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Chang, S.

Publications and source records attributed to Chang, S..

At least 55 records · Page 3

Dynamic thermal episodes in the protosolar nebula: Development of models from observations on CAI's

Evaluation of earlier observations indicated that layered rims on coarse-grained Allende CAI's were possibly the result of partial melting by ablation/drag-heating and reaction of CAI exteriors with a gas or gases of non-solar composition. Bunch and Chang reported the common occurrence of thin, fine-grained, matrix-like bands that at least partially surround rims of CAI's. Although material in these bands in general appears to be similar to matrix, SEM observations show them to be dissimilar in volatile element content, mineral composition, and grain morphology. Moreover, they appear to be related in time of formation with rim development and Na-metasomatism of CAI's. Observations indicate a short-lived but intense heating episode followed by radid cooling as the mechanism responsible for these CAI features.

Bunch, T. E.↗

Photochemical reactions of water and carbon monoxide in earth's primitive atmosphere

The gas-phase photolysis of H2O at 1849 A in the presence of CO yields mainly CO2 and H2 and a variety of organic compounds, including C1-C3 hydrocarbons, alcohols, aldehydes, acetone, and acetic acid. The overall quantum yield for conversion of CO to organic compounds varies between 0.23 and 0.03 as a function of the CO abundance. These results indicate that even if primitive earth's atmosphere initially contained no molecular hydrogen and contained carbon only in the form of CO or a mixture of CO and CO2, the prebiotic environment would have become enriched with a variety of organic compounds produced by photochemical processes.

Bar-Nun, A.↗

Prebiotic organic syntheses and the origin of life

The outline of a modern paradigm for the origins of life on earth was first formulated by Oparin (1924). According to the considered hypothesis, living organisms arose naturally on the primitive earth through a lengthy process of chemical evolution of organic matter which began in the atmosphere and culminated in the primordial seas. Details regarding the chemical evolution paradigm are discussed, and chemical evolutionary processes formulated by principal contributors are reviewed in a historical context. Attention is given to the Oparin model of the prebiotic earth, the Urey model, the Rubey model, a multistage model for early atmospheric evolution, and other variations on the theme of prebiotic atmospheres. Evidence in support of the chemical evolution paradigm is considered along with modern models regarding the accretion of earth and the formation of its core, and problems and prospects for future studies.

Chang, S.↗

The possible role of soluble salts in chemical evolution

A model for a prebiotic environment in which concentration, condensation, and chemical evolution of biomolecules could have occurred is proposed. The principal reactions expected of proteins, nucleic acids, lipids, and some of their precursors in this environment are discussed. The model is based on the concept of a fluctuating system in which hydration and dehydration processes occur in a cyclic manner, with allowance for high concentrations of soluble salts, such as chlorides and sulfates. It is concluded that the proposed prebiotic environment with its dynamical characteristics is a plausible model for the chemical evolution from biomonomers through random oligomers toward self-replicating chemical systems.

Lahav, N.↗

Prebiotic organic matter - Possible pathways for synthesis in a geological context

Models for the accretion of the earth, core formation, differentiation of the planet into core, mantle, crust, and atmosphere, and prebiotic synthesis of organic materials are reviewed. The development of the Haldane-Oparin and Urey models is traced, and the effect of accretion time on the outgassing process and the composition of the consequent atmosphere is examined. Model prebiotic atmospheres are calculated, the extent of equilibration of the primitive atmosphere is studied and the evolution of the atmosphere prior to organic chemical evolution is reviewed. Finally, experimental progress in synthesis of biological monomers and polymers under presumed early earth conditions is covered.

Chang, S.↗

Hydrazines and carbohydrazides produced from oxidized carbon in earth's primitive environment

Whether abiological organic compounds can be formed from the interactions of energy sources with nitrogen, oxidized carbon and water is held to be of importance in geochemical models of the primordial earth atmosphere. It is reported that experiments using quenched spark discharges through molecular nitrogen on aqueous suspensions of CaCO3 and other reactants to simulate the hydrosphere/atmosphere interface yield hydrazine and carbohydrazine in significant but low yields. Such reactions in primitive aquatic environments may have supplied a pathway for chemical evolution and the origin of life, on a primitive earth in which fully oxidized states of carbon were available for the primary synthesis of organic matter.

Folsome, C. E.↗

Noble-gas-rich separates from the Allende meteorite

Predominantly carbonaceous HF/HCl-resistant residues from the Allende meteorite are studied. Samples are characterized by SEM/EDXA, X-ray diffraction, INAA, C, S, H, N, and noble gas analyses. Isotopic data for carbon show variations no greater than 5%, while isotopic data from noble gases confirm previously established systematics. Noble gas abundances correlate with those of C and N, and concomitant partial loss of C and normal trapped gas occur during treatments with oxidizing acids. HF/HCl demineralization of bulk meteorite results in similar fractional losses of C and trapped noble gases, which leads to the conclusion that various macromolecular carbonaceous substances serve as the main host phase for normal trapped noble gases and anomalous gases in acid-resistant residues, and as the carrier of the major part of trapped noble gases lost during HF/HCl demineralization. Limits on the possible abundances of dense mineralic host phases in the residues are obtained, and considerations of the nucleogenetic origin for CCF-XE indicate that carbonaceous host phases and various forms of organic matter in carbonaceous meteorites may have a presolar origin.

Ott, U.↗

Semiempirical hot atom theory. I - Initialization and application

A semiempirical approach to the modeling of the kinetics of reaction systems containing both hot and nonhot atoms is proposed. The approach is based on the probabilistic kinetic theory of hot-atom reactions formulated by Wolfgang (1963), with transmission probabilities estimated for a rectangular potential barrier for hot-atom and nonhot-atom reactions. A computational scheme for determining product concentrations following hot and nonhot reactions in a system containing photolytically produced hot atoms is then applied to the DBr + CH4 and HBr + CD4 hot hydrogen atom systems studied by Martin and Willard (1964), and good agreement is obtained between theoretical and experimental results.

Aronowitz, S.↗

Organic chemical evolution

The course of organic chemical evolution preceding the emergence of life on earth is discussed based on evidence of processes occurring in interstellar space, the solar system and the primitive earth. Following a brief review of the equilibrium condensation model for the origin and evolution of the solar system, consideration is given to the nature and organic chemistry of interstellar clouds, comets, Jupiter, meteorites, Venus and Mars, and the prebiotic earth. Major issues to be resolved in the study of organic chemical evolution on earth are identified regarding condensation and accretion in the solar nebula, early geological evolution, the origin and evolution of the atmosphere, organic production rates, organic-inorganic interactions, environmental fluctuations, phase separation and molecular selectivity.

Chang, S.↗

High spectral resolution airborne spectrometry

An airborne spectroradiometer system developed at Columbia University has been providing new spectral data for use in remote sensing for natural resources. The system has been improved by addition of a solid state silicon detector array, and has been extended into the infrared by addition of a 64 element lead sulfide detector array. The infrared data in the 2000 to 2500 nm region especially holds large potential for mineral and oil exploration.

Collins, W.↗

Behavior of molecules on interstellar grains - Application of the Langevin equation and iterative extended Hueckel

The Langevin equation was used to explore an adsorbate desorption mechanism. Calculations were performed using iterative extended Hueckel on a silica model site with various small adsorbates, e.g., H, CH, OH, NO, CO. It was found that barriers to free traversal from one site to another are substantial (about 3-10 eV). A bootstrap desorption mechanism for some molecules in the process of forming at a site also became apparent from the calculations. The desorption mechanisms appear to be somewhat balanced by a counterforce - the attraction of sites for the newly desorbed molecule. The order of attraction to a silica grain site for the diatomic molecules considered was OH greater than CH greater than CO greater than NO, when these entities were sufficiently distant. The nature of the silica grain and that of the 'cold' desorption mechanism, when considered together, suggest that the abundance of very small grains might be less common than anticipated.

Aronowitz, S.↗

Carbonaceous chondrites. II - Carbonaceous chondrite phyllosilicates and light element geochemistry as indicators of parent body processes and surface conditions

Petrographic analyses of CM matrices characterized four phyllosilicates in Murray and Murchison meteorites and Fe- and Mg-serpentines in Nogoya. All phyllosilicates and bulk matrices show enrichment of K relative to Na when compared with bulk meteorites; the loss of Na and some Cl, and the addition of H2O, CO2, and water-soluble organics during alteration indicates a partially open system. Synthesis of soluble organic materials may have occurred in CM matrices before aqueous alteration of the precursive phases. Nogoya was 95% altered and has a bulk C content of 5.2%, higher than any meteorite; also, it has the lowest measured C-13/C-12 ratio of any carbonaceous chondrite except for Karoonda.

Bunch, T. E.↗

Modified Iterative Extended Hueckel. 2: Application to the interaction of Na(+), Na(+)(aq.), Mg(+)-2(aq.) with adenine and thymine

Modified Iterative Extended Hueckel, which includes explicit effective internuclear and electronic interactions, is applied to the study of the energetics of Na(+),Mg(+), Na(+) (aqueous), and Mg(+2) (aqueous) ions approaching various possible binding sites on adenine and thymine. Results for the adenine + ion and thymine + ion are in good qualitative agreement with ab initio work on analogous systems. Energy differences between competing sites are in excellent agreement. Hydration appears to be a critical factor in determining favorable binding sites. That the adenine Nl and N3 sites cannot displace a water molecule from the hydrated cation indicates that they are not favorable binding sites in aqueous media. Of those sites investigated, 04 was the most favorable binding site on the thymine for the bare Na(+). However, the 02 site was the most favorable binding site for either hydrated cation.

Aronowitz, S.↗

Carbonaceous chondrites. I - Characterization and significance of carbonaceous chondrite /CM/ xenoliths in the Jodzie howardite

Mineralogical, chemical, textural, and isotopic studies of the abundant carbonaceous inclusions in the Jodzie howardite which are consistent with carbonaceous chondrite (CM) characteristics are examined. These CM xenoliths show regolith alteration comparable to the Murray and Murchison meteorites but less than Nogoya, flow-oriented development of phyllosilicates and 'poorly characterized phases', and partial oxidation of sulfides. Temperature-programmed pyrolysis mass spectrometry indicates that gas release patterns of volatiles and hydrocarbons, and N, C, and S contents are typical of CM meteorites. The fact that the Ne content is typical for 'solar' values and the isotopic structure of Xe is 'planetary' indicates that these gases were entrapped by different mechanisms, and cosmic ray exposure ages for the xenoliths agree with the reported exposure age for the eucritic host.

Bunch, T. E.↗

Organic chemistry on Titan

Features taken from various models of Titan's atmosphere are combined in a working composite model that provides environmental constraints within which different pathways for organic chemical synthesis are determined. Experimental results and theoretical modeling suggest that the organic chemistry of the satellite is dominated by two processes: photochemistry and energetic particle bombardment. Photochemical reactions of CH4 in the upper atmosphere can account for the presence of C2 hydrocarbons. Reactions initiated at various levels of the atmosphere by cosmic rays, Saturn 'wind', and solar wind particle bombardment of a CH4-N2 atmospheric mixture can account for the UV-visible absorbing stratospheric haze, the reddish appearance of the satellite, and some of the C2 hydrocarbons. In the lower atmosphere photochemical processes will be important if surface temperatures are sufficiently high for gaseous NH3 to exist. It is concluded that the surface of Titan may contain ancient or recent organic matter (or both) produced in the atmosphere.

Chang, S.↗

Prebiotic nucleotide oligomerization in a fluctuating environment - Effects of kaolinite and cyanamide

The clay kaolinite was tested for its ability to promote nucleotide oligomerization in model prebiotic systems. Heterogeneous mixtures of clay, water and nucleotide were repeatedly evaporated to dryness at 60 C and redissolved in water in cyclic fashion in the presence or absence of cyanamide and/or ammonium chloride. With or without cycling, kaolinite alone did not promote the oligomerization of nucleotides at detectable levels. Cycling of clay in combination with cyanamide, however, promoted high levels of condensation to a mixture of oligonucleotides and dinucleotide pyrophosphate without requiring ammonium chloride. Although cycling with clay favored synthesis of dinucleotide pyrophosphate, cycling without clay enhanced formation of oligonucleotides. These results support the hypothesis that the presence of clays in fluctuating environments would have influenced the course of prebiotic condensation reactions.

Odom, D. G.↗

Comets: Cosmic connections with carbonaceous meteorites, interstellar molecules and the origin of life

The ions, radicals, and molecules observed in comets may be derived intact or by partial decomposition from parent compounds of the sort found either in the interstellar medium or in carbonaceous meteorites. The early loss of highly reducing primitive atmosphere and its replacement by a secondary atmosphere dominated by H2O, CO2, and N2, as depicted in current models of the earth's evolution, pose a dilemma for the origin of life: the synthesis of organic compounds necessary for life from components of the secondary atmosphere appears to be difficult, and plausible mechanisms have not been evaluated. Both comets and carbonaceous meteorites are implicated as sources for the earth's atmophilic and organogenic elements. A mass balance argument involving the estimated ratios of hydrogen to carbon in carbonaceous meteorites, comets, and the crust and upper mantle suggests that comets supplied the earth with a large fraction of its volatiles. The probability that comets contributed significantly to the earth's volatile inventory suggests a chemical evolutionary link between comets, prebiotic organic synthesis, and the origin of life.

Chang, S.↗

Noble gas trapping and fractionation during synthesis of carbonaceous matter

An investigation of noble gas entrapment during synthesis of carbonaceous, macromolecular, and kerogen-like substances is presented. High molecular weight organic matter synthesized in aqueous condensation reactions contained little gas, and the composition was consistent with fractionation due to noble gas solubility in water; however, propane soot produced during a modified Miller-Urey experiment in an aritificial gas mixture contained high concentrations of trapped noble gases that displayed strong elemental fractionation from their reservoirs. It is concluded that theses experiemnts show that processes exist for synthesis of carbonaceous carriers that result in high noble gas concentrations and strong elemental fractionation at temperatures well above those required by absorption to achieve similar effects.

Frick, U.↗