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At least 19 records
All sourcesNASA NTRSDOE OSTI
NASA NTRS2024

Toward Prebiotic Chemistry on Titan: Impact Experiments on Organic Haze Particles

Impacts are critical to producing the aqueous environments necessary to stimulate prebiotic chemistry on Titan's surface. Furthermore, organic hazes resting on the surface are a likely feedstock of biomolecules. In this work, we conduct impact experiments on laboratory-produced organic haze particles and haze/sand mixtures and analyze these samples for life's building blocks. Samples of unshocked haze and sand particles are also analyzed to determine the change in biomolecule concentrations and distributions from shocking. Across all samples, we detect seven nucleobases, nine proteinogenic amino acids, and five other biomolecules (e.g., urea) using a blank subtraction procedure to eliminate signals due to contamination. We find that shock pressures of 13 GPa variably degrade nucleobases, amino acids, and a few other organics in haze particles and haze/sand mixtures; however, certain individual biomolecules become enriched or are even produced from these events. Xanthine, threonine, and aspartic acid are enriched or produced in impact experiments containing sand, suggesting these minerals may catalyze the production of these biomolecules. On the other hand, thymine and isoleucine/norleucine are enriched or produced in haze samples containing no sand, suggesting catalytic grains are not necessary for all impact shock syntheses. Uracil, glycine, proline, cysteine, and tyrosine are the most unstable to impact-related processing. These experiments suggest that impacts alter biomolecule distributions on Titan's surface, and that organic hazes co-occurring with fine-grained material on the surface may provide an initial source for further prebiotic chemistry on Titan.

impact experiments↗
NASA NTRS1980

Infrared laser photolysis - A new tool for the study of prebiotic chemistry

Infrared laser induced dielectric breakdown and multiphoton absorption experiments on CH4/NH3 'atmospheres' are described. It is found that HCN, a central intermediate in prebiotic chemistry, is a principal product. This, combined with the fact that dielectric breakdown appears to have much in common with ordinary electric sparks, suggests that the laser could be a useful tool in studies of prebiotic chemistry. Several possible experiments in this vein are suggested.

Davis, D. D.↗
NASA NTRS1991

Prebiotic chemistry in clouds

The chemical evolution hypothesis of Woese (1979), according to which prebiotic reactions occurred rapidly in droplets in giant atmospheric reflux columns was criticized by Scherer (1985). This paper proposes a mechanism for prebiotic chemistry in clouds that answers Scherer's concerns and supports Woese's hypothesis. According to this mechanism, rapid prebiotic chemical evolution was facilitated on the primordial earth by cycles of condensation and evaporation of cloud drops containing clay condensation nuclei and nonvolatile monomers. For example, amino acids supplied by, or synthesized during entry of meteorites, comets, and interplanetary dust, would have been scavenged by cloud drops containing clay condensation nuclei and would be polymerized within cloud systems during cycles of condensation, freezing, melting, and evaporation of cloud drops.

Oberbeck, Verne R.↗
NASA NTRS2020

Extraterrestrial Hexamethylenetetramine in Meteorites - A Precursor of Prebiotic Chemistry in the Solar System

Despite extensive studies on the formation of organic molecules in various extraterrestrial environments, it still remains under debate when, where, and how such molecules were abiotically formed. A key molecule to solve the problem, hexamethylenetetramine (HMT) has not been confirmed in extraterrestrial materials despite extensive laboratory experimental evidence that it can be produced in interstellar or cometary environments. Here we report the first detection of HMT and functionalized HMT species in the carbonaceous chondrites Murchison, Murray, and Tagish Lake. While the part-per-billion level concentration of HMT in Murchison and Tagish Lake is comparable to other related soluble organic molecules, like amino acids, these compounds may have eluded detection in previous studies due to the loss of HMT during the extraction processes. HMT, which can yield important molecules for prebiotic chemistry such as formaldehyde and ammonia upon degradation, is a likely pre-cursor of meteoritic organic compounds of astrochemical and astrophysical interests.

Yasuhiro Oba↗
NASA NTRS2022

Chirality in Organic and Mineral Systems: A Review of Reactivity and Alteration Processes Relevant to Prebiotic Chemistry and Life Detection Missions

Chirality is a central feature in the evolution of biological systems, but the reason for biology’s strong preference for specific chiralities of amino acids, sugars, and other molecules remains a controversial and unanswered question in origins of life research. Biological polymers tend toward homochiral systems, which favor the incorporation of a single enantiomer (molecules with a specific chiral configuration) over the other. There have been numerous investigations into the processes that preferentially enrich one enantiomer to understand the evolution of an early, racemic, prebiotic organic world. Chirality can also be a property of minerals; their interaction with chiral organics is important for assessing how post-depositional alteration processes could affect the stereochemical configuration of simple and complex organic molecules. In this paper, we review the properties of organic compounds and minerals as well as the physical, chemical, and geological processes that affect organic and mineral chirality during the preservation and detection of organic compounds. We provide perspectives and discussions on the reactions and analytical techniques that can be performed in the laboratory, and comment on the state of knowledge of flight-capable technologies in current and future planetary missions, with a focus on organics analysis and life detection.

chirality↗
NASA NTRS2016

Carbon Monoxide and the Potential for Prebiotic Chemistry on Habitable Planets Around Main Sequence M Stars

Lifeless planets with CO2 atmospheres produce CO by CO2 photolysis. On planets around M dwarfs, CO is a long-lived atmospheric compound, as long as UV emission due to the stars chromospheric activity lasts, and the sink of CO and O2 in seawater is small compared to its atmospheric production. Atmospheres containing reduced compounds, like CO, may undergo further energetic and chemical processing to give rise to organic compounds of potential importance for the origin of life. We calculated the yield of organic compounds from CO2-rich atmospheres of planets orbiting M dwarf stars, which were previously simulated by Domagal- Goldman et al. (2014) and Harman et al. (2015), by cosmic rays and lightning using results of experiments by Miyakawaet al. (2002) and Schlesinger and Miller (1983a, 1983b). Stellar protons from active stars may be important energy sources for abiotic synthesis and increase production rates of biological compounds by at least 2 orders of magnitude compared to cosmic rays. Simple compounds such as HCN and H2CO are more readily synthesized than more complex ones, such as amino acids and uracil (considered here as an example), resulting in higher yields for the former and lower yields for the latter. Electric discharges are most efficient when a reducing atmosphere is present. Nonetheless, atmospheres with high quantities of CO2 are capable of producing higher amounts of prebiotic compounds, given that CO is constantly produced in the atmosphere. Our results further support planetary systems around M dwarf stars as candidates for supporting life or its origin.

M stars↗
NASA NTRS1975

Quantum chemical study of relative reactivities of a series of amines and nitriles - Relevance to prebiotic chemistry

Using the Iterative Extended Huckel Theory (IEHT) calculations of the electron distribution and orbital energies of a series of thirteen amines, nitriles and amino-nitriles relevant to prebiotic and cosmo-chemistry have been carried out. Ground state properties such as the energy and nature of the highest occupied (HOMO) and lowest empty (LEMO) molecular orbitals, net atomic charges and number of nonbonding electrons have been identified as criteria for correlating the relative nucleophilicity of amine and nitrile nitrogens and the electrophilicity of nitrile and other unsaturated carbon atoms. The results of such correlations can be partially verified by known chemical behavior of these compounds and are used to predict and understand their role in prebiotic organic synthesis.

Loew, G. H.↗
NASA NTRS1984

The prebiotic chemistry of nucleotides

Diminosuccinonitrile (DISN), formed by the oxidation of diaminomaleonitrile, has been investigated as a potential prebiotic phosphorylating agent. DISN affects the cyclization of 3'-adenosine monophosphate to adenosine 2',3'-cyclic phosphate in up to 39 percent yield. The mechanism of this reaction was investigated. The DISN-mediated phosphorylation of uridine to uridine monophosphate does not proceed efficiencly in aqueous solution. The reaction of DISN with uridine-5'-phosphate and uridine results in the formation of 2,2'-anhydronucleotides and 2,2'-anhydronucleosides respectively, and other reaction products resulting from an initial reaction at the 2'- and 3'-hydroxyl groups. The clay mineral catalysis of the cyclization of adenosine-3'-phosphate was investigated using homoionic montmorillonites.

Ferris, J. P.↗
NASA NTRS1992

The cometary contribution to prebiotic chemistry

The chemical composition of cometary nuclei is examined to estimate the potential contribution of volatiles to the prebiotic earth from cometary collisions. Observations of cometary nuclei are reviewed to describe the chemical evolution of the objects and their theoretical potential for affecting the terrestrial environment. Specific attention is given to the plausibility of the single-impact formation of the earth-moon system, and experiments are proposed for testing the present theories. It is proposed that significant contributions of biogenic elements such as C, H, N, O, P, and S resulted from these nuclei colliding with the earth. Observations of the solar atmosphere and of the circumstellar shells of C-rich stars indicate that compounds such as CO, C2, and H2O were not pyrolyzed as a result of collision events. The compounds are theorized to have established the foundation for the abiotic synthesis of key biochemical molecules.

Oro, J.↗
NASA NTRS1974

Prebiotic chemistry and nucleic acid replication

Recent work is reviewed on some reactions that could have occurred on the primitive earth and that could have played a part in the evolution of a self-replicating system. The transition from the primitive atmosphere to the simplest replicating molecules is considered in four stages: (1) the formation of a 'prebiotic soup' of organic precursors, including the purine and pyrimidine bases and the pentose sugars; (2) the condensation of these precursors and inorganic phosphate to form monomeric nucleotides and activated nucleotide derivatives; (3) the polymerization of nucleotide derivatives to oligonucleotides; and (4) the complementary replication of oligonucleotides in a template-directed process that depends on Watson-Crick base pairing.

Orgel, L. E.↗
NASA NTRS1984

The cometary connection with prebiotic chemistry

The latent heat of water ice has been established to control the sublimation of most cometary nuclei. The next most abundant molecules are CO and/or CO2, typically reaching 10-30 percent of the water content. The other species are in the range of 1-10 percent or less and include the newly discovered NH3. HCN and CH3CN are two other important prebiotic molecules present at a comparable (1 percent) level. Attention is drawn to similarities between these compositions and those inferred for the primordial earth.

Delsemme, A. H.↗
NASA NTRS2012

Atmospheric Prebiotic Chemistry and Organic Hazes

Earth's atmospheric composition at the time of the origin of life is not known, but it has often been suggested that chemical transformation of reactive species in the atmosphere was a significant source of pre biotic organic molecules. Experimental and theoretical studies over the past half century have shown that atmospheric synthesis can yield molecules such as amino acids and nucleobases, but these processes are very sensitive to gas composition and energy source. Abiotic synthesis of organic molecules is more productive in reduced atmospheres, yet the primitive Earth may not have been as reducing as earlier workers assumed, and recent research has reflected this shift in thinking. This work provides a survey of the range of chemical products that can be produced given a set of atmospheric conditions, with a particular focus on recent reports. Intertwined with the discussion of atmospheric synthesis is the consideration of an organic haze layer, which has been suggested as a possible ultraviolet shield on the anoxic early Earth. Since such a haze layer - if formed - would serve as a reservoir for organic molecules, the chemical composition of the aerosol should be closely examined. The results highlighted here show that a variety of products can be formed in mildly reducing or even neutral atmospheres, demonstrating that contributions of atmospheric synthesis to the organic inventory on early Earth should not be discounted. This review intends to bridge current knowledge of the range of possible atmospheric conditions in the prebiotic environment and pathways for synthesis under such conditions by examining the possible products of organic chemistry in the early atmosphere.

Trainer, Melissa G.↗
NASA NTRS2011

New Insights into Prebiotic Chemistry from Old Archived Miller Extracts

Following the discovery of an archived set of samples from Stanley Miller's early experiments, analyses were undertaken to better understand the diversity of compounds produced from electric discharges acting on reducing gas mixtures. The paper chromatography methods that Miller used in the 1950s were only capable of detecting a few amino acids and were unable to provide substantial quantitative data relative to today's techniques. Current analytical techniques are much more sensitive and selective, and are capable of precisely quantifying a much larger range of amino acids and their enantiomeric abundances. In one study, preserved dried samples produced by Miller using a lesser-known volcanic apparatus which differed from Miller's classic apparatus in that it utilized an aspirator that injected steam into the electric discharge chamber, simulating a volcanic eruption. The volcanic apparatus produced a wider variety of amino acids than the classic configuration. Prebiotic compounds synthesized in these environments may have locally accumulated where they could have undergone further processing. An additional preserved set of samples from an experiment conducted in 1958 were also found in Miller's archived collection. These samples which had been generated using a mixture of CH4, NH3, H2S and CO2 were collected, catalogued, and stored by Miller, but for unknown reasons were never studied. In our analyses a total of 23 amino acids and 4 amines, including 7 organosulfur compounds, were detected in these samples. The major amino acids with chiral centers are racemic within the accuracy of the measurements, indicating that they are not contaminants introduced during sample storage. This experiment marks the first synthesis of sulfur amino acids from spark discharge experiments designed to imitate primordial environments. The relative yield of some amino acids, in particular the isomers of amino butyric acid, are the highest ever found in a spark discharge experiment. The simulated primordial conditions used by Miller in these experiments may serve as a model for early volcanic plume chemistry and provide insight to the possible roles such plumes may have played in abiotic organic synthesis. Additionally, the overall abundances of the synthesized amino acids in the presence of H2S are very similar to the abundances found in some carbonaceous meteorites, suggesting that H2S may have played an important role in prebiotic reactions in early solar system environments. Although experiments using a variety of gases as components of the primordial Earth's atmospheric composition and a spark discharge apparatus configured according to Miller's original or volcanic design can be readily carried out, the unique opportunity to investigate samples prepared by the pioneer in abiotic synthesis using state of the art analytical methods is of considerable historic interest.

Parker, Eric T.↗
NASA NTRS2004

Impact-shocked rocks--insights into Archean and extraterrestrial microbial habitats (and sites for prebiotic chemistry?)

Impact-shocked gneiss shocked to greater than 10 GPa in the Haughton impact structure in the Canadian High Arctic has an approximately 25-times greater pore surface area than unshocked rocks. These pore spaces provide microhabitats for a diversity of heterotrophic microorganisms and in the near-surface environment of the rocks, where light levels are sufficient, cyanobacteria. Shocked rocks provide a moisture retaining, UV protected microenvironment. During the Archean, when impact fluxes were more than two orders of magnitude higher than today, the shocked-rock habitat was one of the most common terrestrial habitats and might have provided a UV-shielded refugium for primitive life. These potential habitats are in high abundance on Mars where impact crater habitats could have existed over geologic time periods of billions of years, suggesting that impact-shocked rocks are important sites to search for biomolecules in extraterrestrial life detection strategies. In addition to being favourable sites for life, during the prebiotic period of planetary history impact-shocked rocks might have acted as a site for the concentration of reactants for prebiotic syntheses. c2004 COSPAR. Published by Elsevier Ltd. All rights reserved.

Evolution, Chemical↗
DOE OSTI2024

Modeling prebiotic chemistries with quantum accuracy at classical costs

Molecular Dynamics (MD) simulations using classical force-fields are commonly employed in numerous scientific investigations. However, many natural processes involve bond breaking and quantum forces. This complexity is compounded by the presence of multiple competing length and timescales. For example, accurately modeling the thermodynamics and dynamics of a chemical reaction requires accounting for the concerted movements of numerous solvent molecules and ions with their own fast or slow timescales. While widely used static Density Functional Theory (DFT) calculations at 0 temperature can be beneficial for such investigations, they do not account for dynamics, and lack precision in describing the molecular environments. They particularly fail at correct, rigorous treatments of finite-temperature fluctuations, and thus generalization to experimentally relevant conditions. In PNAS Benayad et al develop a scalable, generalizable approach for designing Neural Network Potentials (NNPs) that can handle chemical reactivity in solvated systems with quantum accuracy at classical costs. Specifically, they study phosphoester bond formation and rupture, which is fundamentally relevant to the Phosphorus-Oxygen bond formation central to life, and especially for the RNA world hypothesis. The framework developed here has the potential to generalize to different chemical reactions of energy and biological relevance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗