134 research outputs found
Stacked clusters of polycyclic aromatic hydrocarbon molecules
Clusters of polycyclic aromatic hydrocarbon (PAH) molecules are modelled
using explicit all-atom potentials using a rigid body approximation. The PAH's
considered range from pyrene (C10H8) to circumcoronene (C54H18), and clusters
containing between 2 and 32 molecules are investigated. In addition to the
usual repulsion-dispersion interactions, electrostatic point-charge
interactions are incorporated, as obtained from density functional theory
calculations. The general electrostatic distribution in neutral or singly
charged PAH's is reproduced well using a fluctuating charges analysis, which
provides an adequate description of the multipolar distribution. Global
optimization is performed using a variety of methods, including basin-hopping
and parallel tempering Monte Carlo. We find evidence that stacking the PAH
molecules generally yields the most stable motif. A structural transition
between one-dimensional stacks and three-dimensional shapes built from mutiple
stacks is observed at larger sizes, and the threshold for this transition
increases with the size of the monomer. Larger aggregates seem to evolve toward
the packing observed for benzene in bulk.Difficulties met in optimizing these
clusters are analysed in terms of the strong anisotropy of the molecules. We
also discuss segregation in heterogeneous clusters and vibrational properties
in the context of astrophysical observations.Comment: 12 pages, 7 figure
Extended Red Emission and the evolution of carbonaceaous nanograins in NGC 7023
Extended Red Emission (ERE) was recently attributed to the photo-luminescence
of either doubly ionized Polycyclic Aromatic Hydrocarbons (PAH), or
charged PAH dimers. We analysed the visible and mid-infrared (mid-IR) dust
emission in the North-West and South photo-dissociation regions of the
reflection nebula NGC 7023.Using a blind signal separation method, we extracted
the map of ERE from images obtained with the Hubble Space Telescope, and at the
Canada France Hawaii Telescope. We compared the extracted ERE image to the
distribution maps of the mid-IR emission of Very Small Grains (VSGs), neutral
and ionized PAHs (PAH and PAH) obtained with the Spitzer Space
Telescope and the Infrared Space Observatory. ERE is dominant in transition
regions where VSGs are being photo-evaporated to form free PAH molecules, and
is not observed in regions dominated by PAH. Its carrier makes a minor
contribution to the mid-IR emission spectrum. These results suggest that the
ERE carrier is a transition species formed during the destruction of VSGs.
Singly ionized PAH dimers appear as good candidates but PAH molecules
seem to be excluded.Comment: Accepted for publication in A&
Mapping the structural diversity of C60 carbon clusters and their infrared spectra
The current debate about the nature of the carbonaceous material carrying the
infrared (IR) emission spectra of planetary and proto-planetary nebulae,
including the broad plateaus, calls for further studies on the interplay
between structure and spectroscopy of carbon-based compounds of astrophysical
interest. The recent observation of C60 buckminsterfullerene in space suggests
that carbon clusters of similar size may also be relevant. In the present work,
broad statistical samples of C60 isomers were computationally determined
without any bias using a reactive force field, their IR spectra being
subsequently obtained following local optimization with the
density-functional-based tight-binding theory. Structural analysis reveals four
main structural families identified as cages, planar polycyclic aromatics,
pretzels, and branched. Comparison with available astronomical spectra
indicates that only the cage family could contribute to the plateau observed in
the 6-9 micron region. The present framework shows great promise to explore and
relate structural and spectroscopic features in more diverse and possibly
hydrogenated carbonaceous compounds, in relation with astronomical
observations
Size effect in the ionization energy of PAH clusters
We report the first experimental measurement of the near-threshold
photo-ionization spectra of polycyclic aromatic hydrocarbon clusters made of
pyrene C16H10 and coronene C24H12, obtained using imaging photoelectron
photoion coincidence spectrometry with a VUV synchrotron beamline. The
experimental results of the ionization energy are confronted to calculated ones
obtained from simulations using dedicated electronic structure treatment for
large ionized molecular clusters. Experiment and theory consistently find a
decrease of the ionization energy with cluster size. The inclusion of
temperature effects in the simulations leads to a lowering of this energy and
to a quantitative agreement with the experiment. In the case of pyrene, both
theory and experiment show a discontinuity in the IE trend for the hexamer
Formation and destruction of polycyclic aromatic hydrocarbon clusters in the interstellar medium
The competition between the formation and destruction of coronene clusters
under interstellar conditions is investigated theoretically. The unimolecular
nucleation of neutral clusters is simulated with an atomic model combining an
explicit classical force field and a quantum tight-binding approach.
Evaporation rates are calculated in the framework of the phase space theory and
are inserted in an infrared emission model and compared with the growth rate
constants. It is found that, in interstellar conditions, most collisions lead
to cluster growth. The time evolution of small clusters (containing up to 312
carbon atoms) was specifically investigated under the physical conditions of
the northern photodissociation region of NGC 7023. These clusters are found to
be thermally photoevaporated much faster than they are reformed, thus providing
an interpretation for the lowest limit of the interstellar cluster size
distribution inferred from observations. The effects of ionizing the clusters
and density heterogeneities are also considered. Based on our results, the
possibility that PAH clusters could be formed in PDRs is critically discussed.Comment: 14 pages, 14 figures. Astronomy & Astrophysics, accepted for
publicatio
Gas morphology and energetics at the surface of PDRs: new insights with Herschel observations of NGC 7023
We investigate the physics and chemistry of the gas and dust in dense
photon-dominated regions (PDRs), along with their dependence on the
illuminating UV field. Using Herschel-HIFI observations, we study the gas
energetics in NGC 7023 in relation to the morphology of this nebula. NGC 7023
is the prototype of a PDR illuminated by a B2V star and is one of the key
targets of Herschel. Our approach consists in determining the energetics of the
region by combining the information carried by the mid-IR spectrum (extinction
by classical grains, emission from very small dust particles) with that of the
main gas coolant lines. In this letter, we discuss more specifically the
intensity and line profile of the 158 micron (1901 GHz) [CII] line measured by
HIFI and provide information on the emitting gas. We show that both the [CII]
emission and the mid-IR emission from polycyclic aromatic hydrocarbons (PAHs)
arise from the regions located in the transition zone between atomic and
molecular gas. Using the Meudon PDR code and a simple transfer model, we find
good agreement between the calculated and observed [CII] intensities. HIFI
observations of NGC 7023 provide the opportunity to constrain the energetics at
the surface of PDRs. Future work will include analysis of the main coolant line
[OI] and use of a new PDR model that includes PAH-related species.Comment: Accepted for publication in Astronomy and Astrophysics Letters
(Herschel HIFI special issue), 5 pages, 5 figure
Polycyclic aromatic hydrocarbon processing in interstellar shocks
Context: PAHs appear to be an ubiquitous interstellar dust component but the
effects of shocks waves upon them have never been fully investigated. Aims: To
study the effects of energetic (~0.01-1 keV) ion (H, He and C) and electron
collisions on PAHs in interstellar shock waves.Methods: We calculate the
ion-PAH and electron-PAH nuclear and electronic interactions, above the
threshold for carbon atom loss from a PAH, in 50-200 km/s shock waves in the
warm intercloud medium. Results: Interstellar PAHs (Nc = 50) do not survive in
shocks with velocities greater than 100 km/s and larger PAHs (Nc = 200) are
destroyed for shocks with velocities greater/equal to 125 km/s. For shocks in
the ~75 - 100 km/s range, where destruction is not complete, the PAH structure
is likely to be severely denatured by the loss of an important fraction
(20-40%) of the carbon atoms. We derive typical PAH lifetimes of the order of a
few x10^8 yr for the Galaxy. These results are robust and independent of the
uncertainties in some key parameters that have yet to be well-determined
experimentally. Conclusions: The observation of PAH emission in shock regions
implies that that emission either arises outside the shocked region or that
those regions entrain denser clumps that, unless they are completely ablated
and eroded in the shocked gas, allow dust and PAHs to survive in extreme
environments.Comment: 19 pages, 11 figures, 3 tables, typos corrected and PAH acronym in
the title substituted with full name to match version published in Astronomy
and Astrophysic
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