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Register a new userIntermediate-size fullerenes as degradation products of interstellar PAHs
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The high interstellar abundances of polycyclic aromatic hydrocarbons (PAHs) and their size distribution are the result of complex chemical processes implying dust, UV radiation, and the main gaseous components (H, C+, and O). These processes must explain the high abundance of relatively small PAHs in the diffuse interstellar medium (ISM) and imply the continuous formation of some PAHs that are small enough (number of carbon atoms NC <~ 35-50) to be completely dehydrogenated by interstellar UV radiation. The carbon clusters Cn thus formed are constantly exposed to the absorption of ~10-13.6 eV UV photons, allowing isomerization and favoring the formation of the most stable isomers. They might tend to form irregular carbon cages. The frequent accretion of interstellar C+ ions could favor further cage isomerization, as is known in the laboratory for C60, possibly yielding most stable fullerenes, such as C40, C44, and C50. These fullerenes are expected to be very stable in the diffuse ISM because C2 ejection is not possible by single UV photon absorption, but could need rare two-photon absorption. It is possible that at least one of these fullerenes or its cation is as abundant as C60 or C60+ in the diffuse ISM, although this abundance is limited by the lack of observed matching features in observed mid-infrared spectra. B3LYP calculations of the visible spectrum for a number of fullerene isomers with 40 <~ NC <~ 50 show that they generally have a few spectral bands in the visible range, with f-values in the range of a few 10-2. This could make such fullerenes interesting candidates for the carriers of some diffuse interstellar bands.
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[Abridged] Fullerenes have been recently detected in various circumstellar and interstellar environments, raising the question of their formation pathway. It has been proposed that they can form by the photo-chemical processing of large polycyclic aromatic hydrocarbons (PAHs). Following our previous work on the evolution of PAHs in the NGC 7023 reflection nebula, we evaluate, using photochemical modeling, the possibility that the PAH C$_{66}$H$_{20}$ (i.e. circumovalene) can lead to the formation of C$_{60}$ upon irradiation by ultraviolet photons. The chemical pathway involves full dehydrogenation, folding into a floppy closed cage and shrinking of the cage by loss of C$_2$ units until it reaches the symmetric C$_{60}$ molecule. At 10 from the illuminating star and with realistic molecular parameters, the model predicts that 100% of C$_{66}$H$_{20}$ is converted into C$_{60}$ in $sim$ 10$^5$ years, a timescale comparable to the age of the nebula. Shrinking appears to be the kinetically limiting step of the whole process. Hence, PAHs larger than C$_{66}$H$_{20}$ are unlikely to contribute significantly to the formation of C$_{60}$, while PAHs containing between 60 and 66 C atoms should contribute to the formation of C$_{60}$ with shorter timescales, and PAHs containing less than 60 C atoms will be destroyed. Assuming a classical size distribution for the PAH precursors, our model predicts absolute abundances of C$_{60}$ are up to several $10^{-4}$ of the elemental carbon, i.e. less than a percent of the typical interstellar PAH abundance, which is consistent with observational studies. According to our model, once formed, C$_{60}$ can survive much longer than other fullerenes because of the remarkable stability of the C$_{60}$ molecule at high internal energies.Hence, a natural consequence is that C$_{60}$ is more abundant than other fullerenes in highly irradiated environments.
We present experimental data on H2 formation processes on gas-phase polycyclic aromatic hydrocarbon (PAH) cations. This process was studied by exposing coronene radical cations, confined in a radio-frequency ion trap, to gas phase H atoms. Sequential attachment of up to 23 hydrogen atoms has been observed. Exposure to atomic D instead of H allows one to distinguish attachment from competing abstraction reactions, as the latter now leave a unique fingerprint in the measured mass spectra. Modeling of the experimental results using realistic cross sections and barriers for attachment and abstraction yield a 1:2 ratio of abstraction to attachment cross sections. The strong contribution of abstraction indicates that H2 formation on interstellar PAH cations is an order of magnitude more relevant than previously thought.
[Abridged] We combine new CO(1-0) line observations of 24 intermediate redshift galaxies (0.03 < z < 0.28) along with literature data of galaxies at 0<z<4 to explore scaling relations between the dust and gas content using PAH 6.2 $mu$m ($L_{6.2}$), CO ($L_{rm CO}$), and infrared ($L_{rm IR}$) luminosities for a wide range of redshifts and physical environments. Our analysis confirms the existence of a universal $L_{6.2}-L_{rm CO}$ correlation followed by normal star-forming galaxies (SFGs) and starbursts (SBs) at all redshifts. This relation is also followed by local ULIRGs that appear as outliers in the $L_{6.2}-L_{rm IR}$ and $L_{rm IR}-L_{rm CO}$ relations from the sequence defined by normal SFGs. The emerging tight ($sigma approx 0.26$ dex) and linear ($alpha = 1.03$) relation between $L_{6.2}$ and $L_{rm CO}$ indicates a $L_{6.2}$ to molecular gas ($M_{rm H_2}$) conversion factor of $alpha_{6.2} = M_{rm H2}/L_{6.2} = (2.7pm1.3) times alpha_{rm CO}$, where $alpha_{rm CO}$ is the $L_{rm CO}$ to $M_{rm H_2}$ conversion factor. We also find that on galaxy integrated scales, PAH emission is better correlated with cold rather than with warm dust emission, suggesting that PAHs are associated with the diffuse cold dust, which is another proxy for $M_{rm H_2}$. Focusing on normal SFGs among our sample, we employ the dust continuum emission to derive $M_{rm H_2}$ estimates and find a constant $M_{rm H_2}/L_{6.2}$ ratio of $alpha_{6.2} = 12.3 M_{rm H_2}/{rm L}_{odot}$ ($sigmaapprox 0.3$ dex). We propose that the presented $L_{6.2}-L_{rm CO}$ and $L_{6.2}-M_{rm H_2}$ relations will serve as useful tools for the determination of the physical properties of high-$z$ SFGs, for which PAH emission will be routinely detected by the James Webb Space Telescope.
We present observations which probe the small-scale structure of the interstellar medium using diffuse interstellar bands (DIBs). Towards HD 168075/6 in the Eagle Nebula, significant differences in DIB absorption are found between the two lines of sight, which are separated by 0.25 pc, and {lambda}5797 exhibits a velocity shift. Similar data are presented for four stars in the {mu} Sgr system. We also present a search for variations in DIB absorption towards {kappa} Vel, where the atomic lines are known to vary on scales of ~10 AU. Observations separated by ~9 yr yielded no evidence for changes in DIB absorption strength over this scale, but do reveal an unusual DIB spectrum.
In 1985, During experiments aimed at understanding the mechanisms by which long-chain carbon molecules are formed in interstellar space and circumstellar shells, Harry Kroto and his collaborators serendipitously discovered a new form of carbon: fullerenes. The most emblematic fullerene (i.e. C$_{60}$ buckminsterfullerene), contains exactly 60 carbon atoms organized in a cage-like structure similar to a soccer ball. Since their discovery impacted the field of nanotechnologies, Kroto and colleagues received the Nobel prize in 1996. The cage-like structure, common to all fullerene molecules, gives them unique properties, in particular an extraordinary stability. For this reason and since they were discovered in experiments aimed to reproduce conditions in space, fullerenes were sought after by astronomers for over two decades, and it is only recently that they have been firmly identified by spectroscopy, in evolved stars and in the interstellar medium. This identification offers the opportunity to study the molecular physics of fullerenes in the unique physical conditions provided by space, and to make the link with other large carbonaceous molecules thought to be present in space : polycyclic aromatic hydrocarbons.
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