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Synthesis of biologically pertinent peptides under possible primordial conditions.
Synthesis of biologically pertinent peptides under possible primordial conditions
Membrane peptides and their role in protobiological evolution
How simple membrane peptides performed such essential protocellular functions as transport of ions and organic matter across membranes separating the interior of the cell from the environment, capture and utilization of energy, and transduction of environmental signals, is a key question in protobiological evolution. On the basis of detailed, molecular-level computer simulations we explain how these peptides fold at water-membrane interfaces, insert into membranes, self-assemble into higher-order structures and acquire functions. We have investigated the interfacial behavior and folding of several peptides built of leucine and glutamine residues and have demonstrated that many of them tend to adopt ordered structures. Further, we have studied the insertion of an alpha-helical peptide containing leucine (L) and serine (S) of the form (LSLLLSL)3 into a model membrane. The transmembrane state is metastable, and approximately 15 kcal mol(-1) is required to insert the peptide into the membrane. Investigations of dimers formed by (LSLLLSL)3 and glycophorin A demonstrate how the favorable free energy of helix association can offset the unfavorable free energy of insertion, leading to self-assembly of peptide helices in the membrane. An example of a self-assembled structure is the tetrameric transmembrane pore of the influenza virus M2 protein, which is an efficient and selective voltage-gated proton channel. Our simulations explain the gating mechanism and provide guidelines how to re-engineer the channel to act as a simple proton pump. In general, emergence of integral membrane proteins appears to be quite feasible and may be easier to envision than the emergence of water-soluble proteins.
On the existence and stability of liquid water on the surface of mars today
The recent discovery of high concentrations of hydrogen just below the surface of Mars' polar regions by Mars Odyssey has enlivened the debate about past or present life on Mars. The prevailing assumption prior to the discovery was that the liquid water essential for its existence is absent. That assumption was based largely on the calculation of heat and mass transfer coefficients or theoretical climate models. This research uses an experimental approach to determine the feasibility of liquid water under martian conditions, setting the stage for a more empirical approach to the question of life on Mars. Experiments were conducted in three parts: Liquid water's existence was confirmed by droplets observed under martian conditions in part 1; the evolution of frost melting on the surface of various rocks under martian conditions was observed in part 2; and the evaporation rate of water in Petri dishes under Mars-like conditions was determined and compared with the theoretical predictions of various investigators in part 3. The results led to the conclusion that liquid water can be stable for extended periods of time on the martian surface under present-day conditions.
Remote sensing of planetary properties and biosignatures on extrasolar terrestrial planets
The major goals of NASA's Terrestrial Planet Finder (TPF) and the European Space Agency's Darwin missions are to detect terrestrial-sized extrasolar planets directly and to seek spectroscopic evidence of habitable conditions and life. Here we recommend wavelength ranges and spectral features for these missions. We assess known spectroscopic molecular band features of Earth, Venus, and Mars in the context of putative extrasolar analogs. The preferred wavelength ranges are 7-25 microns in the mid-IR and 0.5 to approximately 1.1 microns in the visible to near-IR. Detection of O2 or its photolytic product O3 merits highest priority. Liquid H2O is not a bioindicator, but it is considered essential to life. Substantial CO2 indicates an atmosphere and oxidation state typical of a terrestrial planet. Abundant CH4 might require a biological source, yet abundant CH4 also can arise from a crust and upper mantle more reduced than that of Earth. The range of characteristics of extrasolar rocky planets might far exceed that of the Solar System. Planetary size and mass are very important indicators of habitability and can be estimated in the mid-IR and potentially also in the visible to near-IR. Additional spectroscopic features merit study, for example, features created by other biosignature compounds in the atmosphere or on the surface and features due to Rayleigh scattering. In summary, we find that both the mid-IR and the visible to near-IR wavelength ranges offer valuable information regarding biosignatures and planetary properties; therefore both merit serious scientific consideration for TPF and Darwin.
Martian water: are there extant halobacteria on Mars?
On Earth, life exists in all niches where water exists in liquid form for at least a portion of the year. On Mars, any liquid water would have to be a highly concentrated brine solution. It is likely, therefore, that any present-day Martian microorganisms would be similar to terrestrial halophiles. Even if present-day life does not exist on Mars, it is an interesting speculation that ancient bacteria preserved in salt deposits could be retrieved from an era when the climate of Mars was more conducive to life.
A non-earthcentric approach to life detection
The ultimate goal of a comprehensive life detection strategy is never to miss life when we encounter it. To accomplish this goal, we must define life in universal, that is, non-Earthcentric, measurable terms. Next, we must understand the nature of biosignatures observed from the measured parameters of life. And finally, we must have a clear idea of the end-member states for the search--what does life, past life, or no life look like (in terms of the measured parameters) at multiple spatial and temporal scales? If we can approach these problems both in the laboratory and in the field on Earth, then we have a chance of being able to detect life elsewhere in our solar system. What are the required limits of detection at each of those scales? What spatial, spectral, and temporal resolutions are necessary to detect life? These questions are actively being investigated in our group, and in this report, we present our strategy and approach to non-Earthcentric life detection.
Racemic amino acids from the ultraviolet photolysis of interstellar ice analogues
The delivery of extraterrestrial organic molecules to Earth by meteorites may have been important for the origin and early evolution of life. Indigenous amino acids have been found in meteorites-over 70 in the Murchison meteorite alone. Although it has been generally accepted that the meteoritic amino acids formed in liquid water on a parent body, the water in the Murchison meteorite is depleted in deuterium relative to the indigenous organic acids. Moreover, the meteoritical evidence for an excess of laevo-rotatory amino acids is hard to understand in the context of liquid-water reactions on meteorite parent bodies. Here we report a laboratory demonstration that glycine, alanine and serine naturally form from ultraviolet photolysis of the analogues of icy interstellar grains. Such amino acids would naturally have a deuterium excess similar to that seen in interstellar molecular clouds, and the formation process could also result in enantiomeric excesses if the incident radiation is circularly polarized. These results suggest that at least some meteoritic amino acids are the result of interstellar photochemistry, rather than formation in liquid water on an early Solar System body.
Carbonaceous meteorites as a source of sugar-related organic compounds for the early Earth
The much-studied Murchison meteorite is generally used as the standard reference for organic compounds in extraterrestrial material. Amino acids and other organic compounds important in contemporary biochemistry are thought to have been delivered to the early Earth by asteroids and comets, where they may have played a role in the origin of life. Polyhydroxylated compounds (polyols) such as sugars, sugar alcohols and sugar acids are vital to all known lifeforms-they are components of nucleic acids (RNA, DNA), cell membranes and also act as energy sources. But there has hitherto been no conclusive evidence for the existence of polyols in meteorites, leaving a gap in our understanding of the origins of biologically important organic compounds on Earth. Here we report that a variety of polyols are present in, and indigenous to, the Murchison and Murray meteorites in amounts comparable to amino acids. Analyses of water extracts indicate that extraterrestrial processes including photolysis and formaldehyde chemistry could account for the observed compounds. We conclude from this that polyols were present on the early Earth and therefore at least available for incorporation into the first forms of life.
Adenine derivatives as phosphate-activating groups for the regioselective formation of 3',5'-linked oligoadenylates on montmorillonite: possible phosphate-activating groups for the prebiotic synthesis of RNA
Methyladenine and adenine N-phosphoryl derivatives of adenosine 5'-monophosphate (5'-AMP) and uridine 5'-monophosphate (5'-UMP) are synthesized, and their structures are elucidated. The oligomerization reactions of the adenine derivatives of 5'-phosphoramidates of adenosine on montmorillonite are investigated. 1-Methyladenine and 3-methyladenine derivatives on montmorillonite yielded oligoadenylates as long as undecamer, and the 2-methyladenine and adenine derivatives on montmorillonite yielded oligomers up to hexamers and pentamers, respectively. The 1-methyladenine derivative yielded linear, cyclic, and A5'ppA-derived oligonucleotides with a regioselectivity for the 3',5'-phosphodiester linkages averaging 84%. The effect of pKa and amine structure of phosphate-activating groups on the montmorillonite-catalyzed oligomerization of the 5'-phosphoramidate of adenosine are discussed. The binding and reaction of methyladenine and adenine N-phosphoryl derivatives of adenosine are described.
Permeability of membranes to amino acids and modified amino acids: mechanisms involved in translocation
The amino acid permeability of membranes is of interest because they are one of the key solutes involved in cell function. Membrane permeability coefficients (P) for amino acid classes, including neutral, polar, hydrophobic, and charged species, have been measured and compared using a variety of techniques. Decreasing lipid chain length increased permeability slightly (5-fold), while variations in pH had only minor effects on the permeability coefficients of the amino acids tested in liposomes. Increasing the membrane surface charge increased the permeability of amino acids of the opposite charge, while increasing the cholesterol content decreased membrane permeability. The permeability coefficients for most amino acids tested were surprisingly similar to those previously measured for monovalent cations such as sodium and potassium (approximately 10(-12)-10(-13) cm s-1). This observation suggests that the permeation rates for the neutral, polar and charged amino acids are controlled by bilayer fluctuations and transient defects, rather than partition coefficients and Born energy barriers. Hydrophobic amino acids were 10(2) more permeable than the hydrophilic forms, reflecting their increased partition coefficient values. External pH had dramatic effects on the permeation rates for the modified amino acid lysine methyl ester in response to transmembrane pH gradients. It was established that lysine methyl ester and other modified short peptides permeate rapidly (P = 10(-2) cm s-1) as neutral (deprotonated) molecules. It was also shown that charge distributions dramatically alter permeation rates for modified di-peptides. These results may relate to the movement of peptides through membranes during protein translocation and to the origin of cellular membrane transport on the early Earth.
Accretion of Moon and Earth and the emergence of life
The discrepancy between the impact records on the Earth and Moon in the time period, 4.0-3.5 Ga calls for a re-evaluation of the cause and localization of the late lunar bombardment. As one possible explanation, we propose that the time coverage in the ancient rock record is sufficiently fragmentary, so that the effects of giant, sterilizing impacts throughout the inner solar system, caused by marauding asteroids, could have escaped detection in terrestrial and Martian records. Alternatively, the lunar impact record may reflect collisions of the receding Moon with a series of small, original satellites of the Earth and their debris in the time period about 4.0-3.5 Ga. The effects on Earth of such encounters could have been comparatively small. The location of these tellurian moonlets has been estimated to have been in the region around 40 Earth radii. Calculations presented here, indicate that this is the region that the Moon would traverse at 4.0-3.5 Ga, when the heavy and declining lunar bombardment took place. The ultimate time limit for the emergence of life on Earth is determined by the effects of planetary accretion--existing models offer a variety of scenarios, ranging from low average surface temperature at slow accretion of the mantle, to complete melting of the planet followed by protracted cooling. The choice of accretion model affects the habitability of the planet by dictating the early evolution of the atmosphere and hydrosphere. Further exploration of the sedimentary record on Earth and Mars, and of the chemical composition of impact-generated ejecta on the Moon, may determine the choice between the different interpretations of the late lunar bombardment and cast additional light on the time and conditions for the emergence of life.
Astrobiology: exploring the origins, evolution, and distribution of life in the Universe
The search for the origins of life and its presence beyond Earth is strengthened by new technology and by evidence that life tolerates extreme conditions and that planets are widespread. Astrobiologists learn how planets develop and maintain habitable conditions. They combine biological and information sciences to decipher the origins of life. They examine how biota, particularly microorganisms, evolve, at scales from the molecular to the biosphere level, including interactions with long-term planetary changes. Astrobiologists learn how to recognize the morphological, chemical, and spectroscopic signatures of life in order to explore both extraterrestrial samples and electromagnetic spectra reflected from extrasolar planets.
From non-random molecular structure to life and mind
The evolutionary hierarchy molecular structure-->macromolecular structure-->protobiological structure-->biological structure-->biological functions has been traced by experiments. The sequence always moves through protein. Extension of the experiments traces the formation of nucleic acids instructed by proteins. The proteins themselves were, in this picture, instructed by the self-sequencing of precursor amino acids. While the sequence indicated explains the thread of the emergence of life, protein in cellular membrane also provides the only known material basis for the emergence of mind in the context of emergence of life.
Racemization and the origin of optically active organic compounds in living organisms
The organic compounds synthesized in prebiotic experiments are racemic mixtures. A number of proposals have been offered to explain how asymmetric organic compounds formed on the Earth before life arose, with the influence of chiral weak nuclear interactions being the most frequent proposal. This and other proposed asymmetric syntheses give only sight enantiomeric excess and any slight excess will be degraded by racemization. This applies particularly to amino acids where half-lives of 10(5)-10(6) years are to be expected at temperatures characteristic of the Earth's surface. Since the generation of chiral molecules could not have been a significant process under geological conditions, the origins of this asymmetry must have occurred at the time of the origin of life or shortly thereafter. It is possible that the compounds in the first living organisms were prochiral rather than chiral; this is unlikely for amino acids, but it is possible for the monomers of RNA-like molecules.
Metabolism of proteinoid microspheres
The literature of metabolism in proteinoids and proteinoid microspheres is reviewed and criticized from a biochemical and experimental point of view. Closely related literature is also reviewed in order to understand the function of proteinoids and proteinoid microspheres. Proteinoids or proteinoid microspheres have many activities. Esterolyis, decarboxylation, amination, deamination, and oxidoreduction are catabolic enzyme activities. The formation of ATP, peptides or oligonucleotides is synthetic enzyme activities. Additional activities are hormonal and inhibitory. Selective formation of peptides is an activity of nucleoproteinoid microspheres; these are a model for ribosomes. Mechanisms of peptide and oligonucleotide syntheses from amino acids and nucleotide triphosphate by proteinoid microspheres are tentatively proposed as an integrative consequence of reviewing the literature.
A new paradigm for evolution
Standard evolutionary theory sees little beyond the natural selection of random variation. Yet there is more to life.