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83 records · Page 5
All sourcesNASA NTRSDOE OSTI
NASA NTRS2016

Mechanisms for the Formations of the Thymine Under Astrophysical Conditions and Implications for the Origin of Life

Nucleobases are the carriers of the genetic information in ribonucleic acid and deoxyribonucleic acid (DNA) for all life on Earth. Their presence in meteorites clearly indicates that compounds of biological importance can form via non-biological processes in extraterrestrial environments. Recent experimental studies have shown that the pyrimidine-based nucleobases uracil and cytosine can be easily formed from the ultraviolet irradiation of pyrimidine in H2O-rich ice mixtures that simulate astrophysical processes. In contrast, thymine, which is found only in DNA, is more difficult to form under the same experimental conditions, as its formation usually requires a higher photon dose. Earlier quantum chemical studies confirmed that the reaction pathways were favorable provided that several H2O molecules surrounded the reactants. However, the present quantum chemical study shows that the formation of thymine is limited because of the inefficiency of the methylation of pyrimidine and its oxidized derivatives in an H2O ice, as supported by the laboratory studies. Our results constrain the formation of thymine in astrophysical environments and thus the inventory of organic molecules delivered to the early Earth and have implications for the role of thymine and DNA in the origin of life.

Origin↗
NASA NTRS2017

The Formation of Nucleobases from the UV Irradiation of Astrophysical Ice Analogs

Nucleobases are the fundamental information bearing components of both RNA and DNA. They are central to all known terrestrial life and they are generally conserved between species. Biological nucleobases can be divided into two groups based on the N-heterocyclic molecules pyrimidine (uracil, cytosine, and thymine) and purine (adenine and guanine) respectively. Do date, no experimental conditions have been determined that could produce both pyrimidines and purines together, abiotically, in a ter-restrial environment or an early terrestrial analog. Organic materials produced in extraterrestrial envi-ronments may have been delivered to the primitive earth by comets and meteorites and may have contrib-uted to the emergence of life. To date, some, but not all nucleobases have been detected in meteorites and their isotopic signatures may be consistent with an extraterrestrial origin. Earlier work in our lab demonstrated that it is possible to produce all of the pyrimidine group nucleobases from the UV-irradiation of pyrimidine in astrophysically relevant ice analogs. Here we report our most recent work, which studied the formation of the purine group nucleobases under similar conditions.

Astrophysical Ice↗
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 NTRS2018

The Photochemistry of Purine in Ice Analogs Relevant to Dense Interstellar Clouds

The aromatic nitrogen heterocyclic compound purine is the core structural framework of many important biomolecules, particularly nucleobases. Purine and purine derivatives have been observed in carbonaceous chondrites, and it has been hypothesized that the exogenous delivery of these compounds, along with many other biologically relevant compounds, may have played a role in the emergence of life. Numerous experiments in our laboratory have demonstrated that the nucleobases used by life to encode genetic material could have been produced abiotically under astrophysically relevant conditions. Specically, the UV photoprocessing of pyrimidine and purine in simple ices of astrophysical interest has resulted in the production of all five biological nucleobases, namely, uracil (RNA), cytosine (RNA and DNA), thymine (DNA), adenine (RNA and DNA), and guanine (RNA and DNA). Additionally, follow-up work has examined the photochemistry of pyrimidine in more complex astrophysical ice mixtures to better understand the formation of these compounds under realistic conditions. In this work, we examine the photochemistry of purine in more complex ices of astrophysical interest and compare our results with those from simpler ice mixtures. We also examine the effects of competing parallel synthesis of organic compounds in the ices (unrelated to purine). Finally, we discuss the astrophysical and astrobiological implications of our findings.

Molecular Processes↗
NASA NTRS2019

Prebiotic Chemistry of Pluto

We present the case for the presence of complex organic molecules, such as amino acids and nucleobases, formed by abiotic processes on the surface and in near-subsurface regions of Pluto. Pluto's surface is tinted with a range of non-ice substances with colors ranging from light yellow to red to dark brown; the colors match those of laboratory organic residues called tholins. Tholins are broadly characterized as complex, macromolecular organic solids consisting of a network of aromatic structures connected by aliphatic bridging units (e.g., Imanaka et al.,2004; Materese et al.,2014, 2015). The synthesis of tholins in planetary atmospheres and in surface ices has been explored in numerous laboratory experiments, and both gas- and solid-phase varieties are found on Pluto. A third variety of tholins, exposed at a site of tectonic surface fracturing called Virgil Fossae, appears to have come from a reservoir in the subsurface. Eruptions of tholin-laden liquid H2O from a subsurface aqueous repository appear to have covered portions of Virgil Fossae and its surroundings with a uniquely colored deposit (D.P. Cruikshank, personal communication) that is geographically correlated with an exposure of H2O ice that includes spectroscopically detected NH3 (C.M. Dalle Ore, personal communication). The subsurface organic material could have been derived from presolar or solar nebula processes, or might have formed in situ. Photolysis and radiolysis of a mixture of ices relevant to Pluto's surface composition (N2, CH4, CO) have produced strongly colored, complex organics with a significant aromatic content having a high degree of nitrogen substitution similar to the aromatic heterocycles pyrimidine and purine (Materese et al.,2014, 2015; Cruikshank et al.,2016). Experiments with pyrimidines and purines frozen in H2O-NH3 ice resulted in the formation of numerous nucleobases, including the biologically relevant guanine, cytosine, adenine, uracil, and thymine (Materese et al.,2017). The red material associated with the H2O ice may contain nucleobases resulting from energetic processing on Pluto's surface or in the interior. Some other Kuiper Belt objects also exhibit red colors similar to those found on Pluto and may therefore carry similar inventories of complex organic materials. The widespread and ubiquitous nature of similarly complex organic materials observed in a variety of astronomical settings drives the need for additional laboratory and modeling efforts to explain the origin and evolution of organic molecules. Pluto observations reveal complex organics on a small body that remains close to its place of origin in the outermost regions of the Solar System.

Cruikshank, D. P.↗
NASA NTRS2021

Evidence for the Protection of N-heterocycles from Gamma Radiation by Mars Analogue Minerals

Organic compounds have been delivered to the surface of Mars via meteorites, comets and interplanetary dust particles for billions of years. Determining the effects of high energy radiation and galactic cosmic radiation (GCR) on these organic compounds is critical for understanding the potential for the preservation of organic molecules associated with past or present life, and where to look for possible chemical bio- signatures during future Mars missions. Understanding how these effects are attenuated by the mineral matrix and the depth at which they are buried have been challenging to determine in situ on Mars. There have been very few experimental studies on the survival of organic compounds under radiation from a gamma source under realistic conditions, and their interpretation until now has been difficult due to the lack of data for actual radiation levels on Mars. Using the in-situ data obtained by the MSL/RAD instrument to anchor the dose calculations, here we show that the N-heterocycles purine and uracil, crucial components of biochemical processes in extant living systems, mixed with calcite, anhydrite, and kaolinite as Mars analogue minerals can survive the effects of radiation with a dose corresponding to ~500,000 years on the Martian surface. The extent of survival varied not only with the nature of the organic compound, but its depth from the surface. These results provide new experimental data for the degree of protection offered by the regolith, in conjunction with minerals, for organic compounds that may be present on Mars.

mars↗
NASA NTRS2022

Identifying the Wide Diversity of Extraterrestrial Purine and Pyrimidine Nucleobases in Carbonaceous Meteorites

The lack of pyrimidine diversity in meteorites remains a mystery since prebiotic chemical models and laboratory experiments have predicted that these compounds can also be produced from chemical precursors found in meteorites. Here we report the detection of nucleobases in three carbonaceous meteorites using state-of-the-art analytical techniques optimized for small-scale quantification of nucleobases down to the range of parts per trillion (ppt). In addition to previously detected purine nucleobases in meteorites such as guanine and adenine, we identify various pyrimidine nucleobases such as cytosine, uracil, and thymine, and their structural isomers such as isocytosine, imidazole-4-carboxylic acid, and 6-methyluracil, respectively. Given the similarity in the molecular distribution of pyrimidines in meteorites and those in photon-processed interstellar ice analogues, some of these derivatives could have been generated by photochemical reactions prevailing in the interstellar medium and later incorporated into asteroids during solar system formation. This study demonstrates that a diversity of meteoritic nucleobases could serve as building blocks of DNA and RNA on the early Earth.

Yasuhiro Oba↗
NASA NTRS2018

The Photochemistry of Purine in Ice Analogs Relevant to Dense Interstellar Clouds

The aromatic nitrogen heterocyclic compound purine is the core structural framework of many important biomolecules, particularly nucleobases. Purine and purine derivatives have been observed in carbonaceous chondrites, and it has been hypothesized that the exogenous delivery of these compounds, along with many other biologically relevant compounds, may have played a role in the emergence of life. Numerous experiments in our laboratory have demonstrated that the nucleobases used by life to encode genetic material could have been produced abiotically under astrophysically relevant conditions. Specifically, the UV photoprocessing of pyrimidine and purine in simple ices of astrophysical interest has resulted in the production of all five biological nucleobases, namely, uracil (RNA), cytosine (RNA and DNA), thymine (DNA), adenine (RNA and DNA), and guanine (RNA and DNA). Additionally, follow-up work has examined the photochemistry of pyrimidine in more complex astrophysical ice mixtures to better understand the formation of these compounds under realistic conditions. In this work, we examine the photochemistry of purine in more complex ices of astrophysical interest and compare our results with those from simpler ice mixtures. We also examine the effects of competing parallel synthesis of organic compounds in the ices (unrelated to purine). Finally, we discuss the astrophysical and astrobiological implications of our findings.

Astrobiology↗
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↗
DOE OSTI2020

Unraveling the mechanism of recognition of the 3’ splice site of the adenovirus major late promoter intron by the alternative splicing factor PUF60

Pre-mRNA splicing is critical for achieving required amounts of a transcript at a given time and for regulating production of encoded protein. A given pre-mRNA may be spliced in many ways, or not at all, giving rise to multiple gene products. Numerous splicing factors are recruited to pre-mRNA splice sites to ensure proper splicing. One such factor, the 60 kDa poly(U)-binding splicing factor (PUF60), is recruited to sites that are not always spliced, but rather function as alternative splice sites. In this study, we characterized the interaction of PUF60 with a splice site from the adenovirus major late promoter (the AdML 3' splice site, AdML3’). We found that the PUF60–AdML3’ dissociation constants are in the micromolar range, with the binding affinity predominantly provided by PUF60’s two central RNA recognition motifs (RRMs). A 1.95 Å crystal structure of the two PUF60 RRMs in complex with AdML3’ revealed a dimeric organization placing two stretches of nucleic acid tracts in opposing directionalities, which can cause looping of nucleic acid and explain how PUF60 affects pre-mRNA geometry to effect splicing. Solution characterization of this complex by light-scattering and UV/Vis spectroscopy suggested a potential 2:1 (PUF60 2 :AdML3’) stoichiometry, consistent with the crystal structure. This work defines the sequence specificity of the alternative splicing factor PUF60 at the pre-mRNA 3’ splice site. Our observations suggest that control of pre-mRNA directionality is important in the early stage of spliceosome assembly, and advance our understanding of the molecular mechanism by which alternative and constitutive splicing factors differentiate among 3’ splice sites.

59 BASIC BIOLOGICAL SCIENCES↗