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At least 199 records · Page 11Linked to original sources
PubMed2001

Closed-shell polycyclic aromatic hydrocarbon cations: a new category of interstellar polycyclic aromatic hydrocarbons.

Density functional theory has been employed to calculate the harmonic frequencies and intensities of a range of polycyclic aromatic hydrocarbon (PAH) cations that explore both size and electronic structure effects on the infrared spectroscopic properties of these species. The sample extends the size range of PAH species considered to more than 50 carbon atoms and includes several representatives from each of two heretofore unexplored categories of PAH cations: (1) fully benzenoid PAH cations whose carbon skeleton is composed of an odd number of carbon atoms (C(odd) PAHs); and (2) protonated PAH cations (HPAH+). Unlike the radical electronic structures of the PAH cations that have been the subject of previous theoretical and experimental work, the species in these two classes have a 'closed'-shell electronic configuration. The calculated spectra of circumcoronene, C54H18, in both neutral and (radical) cationic form are also reported and compared with those of the other species. Overall, the C(odd) PAHs spectra are dominated by strong CC stretching modes near 1600 cm(-1) and display spectra that are remarkably insensitive to molecular size. The HPAH+ species evince a more complex spectrum consistent with the added contributions of aliphatic modes and their generally lower symmetry. Finally, for both classes of closed-shell cations, the intensity of the aromatic CH stretching modes is found to increase with molecular size far out of proportion with the number of CH groups, approaching a value more typical of neutral PAHs for the largest species studied.

Carbon Isotopes↗
PubMed2001

Electronic spectra and ionization potentials of a stable class of closed shell polycyclic aromatic hydrocarbon cations.

Due to their stability, closed shell polycyclic aromatic hydrocarbon (PAH) cations are possible candidates as carriers for some of the diffuse interstellar bands (DIBs). The electronic absorption spectra and ionization potentials of several closed shell PAH cations are determined in this study. We use density functional theory (DFT) at the BLYP/6-31G* level to determine the ionization potentials and thus confirm the stability of the PAH cations of interest. We use time-dependent density functional theory (TDDFT), again at the BLYP/6-31G* level, to calculate the vertical excitation energies and oscillator strengths of the PAH cations. We observe dominant single absorptions within the DIB spectral region of interest in all of the PAH cation spectra except for the smallest member of the series.

Astronomical Phenomena↗
PubMed1999

Variations in the strength of the infrared forbidden 2328.2 cm-1 fundamental of solid N2 in binary mixtures.

We present the 2335-2325 cm-1 infrared spectra and band positions, profiles and strengths (A values) of solid nitrogen and binary mixtures of N2 with other molecules at 12 K. The data demonstrate that the strength of the infrared forbidden N2 fundamental near 2328 cm-1 is moderately enhanced in the presence of NH3, strongly enhanced in the presence of H2O and very strongly enhanced (by over a factor of 1000) in the presence of CO2, but is not significantly affected by CO, CH4, or O2. The mechanisms for the enhancements in N2-NH3 and N2-H2O mixtures are fundamentally different from those proposed for N2-CO2 mixtures. In the first case, interactions involving hydrogen-bonding are likely the cause. In the latter, a resonant exchange between the N2 stretching fundamental and the 18O = 12C asymmetric stretch of 18O12C16O is indicated. The implications of these results for several astrophysical issues are briefly discussed.

Ammonia↗
PubMed1998

Single photon infrared emission spectroscopy: a study of IR emission from UV laser excited PAHs between 3 and 15 micrometers.

Single-photon infrared emission spectroscopy (SPIRES) has been used to measure emission spectra from polycyclic aromatic hydrocarbons (PAHs). A supersonic free-jet expansion has been used to provide emission spectra of rotationally cold and vibrationally excited naphthalene and benzene. Under these conditions, the observed width of the 3.3-micrometers (C-H stretch) band resembles the bandwidths observed in experiments in which emission is observed from naphthalene with higher rotational energy. To obtain complete coverage of IR wavelengths relevant to the unidentified infrared bands (UIRs), UV laser-induced desorption was used to generate gas-phase highly excited PAHs. Lorentzian band shapes were convoluted with the monochromator-slit function in order to determine the widths of PAH emission bands under astrophysically relevant conditions. Bandwidths were also extracted from bands consisting of multiple normal modes blended together. These parameters are grouped according to the functional groups mostly involved in the vibration, and mean bandwidths are obtained. These bandwidths are larger than the widths of the corresponding UIR bands. However, when the comparison is limited to the largest PAHs studied, the bandwidths are slightly smaller than the corresponding UIR bands. These parameters can be used to model emission spectra from PAH cations and cations of larger PAHs, which are better candidate carriers of the UIRs.

Argon↗
PubMed1998

Infrared spectra of substituted polycylic aromatic hydrocarbons.

Calculations are carried out using density functional theory (DFT) to determine the harmonic frequencies and intensities of 1-methylanthracene, 9-methylanthracene, 9-cyanoanthracene, 2-aminoanthracene, acridine, and their positive ions. The theoretical data are compared with matrix-isolation spectra for these species also reported in this work. The theoretical and experimental frequencies and relative intensities for the neutral species are in generally good agreement, whereas the positive ion spectra are only in qualitative agreement. Relative to anthracene, we find that substitution of a methyl or CN for a hydrogen does not significantly affect the spectrum other than to add the characteristic methyl C-H and C triple bond N stretches near 2900 and 2200 cm-1, respectively. However, addition of NH2 dramatically affects the spectrum of the neutral. Not only are the NH2 modes themselves strong, but this electron-withdrawing group induces sufficient partial charge on the ring to give the neutral molecule spectra characteristics of the anthracene cation. The sum of the absolute intensities is about four times larger for 2-aminoanthracene than those for 9-cyanoanthracene. Substituting nitrogen in the ring at the nine position (acridine) does not greatly alter the spectrum compared with anthracene.

Acridines↗
PubMed1998

From Panspermia to Bioastronomy, the evolution of the hypothesis of universal life.

During the 19th and early 20th centuries, ideas related to the possible origin in space of bioorganic molecules, or seeds, or even germs and organisms (and how they reached the Earth) included the Panspermia theory. Based on the idea of the eternity of life proposed by eminent physicists - such as Arrhenius and Kelvin - 'Panspermia' is mainly divided into two branches: lithopanspermia (transport of germs inside stones traveling in space) and radiopanspermia (transport of spores by radiative pressure of stellar light). We point out some arguments to help to understand whether 'Panspermia' could exist nowadays as the same theory defined one century ago. And we wonder about the kind of evolution 'Panspermia' could have undergone during only a few decades. This possible evolution of the 'Panspermia' concept takes place in the framework of the emergence of a new field, Bioastronomy. We present how this discipline has emerged during a few decades and how it has evolved. We consider its relationship with the progression of other scientific fields, and finally we examine how it is now included in different projects of space agencies. Bioastronomy researches having become more and more robust during the last few years, we emphasize several questions about new ideas and their consequences for the current hypothesis of 'Panspermia' and of universal life.

Astronomy↗
PubMed2002

The Perseus Exobiology mission on MIR: behaviour of amino acids and peptides in Earth orbit.

Leucine, alpha-methyl leucine and two peptides were exposed to space conditions on board the MIR station during the Perseus-Exobiology mission. This long duration space mission was aimed at testing the delivery of prebiotic building blocks. During this mission, two amino acids (leucine and alpha-methyl leucine) and two peptides (leucine-diketopiperazine and trileucine thioethylester) were exposed in Earth orbit for three months. Basalt, clay and meteorite powder were also mixed with the samples in order to simulate the effects of potential meteorite protection. Analysis of the material after the flight did not reveal any racemization or polymerisation but did provide information regarding photochemical pathways for the degradation of leucine and of the tripeptide. Amino acids appeared to be more sensitive to UV radiation than peptides, the cyclic dipeptide being found to be as particularly resistant. Meteorite powder which exhibits the highest absorption in Vacuum UltraViolet (VUV) afforded the best protection to the organic molecules whereas montmorillonite clay, almost transparent in VUV, was the least efficient. By varying the thickness of the meteorite, we found that the threshold for efficient protection against radiation was about 5 microm. The possible exogenous origin of biological building blocks is discussed with respect to the stability to the molecules and the nature of the associated minerals.

Bentonite↗
PubMed1984

A new interstellar molecule: tricarbon monoxide.

The cold dark interstellar Taurus Molecular Cloud One (TMC-1) is a rich source of acetylenic and polyacetylenic molecular species. As well as linear closed-shell molecules (H(C triple bond C)nCN) and symmetric rotors (CH3C triple bond CH, CH3C triple bond CCN), several radicals (C triple bond CH, C triple bond CCN, (C triple bond C2H) have also been identified, many of which had not been studied previously in the laboratory. Whether the observed abundances can be understood in terms of purely gas-phase ion-molecule chemical schemes, which produce reasonable agreement for the simplest polyatomic species, is unclear; alternative models involving the particulate interstellar grains as catalysts or sources have also been suggested. We now report the detection in TMC-1 of a new molecule, tricarbon monoxide (C3O), whose pure rotational spectrum has only very recently been studied in the laboratory. As C3O is the first known interstellar carbon chain molecule to contain oxygen, its existence places an important new constraint on chemical schemes for cold interstellar clouds. In fact, the observed abundance of tricarbon monoxide fits quite well into our model of galactochemistry.

Astronomical Phenomena↗
PubMed2001

Substantial reservoirs of molecular hydrogen in the debris disks around young stars.

Circumstellar accretion disks transfer matter from molecular clouds to young stars and to the sites of planet formation. The disks observed around pre-main-sequence stars have properties consistent with those expected for the pre-solar nebula from which our own Solar System formed 4.5 Gyr ago. But the 'debris' disks that encircle more than 15% of nearby main-sequence stars appear to have very small amounts of gas, based on observations of the tracer molecule carbon monoxide: these observations have yielded gas/dust ratios much less than 0.1, whereas the interstellar value is about 100 (ref. 9). Here we report observations of the lowest rotational transitions of molecular hydrogen (H2) that reveal large quantities of gas in the debris disks around the stars beta Pictoris, 49 Ceti and HD135344. The gas masses calculated from the data are several hundreds to a thousand times greater than those estimated from the CO observations, and yield gas/dust ratios of the same order as the interstellar value.

Astronomy↗
PubMed1994

Fullerenes in an impact crater on the LDEF spacecraft.

The fullerenes C60 and C70 have been found to occur naturally on Earth and have also been invoked to explain features in the absorption spectra of interstellar clouds. But no definitive spectroscopic evidence exists for fullerenes in space and attempts to find fullerenes in carbonaceous chondrites have been unsuccessful. Here we report the observation of fullerenes associated with carbonaceous impact residue in a crater on the Long Duration Exposure Facility (LDEF) spacecraft. Laser ionization mass spectrometry and Raman spectroscopy indicate the presence of fullerenes in the crater and in adjacent ejecta. Man-made fullerenes survive experimental hypervelocity (approximately 6.1 km s-1) impacts into aluminium targets, suggesting that space fullerenes contained in a carbonaceous micrometeorite could have survived the LDEF impact at velocities towards the lower end of the natural particle encounter range (<13 km s-1). We also demonstrate that the fullerenes were unlikely to have formed as instrumental artefacts, nor are they present as contaminants. Although we cannot specify the origin of the fullerenes with certainty, the most plausible source is the chondritic impactor. If, alternatively, the impact produced the fullerenes in situ on LDEF, then this suggests a viable mechanism for fullerene production in space.

Aluminum↗
PubMed1996

Detection of acetylene in the infrared spectrum of comet Hyakutake.

Comets are rich in volatile materials, of which roughly 80% (by number) are water molecules. Considerable progress is being made in identifying the other volatile species, the abundances of which should enable us to determine whether comets formed primarily from ice-covered interstellar grains, or from material that was chemically processed in the early solar nebula. Here we report the detection of acetylene (C2H2) in the infrared spectrum of comet C/1996 B2 (Hyakutake). The estimated abundance is 0.3-0.9%, relative to water, which is comparable to the predicted solid-phase abundance in cold interstellar clouds. This suggests that the volatiles in comet Hyakotake may have come from ice-covered interstellar grains, rather than material processed in the accretion disk out of which the Solar System formed.

Acetylene↗
PubMed1998

H3+ in dense and diffuse clouds.

Interstellar H3+ has been detected in dense as well as diffuse clouds using three 3.7 microns infrared spectral lines of the nu 2 fundamental band. Column densities of H3+ from (1.7-5.5) x 10(14) cm-2 have been measured in dense clouds in absorption against the infrared continua of the deeply embedded young stellar objects GL2136, W33A, MonR2 IRS 3, GL961E, and GL2591. Strong and broad H3+ absorptions have been detected in dense and diffuse clouds towards GC IRS 3 and GCS3-2 in the region of the galactic center. A large column density of H3+, comparable to that of a dense cloud, has been detected towards the visible star Cygnus OB2 No. 12, which has a line of sight that crosses mostly diffuse clouds. The H3+ chemistry of dense and diffuse clouds are discussed using a very simple model. Some future projects and problems are discussed.

Astronomical Phenomena↗
PubMed2006

Interstellar H(3)(+).

Protonated molecular hydrogen, H(3)(+), is the simplest polyatomic molecule. It is the most abundantly produced interstellar molecule, next only to H(2), although its steady state concentration is low because of its extremely high chemical reactivity. H(3)(+) is a strong acid (proton donor) and initiates chains of ion-molecule reactions in interstellar space thus leading to formation of complex molecules. Here, I summarize the understandings on this fundamental species in interstellar space obtained from our infrared observations since its discovery in 1996 and discuss the recent observations and analyses of H(3)(+) in the Central Molecular Zone near the Galatic center that led to a revelation of a vast amount of warm and diffuse gas existing in the region.

Astronomy↗
PubMed2006

The chemistry in circumstellar envelopes of evolved stars: following the origin of the elements to the origin of life.

Mass loss from evolved stars results in the formation of unusual chemical laboratories: circumstellar envelopes. Such envelopes are found around carbon- and oxygen-rich asymptotic giant branch stars and red supergiants. As the gaseous material of the envelope flows from the star, the resulting temperature and density gradients create a complex chemical environment involving hot, thermodynamically controlled synthesis, molecule "freeze-out," shock-initiated reactions, and photochemistry governed by radical mechanisms. In the circumstellar envelope of the carbon-rich star IRC+10216, >50 different chemical compounds have been identified, including such exotic species as C(8)H, C(3)S, SiC(3), and AlNC. The chemistry here is dominated by molecules containing long carbon chains, silicon, and metals such as magnesium, sodium, and aluminum, which makes it quite distinct from that found in molecular clouds. The molecular composition of the oxygen-rich counterparts is not nearly as well explored, although recent studies of VY Canis Majoris have resulted in the identification of HCO(+), SO(2), and even NaCl in this object, suggesting chemical complexity here as well. As these envelopes evolve into planetary nebulae with a hot, exposed central star, synthesis of molecular ions becomes important, as indicated by studies of NGC 7027. Numerous species such as HCO(+), HCN, and CCH are found in old planetary nebulae such as the Helix. This "survivor" molecular material may be linked to the variety of compounds found recently in diffuse clouds. Organic molecules in dense interstellar clouds may ultimately be traced back to carbon-rich fragments originally formed in circumstellar shells.

Astronomical Phenomena↗
PubMed2006

Interstellar chemistry.

In the past half century, radioastronomy has changed our perception and understanding of the universe. In this issue of PNAS, the molecular chemistry directly observed within the galaxy is discussed. For the most part, the description of the molecular transformations requires specific kinetic schemes rather than chemical thermodynamics. Ionization of the very abundant molecular hydrogen and atomic helium followed by their secondary reactions is discussed. The rich variety of organic species observed is a challenge for complete understanding. The role and nature of reactions involving grain surfaces as well as new spectroscopic observations of interstellar and circumstellar regions are topics presented in this special feature.

Astronomy↗