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PubMed1997

Collisions with ice/volatile objects: geological implications--a qualitative treatment.

An aperiodic collision of the Earth with extra-terrestria] ice/volatile bodies is proposed as a mechanism to produce rapid changes in the geologic record. Due to the volatile nature of these bodies, evidence for their impacts, particularly in the ocean might be subtle and best seen as 'spikes' in the geochemical or fossil record against normal background. Differing effects would result depending on the site of the major break-up of the object: in the atmosphere, on land, or in the ocean. This paper focuses on the effects of adding material to the seas, oceans, and atmosphere. The treatment is largely qualitative, however mass balance calculations were used to estimate the relative mass needed to affect changes in a variety of reservoirs. Although actual impactors probably have a variable composition, the effects of water-, C-, N-, and S-containing objects are discussed. In the atmosphere, effects could include increased rain acidity, increased levels of nutrients, and enhanced greenhouse warming/cooling. Oceanic effects might include increased oceanic productivity (nitrogen-containing objects). As a result of increased chemical weathering and/or greenhouse effects, increased temperatures coupled with enhanced productivity could result in wider-spread oceanic anoxia or altered calcite/aragonite stability. Possible examples of such impacts from the geologic record and potential biotic effects are given.

Acid Rain↗
PubMed1997

Quenched Carbonaceous Composite: a laboratory analog for carbonaceous material in the interstellar medium.

We review the properties of Quenched Carbonaceous Composite (QCC), a residue produced from a hydrocarbon plasma, and the properties of its derivatives. A. Sakata and his colleagues have shown that QCC has a 220 nm absorption band, visible fluorescence matching the extended red emission seen in reflection nebulae, and infrared absorption bands that correspond to the infrared emission features in reflection nebulae, HII regions, and planetary nebulae. These properties make QCC a strong candidate material as a laboratory analog to the carbonaceous material in the interstellar medium. QCC is distinguished from the PAH hypothesis in that (1) it is a condensate composed of aromatic and aliphatic molecules, as well as radicals; (2) it exhibits a 220 nm absorption that is very similar in wavelength to the 217 nm absorption in the interstellar medium; (3) it exhibits visible fluorescence consistent with that seen in reflection nebulae; and (4) the bands at 7.7 and 8.6 microns are caused by ketone bands in oxidized QCC. The aromatic component in QCC is thought to be typically 1-4 rings, with the majority being about 1-2 rings.

Carbon↗
PubMed1999

Transport of extraterrestrial biomolecules to the Earth: problem of thermal stability.

The idea of extraterrestrial delivery of organic matter to the early Earth is especially attractive at present and is strongly supported by the detection of a large variety of organic compounds, including amino acids and nucleobases, in carbonaceous chondrites. Whether these compounds can be delivered by other space bodies is unclear and depends primarily on capability of the biomolecules to survive high temperatures during atmospheric deceleration and impacts to the terrestrial surface. In the present study we estimated survivability of simple amino acids (alpha-aminoisobutyric acid, L-alanine, L-valine and L-leucine), purines (adenine and guanine) and pyrimidines (uracil and cytosine) under rapid heating to temperatures of 400 to 1000 degrees C under N2 or CO2 atmosphere. We have found that most of the compounds studied cannot survive the temperatures substantially higher than 700 degrees C; however at 500-600 degrees C, the recovery can be at a per cent level (or even 10%-level for adenine, uracil, alanine, and valine). Implications of the data for extraterrestrial delivery of the biomolecules are discussed.

Adenine↗
PubMed1995

Comets and life in the Universe.

The notion that comets supplied the primitive Earth with the requisite chemical species for the process of chemical evolution, which is widely held to have led to the origin of life on Earth, has now gained considerable intellectual momentum since its first formulation in 1961. In fact, in the fall of 1991, the University of Wisconsin-Eau Claire hosted a well attended scientific meeting devoted solely to the discussion of this topic, entitled Comets and the Origin and Evolution of Life [see Special Issue of Origins of Life, P.J. Thomas (ed), vol. 21(5-6)]. As a result of the above meeting, the recently completed COSPAR/World Space Congress Symposium on Extraterrestrial Organic Chemistry and the Origins of Life, and numerous independent reports, the role of comets in the Earth's biogenesis has been thoroughly addressed in the literature. At this time, in light of a few recent findings, we present here a concise review of this topic together with a brief discussion of the possible role of cometary material in the origin of life elsewhere in the Universe.

Carbon↗
PubMed1995

Exobiology research on Space Station Freedom.

The Gas-Grain Simulation Facility (GGSF) is a multidisciplinary experiment laboratory being developed by NASA at Ames Research Center for delivery to Space Station Freedom in 1998. This facility will employ the low-gravity environment of the Space Station to enable aerosol experiments of much longer duration than is possible in any ground-based laboratory. Studies of fractal aggregates that are impossible to sustain on Earth will also be enabled. Three research areas within exobiology that will benefit from the GGSF are described here. An analysis of the needs of this research and of other suggested experiments has produced a list of science requirements which the facility design must accommodate. A GGSF design concept developed in the first stage of flight hardware development to meet these requirements is also described.

Cosmic Dust↗
PubMed2001

The unidentified diffuse interstellar bands as evidence for large organic molecules in the interstellar medium.

Since 1921, astronomers have been aware of a set of spectral absorption features that are formed in interstellar space but are not identifiable with any known atomic or molecular species. Today some 200 of these so-called diffuse interstellar bands (DIBs) are known, yet none has yet been identified unambiguously with any specific carrier. Recent evidence from astronomical observations, laboratory spectroscopy, and chemical studies suggests that the responsible species are large carbon-bearing molecules. This paper provides a brief history of the DIB problem, a review of suggested carriers, and a description and discussion of new results from the telescope and from laboratory measurements of chemical reaction rates in candidate carriers.

Absorption↗
PubMed2001

Searches for new interstellar molecules, including a tentative detection of aziridine and a possible detection of propenal.

Rotational spectroscopy at millimeter wavelengths is a powerful means of investigating the chemistry of dense interstellar clouds. These regions can exhibit an interesting complement of gas phase molecules, including relatively complex organics. Here we report the tentative first astronomical detection of aziridine (ethylenimine), the possible detection of propenal (acrolein), and upper limits on the abundances of cyclopropenone, furan, hydroxyethanal (glycolaldehyde), thiohydroxylamine (NH2SH), and ethenol (vinyl alcohol) in various interstellar clouds.

Acetaldehyde↗
PubMed2001

Spectroscopy of H3+ and its impact on astrophysics.

Since the original laboratory detection of an H3+ spectrum 20 years ago, the search has been on for astronomical observations of this important and fundamental molecular ion. Successful detection of H3+ in gas-giant planets, supernova ejecta and the interstellar medium as well as the prospects for future observations are discussed. The role H3+ has in determining the atmospheric structure of both the gas giants and cool metal-free planets is explored.

Astronomical Phenomena↗
PubMed2001

Interstellar matrices: the chemical composition and evolution of interstellar ices as observed by ISO.

Matrix isolation techniques have been developed in the early sixties as a tool for studying the spectroscopic properties of out of equilibrium species (atoms, radicals, ions, reactive molecules), embedded in rare gas inert matrices at low temperatures. Cold interstellar grains surfaces are able to condense out gas phase molecules, routinely observed by radioastronomy. These grain 'mantles' can be considered as 'interstellar matrices'. However, these matrices are not clean and unreactive. They are made principally of dirty ices whose composition must be determined carefully to assess the importance of the solid state chemistry that takes place in the Interstellar Medium. Infrared spectroscopy, both in astronomy and in the laboratory, is the unique tool to determine the chemical composition of these ices. Astronomical spectra can directly be compared with laboratory ones obtained using classical matrix isolation techniques. Furthermore, dedicated experiments may be undertaken to further improve the understanding of the basic physico-chemical processes that take place in cosmic ices.

Astronomical Phenomena↗
PubMed2001

Laboratory spectra of cold gas phase polycyclic aromatic hydrocarbon cations, and their possible relation to the diffuse interstellar bands.

A novel laboratory technique is described, combining the use of supersonic expansion, laser excitation and small aromatic-rare gas van der Waals (vdW) clusters properties, which was developed to access the electronic absorption spectra of the polycyclic aromatic hydrocarbon (PAH) cations in the visible. It consists in preparing vdW complexes of the PAH molecule with a rare gas in a molecular beam, to photoionize it by resonant selective two-photon ionization, then to photodissociate this ionic complex by means of a delayed laser pulse in a time-of-flight mass spectrometer. The method is illustrated by presenting the visible spectra of the Naphthalene, Phenanthrene, Fluorene and Phenylacetylene cations. Such spectra can be unambiguously compared to the astronomical spectra of reddened stars, which exhibit the so-called diffuse interstellar bands (DIBs) in absorption. An interesting feature of the technique is its ability to measure the absolute absorption cross-sections. The large values of the oscillator strengths of the transitions, which are derived, are discussed in the astrophysical context which consists in considering that the PAH cations could be carriers for some of the DIBs.

Acetylene↗
PubMed2001

Carbon chains and rings in the laboratory and in space.

Seventy-seven reactive organic molecules of astrophysical interest have been identified in a supersonic molecular beam, 73 in the radio band by Fourier-transform microwave spectroscopy, four in the optical by laser cavity ringdown spectroscopy. Most are linear carbon chains, but six consist of carbon chains attached to the compact, highly polar C3 ring, and two are rhomboidal cyclic configurations of SiC3. The laboratory astrophysics of the radio molecules is complete for the time being, in the sense that essentially all the rotational transitions of current interest to radio astronomy (including hyperfine structure when present) can now be calculated to a small fraction of 1 km s(-1) in equivalent radial velocity; six of the radio molecules have already been detected in space on the basis of the present data. The FTM spectrometer employed in this work is far from fundamental limits of sensitivity, so many more molecules can probably be found by refinements of present techniques. The density of reactive molecules in our supersonic beam is generally high by the standards of laser spectroscopy, and many of the radio molecules probably have detectable optical transitions which we are attempting to find, largely motivated by the long-standing problem of the diffuse interstellar bands. Our most interesting result to date is the detection of a fairly strong molecular band at 443 nm in a benzene discharge, in exact coincidence with the strongest and best known interstellar band. Isotopic shifts measured with partially and totally deuterated benzene suggest that the carrier of the laboratory band is a hydrocarbon molecule with the elemental formula CnH5, with n most likely in the range 3-6.

Astronomical Phenomena↗
PubMed2001

Vibrational spectroscopy of ion-irradiated ices.

In the last 20 years we have studied some effects induced by fast ions (E approximately keV-MeV) impinging on solid materials (mainly ices) with a view to their astrophysical relevance. The main techniques used have been infrared and Raman spectroscopy. Here we review some of the results obtained so far concerning, in particular, the formation of new species not present in the original sample. When hydrocarbons are an important constituent of the target ion irradiation gives rise also to a refractory residue which is left over after warming up. In addition we present some preliminary results of a new study, still in progress, on the infrared properties of the organic residue formed after irradiation of an icy mixture with H-, C-, N- and O-bearing species. Furthermore we present the micro-Raman spectra of some fragments of Orgueil a carbonaceous chondrite meteorite. Some astrophysical applications of these laboratory results are also discussed.

Astronomical Phenomena↗
PubMed2001

Mid- and far-infrared spectroscopic studies of the influence of temperature, ultraviolet photolysis and ion irradiation on cosmic-type ices.

Infrared (IR) studies of laboratory ices can provide information on the evolution of cosmic-type ices as a function of different simulated space environments involving thermal, ultraviolet (UV), or ion processing. Laboratory radiation experiments can lead to the formation of complex organic molecules. However, because of our lack of knowledge about UV photon and ion fluxes, and exposure lifetimes, it is not certain how well our simulations represent space conditions. Appropriate laboratory experiments are also limited by the absence of knowledge about the composition, density, and temperature of ices in different regions of space. Our current understanding of expected doses due to UV photons and cosmic rays is summarized here, along with an inventory of condensed-phase molecules identified on outer solar system surfaces, comets and interstellar grains. Far-IR spectra of thermally cycled H2O are discussed since these results reflect the dramatic difference between the amorphous and crystalline phases of H2O ice, the most dominant condensed-phase molecule in cosmic ices. A comparison of mid-IR spectra of products in proton-irradiated and UV-photolyzed ices shows that few differences are observed for these two forms of processing for the simple binary mixtures studied to date. IR identification of radiation products and experiments to determine production rates of new molecules in ices during processing are discussed. A new technique for measuring intrinsic IR band strengths of several unstable molecules is presented. An example of our laboratory results applied to Europa observations is included.

Carbonic Acid↗
PubMed2001

A fully ab initio potential curve of near-spectroscopic quality for OH- ion: importance of connected quadruple excitations and scalar relativistic effects.

A benchmark study has been carried out on the ground-state potential curve of the hydroxyl anion, OH-, including detailed calibration of both the l-particle and n-particle basis sets. The CCSD(T) basis set limit overestimates omega(e) by about 10 cm(-1), which is only remedied by inclusion of connected quadruple excitations in the coupled cluster expansion--or, equivalently, the inclusion of the 2pi orbitals in the active space of a multireference calculation. Upon inclusion of scalar relativistic effects (-3 cm(-1) on omega(e)), a potential curve of spectroscopic quality (sub-cm(-1) accuracy) is obtained. Our best computed EA(OH), 1.828 eV, agrees to three decimal places with the best available experimental value. Our best computed dissociation energies, D0(OH-) = 4.7796 eV and D0(OH) = 4.4124 eV, suggest that the experimental D0(OH) = 4.392 eV may possibly be about 0.02 eV too low.

Astronomical Phenomena↗
PubMed2001

Ab initio calculations of electronically excited states of cyano-substituted polyacetylene cations.

The transition energies for the lowest energy pi --> pi* electronic excitations are calculated with the complete active space self-consistent field method (CASSCF) and with the complete active space second-order perturbation theory method (CASPT2) for the linear cyano-substituted polyacetylene cations, H-Cn-CN+, n = 4-11, and NC-Cn-CN+, n = 2-10. These systems are models for an important class of interstellar species. We demonstrate the utility of the theoretical calculations in assigning the experimental spectra.

Acetylene↗