the solar value. An infall rate integrated over the entire disk of the Milky Way of approximately 1 solar mass per year can solve the 'G-dwarf problem'--the observational fact that the metallicities of most long-lived stars near the Sun lie in a relatively narrow range. This infall dilutes the enrichment arising from the production of heavy elements in stars, and thereby prevents the metallicity of the interstellar medium from increasing steadily with time. However, in other spiral galaxies, the low-metallicity gas needed to provide this infall has been observed only in associated dwarf galaxies and in the extreme outer disk of the Milky Way. In the distant Universe, low-metallicity hydrogen clouds (known as 'damped Ly alpha absorbers') are sometimes seen near galaxies. Here we report a metallicity of 0.09 times solar for a massive cloud that is falling into the disk of the Milky Way. The mass flow associated with this cloud represents an infall per unit area of about the theoretically expected rate, and approximately 0.1-0.2 times the amount required for the whole Galaxy.

Astronomical Phenomena↗
PubMed2005

Density of hydrous silicate melt at the conditions of Earth's deep upper mantle.

The chemical evolution of the Earth and the terrestrial planets is largely controlled by the density of silicate melts. If melt density is higher than that of the surrounding solid, incompatible elements dissolved in the melt will be sequestered in the deep mantle. Previous studies on dry (water-free) melts showed that the density of silicate melts can be higher than that of surrounding solids under deep mantle conditions. However, melts formed under deep mantle conditions are also likely to contain some water, which will reduce the melt density. Here we present data constraining the density of hydrous silicate melt at the conditions of approximately 410 km depth. We show that the water in the silicate melt is more compressible than the other components, and therefore the effect of water in reducing melt density is markedly diminished under high-pressure conditions. Our study indicates that there is a range of conditions under which a (hydrous) melt could be trapped at the 410-km boundary and hence incompatible elements could be sequestered in the deep mantle, although these conditions are sensitive to melt composition as well as the composition of the surrounding mantle.

Journal Article↗
PubMed2006

Long gamma-ray bursts and core-collapse supernovae have different environments.

When massive stars exhaust their fuel, they collapse and often produce the extraordinarily bright explosions known as core-collapse supernovae. On occasion, this stellar collapse also powers an even more brilliant relativistic explosion known as a long-duration gamma-ray burst. One would then expect that these long gamma-ray bursts and core-collapse supernovae should be found in similar galactic environments. Here we show that this expectation is wrong. We find that the gamma-ray bursts are far more concentrated in the very brightest regions of their host galaxies than are the core-collapse supernovae. Furthermore, the host galaxies of the long gamma-ray bursts are significantly fainter and more irregular than the hosts of the core-collapse supernovae. Together these results suggest that long-duration gamma-ray bursts are associated with the most extremely massive stars and may be restricted to galaxies of limited chemical evolution. Our results directly imply that long gamma-ray bursts are relatively rare in galaxies such as our own Milky Way.

Journal Article↗
PubMed2002

Organic compounds in carbonaceous meteorites.

The carbonaceous chondrite meteorites are fragments of asteroids that have remained relatively unprocessed since the formation of the solar system 4.6 billion years ago. These carbon-rich objects contain a variety of extraterrestrial organic molecules that constitute a record of chemical evolution prior to the origin of life. Compound classes include aliphatic hydrocarbons, aromatic hydrocarbons, amino acids, carboxylic acids, sulfonic acids, phosphonic acids, alcohols, aldehydes, ketones, sugars, amines, amides, nitrogen heterocycles, sulfur heterocycles and a relatively abundant high molecular weight macromolecular material. Structural and stable isotopic characteristics suggest that a number of environments may have contributed to the organic inventory, including interstellar space, the solar nebula and the asteroidal meteorite parent body. This review covers work published between 1950 and the present day and cites 193 references.

Algorithms↗
PubMed1969

Peptide formation mediated by hydrogen cyanide tetramer: a possible prebiotic process.

Chemical evolution on the primitive earth must have involved condensation of alpha-amino acids to peptides. Under aqueous conditions consistent with current conceptions of primordial waters, heating glycerine with the hydrogen cyanide tetramer, diaminomaleonitrile, yields dipeptide. If nitrogen was cycled through primordial waters as cyanide, peptide synthesis by stepwise tetramer-mediated condensation of alpha-amino acids would have been a plausible process.

Dipeptides↗
PubMed1971

Nonprotein amino acids in the murchison meteorite.

Twelve nonprotein amino acids appear to be present in the Murchison meteorite. The identity of eight of them has been conclusively established as N-methylglycine, beta-alanine, 2-methylalanine, alpha-amino-n-butyric acid, beta-amino-n-butyric acid, gamma-amino-n-butyric acid, isovaline, and pipecolic acid. Tentative evidence is presented for the presence of N-methylalanine, N-ethylglycine, beta-aminoisobutyric acid, and norvaline. These amino acids appear to be extraterrestrial in origin and may provide new evidence for the hypothesis of chemical evolution.

Journal Article↗
PubMed1989

X-ray studies on crystalline complexes involving amino acids and peptides. Part XX. Crystal structures of DL-arginine acetate monohydrate and DL-lysine acetate and a comparison with the corresponding L-amino acid complexes.

Crystals of DL-arginine acetate monohydrate, C6H15N4O2+C2H3O2-.H2O, are monoclinic, P2(1)/c, with a = 13.552(2), b = 5.048(2), c = 18.837(3) A, beta = 101.34(2) degrees and Z = 4, and those of DL-lysine acetate, C6H15N2O2+.C2H3O2- are triclinic, P1, with a = 5.471(2), b = 7.656(2), c = 12.841(2) A, alpha = 94.48(1), beta = 94.59(2), gamma = 98.83(2) degrees and Z = 2. The structures have been solved by direct methods and refined to R = 0.058 and 0.077 for 1522 and 1259 observed reflections respectively. The difference in the number and the nature of proton donors leads to a difference in hydrogen bond density in the two structures. The basic elements of aggregation in both the structures are pairs of amino acid molecules, each pair stabilized by two centrosymmetrically related hydrogen bonds involving alpha-amino and alpha-carboxylate groups, stacked along the shortest dimension to form columns. The pairs are held together in each column by head-to-tail sequences. The columns stack along a crystallographic axis to form layers. Adjacent layers are bridged by acetate ions. The amino acid-acetate interactions are primarily through side chains and involve specific interactions and characteristic interaction patterns. The gross features of molecular aggregation are nearly the same in DL-arginine acetate monohydrate and L-arginine acetate whereas they are substantially different in the lysine complexes. In both cases, one of the two head-to-tail sequences in the L complex is replaced by a hydrogen bonded loop involving alpha-amino and alpha-carboxylate groups, in the DL complex. This may have implications for prebiotic condensation during chemical evolution.

Acetates↗
PubMed2000

The Origin of Extremely Metal-poor Carbon Stars and the Search for Population III.

The number of known extremely metal-deficient stars has recently increased substantially, stimulating inquiry into the formation and initial chemical evolution of the Milky Way. In order to draw proper inferences from the observations, it is necessary to understand the evolution of these low-mass stars and the modifications in their surface elemental abundances that they have experienced during their long lifetimes. Among the observations to be explained is the fact that the incidence of carbon-enhanced stars increases with decreasing metallicity. We show that low-mass, extremely metal-poor stars evolve into carbon stars along paths that are quite different from those followed by more metal-rich stars of younger populations. This permits us, in principle, to distinguish the brightest survivors of the first generations of stars formed in the universe (Population III carbon stars) from stars belonging to younger populations.

Journal Article↗
PubMed2000

Primordial Lithium and Big Bang Nucleosynthesis.

Recent determinations of the abundance of the light-element Li in very metal-poor stars show that its intrinsic dispersion is essentially zero and that the random error in the estimated mean Li abundance is negligible. However, a decreasing trend in the Li abundance toward lower metallicity indicates that the primordial abundance of Li can be inferred only after allowing for nucleosynthesis processes that must have been in operation in the early history of the Galaxy. We show that the observed Li versus Fe trend provides a strong discriminant between alternative models for Galactic chemical evolution of the light elements at early epochs. We critically assess current systematic uncertainties and determine the primordial Li abundance within new, much tighter limits: &parl0;Li&solm0;H&parr0;p=1.23+0.68-0.32x10-10. We show that the Li constraint on OmegaB is now limited as much by uncertainties in the nuclear cross sections used in big bang nucleosynthesis (BBN) calculations as by the observed abundance itself. A clearer understanding of systematics allows us to sharpen the comparison with 4He and deuterium and the resulting test of BBN.

Journal Article↗
PubMed2000

Probing the Site for r-Process Nucleosynthesis with Abundances of Barium and Magnesium in Extremely Metal-poor Stars.

We suggest that if the astrophysical site for r-process nucleosynthesis in the early Galaxy is confined to a narrow mass range of Type II supernova (SN II) progenitors, with a lower mass limit of Mms=20 M middle dot in circle, a unique feature in the observed distribution of [Ba/Mg] versus [Mg/H] for extremely metal-poor stars can be adequately reproduced. We associate this feature, a bifurcation of the observed elemental ratios into two branches in the Mg abundance interval -3.7</=&sqbl0;Mg&solm0;H&sqbr0;</=-2.3, with two distinct processes. The first branch, which we call the y-branch, is associated with the production of Ba and Mg from individual massive supernovae. The derived mass of Ba synthesized in SNe II is 8.5x10-6 M middle dot in circle for Mms=20 M middle dot in circle and 4.5x10-8 M middle dot in circle for Mms=25 M middle dot in circle. We conclude that SNe II with Mms approximately 20 M middle dot in circle are the dominant source of r-process nucleosynthesis in the early Galaxy. An SN-induced chemical evolution model with this Mms-dependent Ba yield creates the y-branch, reflecting the different nucleosynthesis yields of [Ba/Mg] for each SN II with Mms greater, similar20 M middle dot in circle. The second branch, which we call the i-branch, is associated with the elemental abundance ratios of stars which were formed in the dense shells of the interstellar medium swept up by SNe II with Mms<20 M middle dot in circle that do not synthesize r-process elements, and it applies to stars with observed Mg abundances in the range &sqbl0;Mg&solm0;H&sqbr0;<-2.7. The Ba abundances in these stars reflect those of the interstellar gas at the (later) time of their formation. The existence of a [Ba/Mg] i-branch strongly suggests that SNe II that are associated with stars of progenitor mass Mms</=20 M middle dot in circle are infertile sources for the production of r-process elements. We predict the existence of this i-branch for other r-process elements, such as europium (Eu), to the extent that their production site is in common with Ba.

Journal Article↗
PubMed2003

Necessary, but not sufficient: Raman identification of disordered carbon as a signature of ancient life.

To identify microscopic particles as actual fossil material, it would be useful to have a means of unambiguously recognizing which carbonaceous deposits found in rocks are residues from once-living organisms (i.e., biogenic material). Those residues consist of many different, mostly aromatic (i.e., benzene ring-containing), C-O-H-dominated molecules, and typically are called kerogens. Raman microprobe spectroscopy can be applied to minute samples of ancient kerogens either isolated from their host rocks or in situ in thin section. The Raman spectra generated by monochromatic blue or green laser excitation (e.g., at 488, 514, 532 nm) typically show only generic spectral features indicative of discontinuous arrays of condensed benzene rings (i.e., structures referred to as "disordered carbonaceous material"). Thus, despite the complex chemistry of kerogens and the expected presence of H, O, and N, the Raman spectra typically do not show any evidence of functional groups, such as CH, CH(2), CH(3), CO, and CN. Moreover, the same kind of Raman spectral signature as is obtained from kerogens also is obtained from many other poorly ordered carbonaceous materials that arise through nonbiological processes, such as in situ heating of organic or inorganic compounds (whether or not they are of biological origin), metamorphic mobilization of preexisting carbon compounds, and high-temperature precipitation from hydrothermal solutions. Thus, neither a Raman spectrum, nor a Raman image derived from such spectra, definitively can identify a sample as "kerogen," but only as "disordered carbonaceous material." Clearly, the fact that small, opaque grains consist of disordered carbonaceous material is necessary, but not sufficient, to prove them to be residues of cellular material and, thus, biogenic.

Carbon↗
PubMed1982

Template directed reactions of 2-aminoadenylic acid derivatives.

The template-directed oligomerization of activated derivatives of 2-aminoadenylic acid (paA) on polyuridylic acid (poly(U)) in aqueous buffers was studied. The reaction differs from that of adenylic acid (pA) under identical conditions, in that only di- and tri-nucleotides are observed as substantial products rather than a longer sequence of oligomers. The reaction of paA also differs from that of pA in that it does not require Mg++, and is less susceptible to increased temperature. The relevance of these observations to the chemical evolution of polynucleotide replication is discussed. Improved syntheses of paA and its diphosphate are reported.

Animals↗
PubMed1985

Thermophilic microspheres of peptide-like polymers and silicates formed at 250 degrees C.

We examined the possibility of chemical evolution in superheated hydrothermal environments and found the formation of microspheres at 250 degrees C and above from a mixture of glycine, alanine, valine, and aspartic acid. The microspheres did not form at lower temperatures and consisted of silicates and peptide-like polymers that contained imide bonds and amino acid residues having an abundance of valine. The results show the possibility of thermophilic cellular structures, which might be adopted by the extremely thermophilic organisms, if they exist, reported by Baross and Deming.

Amino Acids↗
PubMed1987

Comparative uptake from sea water and tissue distribution of 60Co in marine mollusks.

Five different species of marine mollusks, Mytilus galloprovincialis Lmk., Tapes decussatus L., Cerastoderma (Cardium) edule (L.), Donax vittatus (da Costa) and Patella vulgata L., were exposed to 60Co-labelled sea water under laboratory conditions. After a 1-mo exposure, tested species reached different whole-body 60Co concentration factors (CF) over radioactive sea water of 73 +/- 27, 22 +/- 10, 84 +/- 25, 6.3 +/- 1.4 and 31 +/- 10, respectively, which are not dependent upon the size of mollusks. Equations for the experimental uptake curves, obtained using a multi-exponential model, indicate that 60Co uptake by mollusks involves two or three compartments, according to the species. In all species, the larger compartments turn over with long biological half-lives (24-251 d), dependent upon species. At the beginning of the experiment, 60CoCl2 added to sea water was mainly in cationic forms. These forms were progressively converted into anionic plus neutral forms most likely due to complex formation with organic ligands. With time this physico-chemical evolution had a lowering effect on 60Co bioaccumulation by mollusks. Analysis of 60Co in tissues revealed that Donax shell and mantle do not accumulate the radionuclide in great quantities, generating the low whole-body concentration factor found. In contrast, shell and mantle from all other species displayed variable but high CFs. Shell by itself accounts for more than half of the 60Co whole-body burden. Among soft tissues, gills and viscera displayed the highest CF and muscle the lowest. From these experiments, one may conclude that significant differences among species do exist regarding Co bioaccumulation potential. The wide range in Co CF values for mollusks found in the literature is also largely supported by interspecific differences actually existing.

Animals↗
PubMed1999

Calculations of background beta-gamma radiation dose through geologic time.

Life on earth is exposed to a background level of ionizing radiation from a number of sources, including beta and gamma radiation from geologic and biologic materials. Radiation dose from geologic emitters has changed because of the chemical evolution of the continental crust, changes in the relative abundances of 235U and 238U, and the radioactive decay of uranium, thorium, and 40K with time. The radiation dose from internal 40K has decreased by a factor of about eight because of changes in the activity concentration of 40K in potassium over the past 4 billion years. Radiation exposure from geologic materials has decreased from about 1.6 mGy y(-1) to 0.66 mGy y(-1) over the past 4 billion years, and radiation exposure to an organism with a potassium concentration of 250 mmol L(-1) has decreased from about 5.5 to about 0.70 mGy y(-1). Accordingly, background radiation exposure from these two sources has dropped from about 7.0 to 1.35 mGy y(-1) during the time life has existed on Earth. The conservative nature of mutation repair mechanisms in modern organisms suggest that these mechanisms may have evolved in the distant past and that organisms may retain some of the capability of efficiently repairing damage from higher radiation levels than exist at present.

Beta Particles↗
PubMed2002

Have sudden large releases of methane from geological reservoirs occurred since the Last Glacial Maximum, and could such releases occur again?

Methane emissions from geological reservoirs may have played a major role in the sudden events terminating glaciation, both at the start of the Bølling/Allerød and also at the end of the Younger Dryas. These reservoirs include Arctic methane hydrates and also methane hydrate stored in offshore marine sediments in tropical and temperate latitudes. Emissions from hydrate stores may have resonated with tropical wetland emissions, each reinforcing the other. Because methane is such a powerful greenhouse gas, much smaller emissions of methane, compared with carbon dioxide, are required in order to have the same short-term impact by climate forcing. The methane-linked hypothesis has much geological support from sea-floor evidence of emission. However, Greenland ice-core records have been interpreted as showing methane as a consequential factor, rather than the leader, of change. This interpretation can be challenged on the grounds that temperature gradients in Greenland ice record local changes and local timing of a step-like shift in weather fronts, while methane concentrations record changes on a hemispheric and global scale. There are large remaining hydrate reservoirs in the Arctic and in shelf sediments globally, and there is substantial risk of further emissions.

Climate↗