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PubMedDate not supplied

The early atmosphere: a new picture.

Over the last several years, many of the fundamental ideas concerning the composition and chemical evolution of the Earth's early atmosphere have changed. While many aspects of this subject are clouded--either uncertain or unknown, a new picture is emerging. We are just beginning to understand how astronomical, geochemical, and atmospheric processes each contributed to the development of the gaseous envelope around the third planet from the sun some 4.6 billion years ago and how that envelope chemically evolved over the history of our planet. Simple compounds in that gaseous envelope, energized by atmospheric lightning and/or solar ultraviolet radiation, formed molecules of increasing complexity that eventually evolved into the first living systems on our planet. This process is called "chemical evolution" and immediately preceded biological evolution; once life developed and evolved, it began to alter the chemical composition of the atmosphere that provided the very essence of its creation. Photosynthetic organisms which have the ability to biochemically transform carbon dioxide and water to carbohydrates, which they use for food, produce large amounts of molecular oxygen (O2) as a by-product of the reaction. Atmospheric oxygen photochemically formed ozone, which absorbs ultraviolet radiation from the sun and shields the Earth's surface from this biologically lethal radiation. Once atmospheric ozone levels increased sufficiently, life could leave the safety of the oceans and go ashore for the first time. Throughout the history of our planet, there has been strong interaction between life and the atmosphere. Understanding our cosmic roots is particularly relevant as we embark on a search for life outside the Earth. At this very moment, several radio telescopes around the world are searching for extraterrestrial intelligence (SETI).

Atmosphere↗

PubMed1990

Could organic matter have been preserved on Mars for 3.5 billion years?

3.5 billion years (byr) ago, when it is thought that Mars and Earth had similar climates, biological evolution on Earth had made considerable progress, such that life was abundant. It is therefore surmised that prior to this time period the advent of chemical evolution and subsequent origin of life occurred on Earth and may have occurred on Mars. Analysis for organic compounds in the soil buried beneath the Martian surface may yield useful information regarding the occurrence of chemical evolution and possibly biological evolution. Calculations based on the stability of amino acids lead to the conclusion that remnants of these compounds, if they existed on Mars 3.5 byr ago, might have been preserved buried beneath the surface oxidizing layer. For example, if phenylalanine, an amino acid of average stability, existed on Mars 3.5 byr ago, then 1.6% would remain buried today, or 25 pg-2.5 ng of C g-1 Martian soil may exist from remnants of meteoritic and cometary bombardment, assuming that 1% of the organics survived impact.

Amino Acids↗

PubMed1984

Chemical and biological evolution in space.

Astronomical infrared spectra are used to confirm the existence of complex organic molecules produced by ultraviolet photoprocessing of interstellar grain mantles. This material is shown to be the major component of the interstellar grains between the sun and the galactic center and, by inference, constitutes more than 10 million solar masses--or close to one part in a thousand of the entire mass of the milky way galaxy. It may be demonstrated that the primitive chemistry of the earth's surface was dominated by these extraterrestrial molecules after aggregated into comets if the rate of comet impacts with the earth was comparable with that required to account for the extinction of species over the past 300 million years. Ultraviolet irradiation of bacterial spores has been studied for the first time under simulated interstellar conditions. The inactivation time predicted for the less dense regions of space is at most several hundred years. Within molecular clouds it is shown on theoretical and experimental grounds that this time may be extended to tens of million of years which is the estimated time required for their transport from one solar system to another by a molecular cloud. However survival of spores during their initial exposure to the solar ultraviolet presents a problem for panspermia because it requires that in the process of ejection from the earth's surface they must be enclosed within a cocoon (or mantle) of ultraviolet absorbing material of approximately 0.6 micrometer thickness. Thus, although panspermia can not be rejected on the basis of lack of interstellar survival there may remain insurmountable obstacles to its occurring because of the very special protective shield requirements during ejection from its planetary source.

Bacillus subtilis↗

PubMed2002

The cosmological density of baryons from observations of 3He+ in the Milky Way.

Primordial nucleosynthesis after the Big Bang can be constrained by the abundances of the light elements and isotopes 2H, 3He, 4He and 7Li (ref. 1). The standard theory of stellar evolution predicts that 3He is also produced by solar-type stars, so its abundance is of interest not only for cosmology, but also for understanding stellar evolution and the chemical evolution of the Galaxy. The 3He abundance in star-forming (H II) regions agrees with the present value for the local interstellar medium, but seems to be incompatible with the stellar production rates inferred from observations of planetary nebulae, which provide a direct test of stellar evolution theory. Here we develop our earlier observations, which, when combined with recent theoretical developments in our understanding of light-element synthesis and destruction in stars, allow us to determine an upper limit for the primordial abundance of 3He relative to hydrogen: 3He/H = (1.1 +/- 0.2) x 10(-5). The primordial density of all baryons determined from the 3He data is in excellent agreement with the densities calculated from other cosmological probes. The previous conflict is resolved because most solar-mass stars do not produce enough 3He to enrich the interstellar medium significantly.

Journal Article↗

PubMed1990

Adsorption of 5'-adenosine monophosphate onto precipitated calcium phosphate: effects of inorganic polyphosphates and carbamyl phosphate.

In this paper it is shown that the adsorption of 5'-adenosine monophosphate (5'-AMP) onto precipitated calcium phosphate exhibits a sigmoidal profile as revealed by isotherms at 45 degrees C. This result indicates a cooperative behavior in the adsorption of 5'-AMP. The relationship between adsorption capacity and surface area of the sedimented matrix may be interpreted as an indication that there is a monolayer of the absorbed nucleotide on the solid surface. The pH dependence of adsorption suggests that the negatively charged phosphoryl group of 5'-AMP interacts with a positively charged site (possibly Ca2+) on the matrix surface. The adsorption of the nucleotide is markedly decreased at pH values above 8.0. The Dixon-like plot of the effect of pH suggests an inhibitory role of hydroxyl ions in the adsorption of 5'-AMP. At pH 7.5, other anions such as pyrophosphate, tripolyphosphate and carbamyl phosphate also inhibit the adsorption of the nucleotide, probably by interacting with its adsorption site. We suggest that these phosphorylated molecules could have played a role in chemical evolution by modulating the amount of nucleotides adsorbed onto mineral surfaces. The significance of these phenomena in chemical evolution is discussed.

Adenosine Monophosphate↗

PubMed2005

Electronic and structural evolution and chemical bonding in ditungsten oxide clusters: W2O(n)- and W2O(n) (n = 1-6).

We report a systematic and comprehensive investigation of the electronic structures and chemical bonding in a series of ditungsten oxide clusters, W2O(n)- and W2O(n) (n = 1-6), using anion photoelectron spectroscopy and density functional theory (DFT) calculations. Well-resolved photoelectron spectra were obtained at several photon energies (2.331, 3.496, 4.661, 6.424, and 7.866 eV), and W 5d-based spectral features were clearly observed and distinguished from O 2p-based features. More complicated spectral features were observed for the oxygen-deficient clusters because of the W 5d electrons. With increasing oxygen content in W2O(n)-, the photoelectron spectra were observed to shift gradually to higher binding energies, accompanied by a decreasing number of W 5d-derived features. A behavior of sequential oxidation as a result of charge transfers from W to O was clearly observed. A large energy gap (2.8 eV) was observed in the spectrum of W2O6-, indicating the high electronic stability of the stoichiometric W2O6 molecule. Extensive DFT calculations were carried out to search for the most stable structures of both the anion and neutral clusters. Time-dependent DFT method was used to compute the vertical detachment energies and compare to the experimental data. Molecular orbitals were used to analyze the chemical bonding in the ditungsten oxide clusters and to elucidate their electronic and structural evolution.

Journal Article↗

PubMed1992

The seeding of life by comets.

The evidence that living organisms were already extant on the earth almost 4 Gyr ago and that early bombardment by comets and asteroids created a hostile environment up to about this time has revived the question of how it was possible for prebiotic chemical evolution to have provided the necessary ingredients for life to have developed in the short intervening time. The actual bracketed available temporal space is no more than 0.5 Gyr and probably much less. Was this sufficient time for an earth-based source of the first simple organic precursor molecules to have led to the level of the prokaryotic cell? If not, then the difficulty would be resolved if the ancient earth was impregnated by organic molecular seed from outer space. Curiously, it seems that the most likely source of such seeds was the same a one of the sources of the hostile enviroment, namely the comets which bombarded the earth. With the knowledge of comets gained by the space missions it has become clear that a very large fraction of the chemical composition of comet nuclei consists of quite complex organic molecules. Furthermore it has been demonstrated that comets consist of very fluffy aggregates of interstellar dust whose chemistry derives from photoprocessing of simple ice mixtures in space. Thus, the ultimate source of organics in comets comes from the chemical evolution of interstellar dust. An important and critical justification for assuming that interstellar dust is the ultimate source of prebiotic molecular insertion on the earth is the proof that comets are extremely fluffy aggregates, which have the possibility of breaking up into finely divided fragments when the comet impacts the earth's atmosphere. In the following we will summarize the properties of interstellar dust and the chemical and morphological structure of comets indicated by the most recent interpretations of comet observations. It will be shown that the suitable condition for comets having provided abundant prebiotic molecules as well as the water in which they could have further evolved are consistent with theories of the early earth environment.

Cosmic Dust↗

PubMedDate not supplied

Amino acids in carbonaceous chondrites.

For almost 20 years laboratory experiments have advanced the concepts of chemical evolution, particularly with regard to formation of the amino acids. What has been generally lacking is concrete natural evidence for this chemical evolution hypothesis. The recent development of sophisticated analytical techniques and availability of carbonaceous chondrites with a minimum of terrestrial contamination has resulted in the identification of amino acids which provide strong evidence for a natural extraterrestrial chemical synthesis. Since the initial find in the Murchison meteorite (a type II carbonaceous chondrite) of both protein and nonprotein amino acids with nearly equal abundances of D and L isomers, further studies have been carried out. These studies have revealed the presence of at least 35 amino acids; the population consists of a wide variety of linear, cyclic and polyfunctional amino acids which shows a trend of decreasing concentration with increasing carbon number. Investigations of the Murray meteorite (a type II carbonaceous chondrite) has produced similar results, but studies of the Orgueil meteorite (a type I carbonaceous chondrite) show only a limited suite of amino acids, some of which appear to be indigenous while others appear to be terrestrial contaminanats. A sample of the Murchison meteorite was extracted with D2O and in addition of 'free' amino acids, showing no deuterium incorporation, some amino acids showed the presence of deuterium suggesting either a 'precursor(s)' or hydrogen-deuterium exchange which require(s) formation of carbon-hydrogen bonds.

Amino Acids↗

PubMed1976

Model consideration for the origin of life. Environmental structure as stimulus for the evolution of chemical systems.

In an attempt to understand the origin of living systems we encounter the following problems: How can we conceive the origin of the first self-reproducing forms, and by means of what stimuli could a constant increase in the complexity of such forms commence? How can a translation apparatus for genetic information develop? One cannot imagine that such an apparatus for the synthesis of enzymes can function alone without the interference of enzymes themselves, which, however, could only become available after the construction of the apparatus itself. What stimulus mechanism is conceivable that leads to the division of the genetic apparatus into a replication system, and an enzyme-synthesis system? The main problem therefore, is not the search for basic theoretical concepts. It is not a question which can be answered by means of specific experiments. One should rather explore the principal possibilities of how molecules combine to produce more and more complicated functional units. We look for the fundamental structural changes in the organizational systems and the driving forces initiating these developments. Questions concerning the detailed chemical realization are of secondary importance. In trying to solve the puzzle of how the genetic apparatus is gradually built up as complex aggregates of molecules, we consider a consistent causal chain of simple and transparent physiochemical model steps. The driving force for the self-organization of matter is seen in a specific environmental structure to be found on the surface of the earth. By this structure, which is periodic in time and heterogeneous in space, evolution is initiated and driven towards a continuously increasing degree of complexity correlated with a continuous expansion of the accessible living space. This process is a necessity under proper environmental conditions. Accidental events initiate each step but do not determine the general course of evolution which is determined by the selection mechanism.

Adenosine Monophosphate↗

PubMed2005

Point defect dynamics and evolution of chemical reactions in alanates by anelastic spectroscopy.

We report the first measurements of elastic modulus and energy dissipation in Ti-doped and undoped sodium aluminum hydride. It is shown that the chemical reactions that occur by varying the sample temperatures or by aging most sensitively affect the elastic constants, such that the modulus variations allow the time and temperature evolution of decomposition to be monitored. After a well-defined thermal treatment at 436 K, a thermally activated relaxation process appears at 70 K in the kilohertz range, denoting the existence of a new species, likely involving hydrogen, having a very high mobility, that is, 10(3) jumps/s at the peak temperature corresponding to a relaxation rate of about 10(11) s(-1) at room temperature. The activation energy of the process is 0.126 eV and the preexponential factor 7 x 10(-14) s, which is typical of point defect relaxation. The peak is very broad with respect to a single Debye process, indicating strong interaction or/and multiple jumping type of the mobile entity. The present data suggest that the models aiming at interpreting the decomposition reactions and kinetics should take into account the indicated point-defect dynamics and stoichiometry defects.

Journal Article↗

PubMed1999

Phylogeny and evolution of chemical communication: an endocrine approach.

The present review assesses the phylogenetic history of information molecules (bioregulators pheromones, hormones, neuroactive compounds), receptors, transducers, second messengers) in uni- and multicellular organisms. Transitional stages between contemporary endocrine secretions including hormones and neuroactive materials, and primogenial exocrine compounds (pheromones) are proposed. Severalhypotheses have been developed to explain the origin and evolution of bioregulator/receptor units. Finally, how these primordial information molecules have either been co-opted or have changed their function during the course of biological evolution is analysed.

Amino Acid Sequence↗

PubMed1997

The physical and chemical nature of technegas.

UNLABELLED: Technegas, the discrete radio-aerosol particle, containing 99mTc has been investigated, and the chemical evolution and physical properties of the particle demonstrated. METHODS: A commercial technegas generator was used to produce aerosols according to standard clinical procedures. The aerosols were collected by electrostatic precipitation and examined with transition electron microscopy (TEM), scanning electron microscopy (SEM) and force microscopy. The chemical evolution was examined by x-ray techniques and thermogravimetric analysis. RESULTS: The active particle was identified as hexagonal platelets of metallic technetium contained within a thin layer of graphitic carbon. This composite structure is discussed in light of the metal particle behaving as a template for the carbon capsule. The average size of the observed hexagonal platelets, 30-60 nm, was only weakly dependent on the concentration of technetium in the crucible. CONCLUSION: The mechanism for the formation of the technegas pancreas has been developed and the particles involved characterized. It appears that the use of other metals also leads to the formation of similar materials.

Aerosols↗

PubMed2006

Coupled partitioning, dilution, and chemical aging of semivolatile organics.

A unified framework of semi-volatile partitioning permits models to efficiently treat both semi-volatile primary emissions and secondary organic aerosol production (SOA), and then to treat the chemical evolution (aging) of the aggregate distribution of semi-volatile material. This framework also reveals critical deficiencies in current emissions and SOA formation measurements. The key feature of this treatment is a uniform basis set of saturation vapor pressures spanning the range of ambient organic saturation concentrations, from effectively nonvolatile material at 0.01 microg m(-3) to vapor-phase effluents at 100 mg m(-3). Chemical evolution can be treated by a transformation matrix coupling the various basis vectors. Using this framework, we show that semi-volatile partitioning can be described in a self-consistent way, with realistic behavior with respect to temperature and varying organic aerosol loading. The time evolution strongly suggests that neglected oxidation of numerous "intermediate volatility" vapors (IVOCs, with saturation concentrations above approximately 1 mg m(-3)) may contribute significantly to ambient SOA formation.

Aerosols↗

PubMed2004

Loss of co-linearity by modular polyketide synthases: a mechanism for the evolution of chemical diversity.

Modular polyketide synthases biosynthesise natural products through successive Claisen-type condensations, where one module is responsible for one round of chain extension. This review describes recent findings where this rule of co-linearity is broken, either by one module being bypassed (skipping) or through one module being used for multiple chain extension events (stuttering).

Biological Evolution↗

PubMed1979

Phosphorylation of adenosine in aqueous solution by electric discharges.

Dehydration reactions involving condensing reagents in aqueous solution have been studied as models of chemical evolution, and one such reagent has been found to be produced in the supposed primitive Earth conditions. We assumed that the dehydration condensation in aqueous solution could occur if the condensing reagents, which appear to be produced by electric discharges in the gas phase, could be carried to the aqueous solution through the recycling of water washing the wall of the vessel. We present here an experimental study of the dehydration condensation between phosphate and adenosine in aqueous solution using a new discharge apparatus (Fig. 1) which simulates prebiotic chemical evolution. The apparatus was designed so that water recycles in a vessel containing a solution at a relatively low temperature (approximately 30 degrees C), achieved by showering water at 18 degrees C from above the vessel. This is a simulation of the recycling system of water on the Earth, depending on a large difference in temperature between the ocean surface and the sky.

Adenosine↗

PubMed1976

Evolutionary oscillation in prebiology: igneous activity and the origins of life.

The processes of chemical evolution are responsible for the origin of life. Three such processes have special importance: oscillation, creation, and competition. An oscillation from one kind of environment to another provides a mechanism for instituting processes that can only take place under conditions far removed from equilibrium. Oscillating evolutionary processes are likely to have played an important part in the origin of life. It is a mistake to assume that life originated in any one environment. It did not arrive in a moment of time. It was the result of a long period of chemical evolution during which it passed through a variety of environments. Biopoesis took place in an environment in which a variety of different kinds of protolife were assembled and concentrated. One essential form of protolife involved in these processes is the protocell. The experiments of Fox suggest that the creation of protocells involves violent oscillations of temperature and hydration. Igneous activity is especially characterised by oscillating conditions. Volcanic eruptions consist of violent changes from one extreme condition to another. Temperatures, pressure, phase, concentration and hydration all oscillate violently, and are subject to shock pulses of many kinds. Protolife may well have passed through extremes of environment for wider that those that life itself can sustain. The most probable environment for the assembly of the various forms of protolife would be on mudbanks forming either at the mouth of streams draining regions of active vulcanicity, or round the edge of hot volclanic pools. In this situation one could fins concentrated not only the various stands of protolife necessary for the final act of biopoesis, but also perbiologically formed nutrients necessary as for the first eobionts. As soon as the first protocells start to grow, they start to compete with each other, and so initiate a new additional evolutionary process, that of natural selection. Only after such competition has been initiated is life itself likely to be established"20

Biological Evolution↗

PubMed1975

Methyleneaminoacetonitrile: possible role in chemical evolution-II.

Methyleneaminoacetonitrile (MAAN) when reacted with other amino acids, gives rise to the formation of peptides in addition to the usual hydrolytic products. It acts as a precursor of glycine and also as a dehydration condensing agent. It has been shown that MAAN is easily formed by the reaction of hydrogen cyanide, ammonia and formaldehyde as well as by the reaction of formaldehyde with aminoacetonitrile, in dilute ammoniacal solution.

Acetonitriles↗

PubMed2007

Size-dependent structural evolution and chemical reactivity of gold clusters.

Ground-state structures and other experimentally relevant isomers of Au(15) (-) to Au(24) (-) clusters are determined through joint first-principles density functional theory and photoelectron spectroscopy measurements. Subsequent calculations of molecular O(2) adsorption to the optimal cluster structures reveal a size-dependent reactivity pattern that agrees well with earlier experiments. A detailed analysis of the underlying electronic structure shows that the chemical reactivity of the gold cluster anions can be elucidated in terms of a partial-jellium picture, where delocalized electrons occupying electronic shells move over the ionic skeleton, whose geometric structure is strongly influenced by the directional bonding associated with the highly localized "d-band" electrons.

Journal Article↗