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We present a model for the formation of large organic molecules in dark clouds. The molecules are produced in the high density gas-phase that exists immediately after ice mantles are explosively sublimated. The explosions are initiated by the catastrophic recombination of trapped atomic hydrogen. We propose that, in molecular clouds, the processes of freeze-out onto ice mantles, accumulation of radicals, explosion and then rapid (three-body) gas-phase chemistry occurs in a cyclic fashion. This can lead to a cumulative molecular enrichment of the interstellar medium. A model of the time-dependent chemistries, based on this hypothesis, shows that significant abundances of large molecular species can be formed, although the complexity of the species is limited by the short expansion timescale in the gas, immediately following mantle explosion. We find that this mechanism may be an important source of smaller organic species, such as methanol and formaldehyde, as well as precursors to bio-molecule formation. Most significantly, we predict the gas-phase presence of these larger molecular species in quiescent molecular clouds and not just dynamically active regions, such as hot cores. As such the mechanism that we propose complements alternative methods of large molecule formation, such as those that invoke solid-state chemistry within activated ice mantles.
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Isolated dense molecular cores are investigated to study the onset of complex organic molecule formation in interstellar ice. Sampling three cores with ongoing formation of low-mass stars (B59, B335, and L483) and one starless core (L694-2) we sample lines of sight to nine background stars and five young stellar objects (YSOs; A_K ~0.5 - 4.7). Spectra of these stars from 2-5 $mu$m with NASAs Infrared Telescope Facility (IRTF) simultaneously display signatures from the cores of H$_2$O (3.0 $mu$m), CH$_3$OH (C-H stretching mode, 3.53 $mu$m) and CO (4.67 $mu$m) ices. The CO ice is traced by nine stars in which five show a long wavelength wing due to a mixture of CO with polar ice (CO$_r$), presumably CH$_3$OH. Two of these sight lines also show independent detections of CH$_3$OH. For these we find the ratio of the CH$_3$OH:CO$_r$ is 0.55$pm$0.06 and 0.73$pm$0.07 from L483 and L694-2, respectively. The detections of both CO and CH$_3$OH for the first time through lines of sight toward background stars observationally constrains the conversion of CO into CH$_3$OH ice. Along the lines of sight most of the CO exists in the gas phase and $leq$15% of the CO is frozen out. However, CH$_3$OH ice is abundant with respect to CO (~50%) and exists mainly as a CH$_3$OH-rich CO ice layer. Only a small fraction of the lines of sight contains CH$_3$OH ice, presumably that with the highest density. The high conversion of CO to CH$_3$OH can explain the abundances of CH$_3$OH ice found in later stage Class 1 low mass YSO envelopes (CH$_3$OH:CO$_r$ ~ 0.5-0.6). For high mass YSOs and one Class 0 YSO this ratio varies significantly implying local variations can affect the ice formation. The large CH$_3$OH ice abundance indicates that the formation of complex organic molecules is likely during the pre-stellar phase in cold environments without higher energy particle interactions (e.g. cosmic rays).
We present the spatially-resolved near-infrared (2.5-5.0 um) spectra of the edge-on starburst galaxy NGC253 obtained with the Infrared Camera onboard AKARI. Near the center of the galaxy, we clearly detect the absorption features of interstellar ices (H_2O: 3.05 um, CO_2: 4.27 um, and XCN: 4.62 um) and the emission of polycyclic aromatic hydrocarbons (PAHs) at 3.29 um and hydrogen recombination line Br alpha at 4.05 um. We find that the distributions of the ices differ from those of the PAH and gas. We calculate the column densities of the ices and derive the abundance ratios of N(CO_2)/N(H_2O) = 0.17 +- 0.05. They are similar to those obtained around the massive young stellar objects in our Galaxy (0.17 +- 0.03), although much stronger interstellar radiation field and higher dust temperature are expected near the center of NGC253.
Spectroscopic studies play a key role in the identification and analysis of interstellar ices and their structure. Some molecules have been identified within the interstellar ices either as pure, mixed, or even as layered structures. Absorption band features of water ice can significantly change with the presence of different types of impurities (CO, CO2, CH3OH, H2CO, etc.). In this work, we carried out a theoretical investigation to understand the behavior of water band frequency, and strength in the presence of impurities. The computational study has been supported and complemented by some infrared spectroscopy experiments aimed at verifying the effect of HCOOH, NH3 , and CH3 OH on the band profiles of pure H2O ice. Specifically, we explored the effect on the band strength of libration, bending, bulk stretching, and free-OH stretching modes. Computed band strength profiles have been compared with our new and existing experimental results, thus pointing out that vibrational modes of H2O and their intensities can change considerably in the presence of impurities at different concentrations. In most cases, the bulk stretching mode is the most affected vibration, while the bending is the least affected mode. HCOOH was found to have a strong influence on the libration, bending, and bulk stretching band profiles. In the case of NH3, the free-OH stretching band disappears when the impurity concentration becomes 50%. This work will ultimately aid a correct interpretation of future detailed spaceborne observations of interstellar ices by means of the upcoming JWST mission.
In this work, we reexamine sulfur chemistry occurring on and in the ice mantles of interstellar dust grains, and report the effects of two new modifications to standard astrochemical models; namely, (a) the incorporation of cosmic ray-driven radiation chemistry and (b) the assumption of fast, non-diffusive reactions for key radicals in the bulk. Results from our models of dense molecular clouds show that these changes can have a profound influence on the abundances of sulfur-bearing species in ice mantles, including a reduction in the abundance of solid-phase H$_2$S and HS, and a significant increase in the abundances of OCS, SO$_2$, as well as pure allotropes of sulfur, especially S$_8$. These pure-sulfur species - though nearly impossible to observe directly - have long been speculated to be potential sulfur reservoirs and our results represent possibly the most accurate estimates yet of their abundances in the dense ISM. Moreover, the results of these updated models are found to be in good agreement with available observational data. Finally, we examine the implications of our findings with regard to the as-yet-unknown sulfur reservoir thought to exist in dense interstellar environments.
We present experimental measurements of photodesorption from ices of astrophysical relevance. Layers of benzene and water ice were irradiated with a laser tuned to an electronic transition in the benzene molecule. The translational energy of desorbed molecules was measured by time-of-flight (ToF) mass spectrometry. Three distinct photodesorption processes were identified - a direct adsorbate-mediated desorption producing benzene molecules with a translational temperature of around 1200 K, an indirect adsorbate-mediated desorption resulting in water molecules with a translational temperature of around 450 K, and a substrate-mediated desorption of both benzene and water producing molecules with translational temperatures of around 530 K and 450 K respectively. The translational temperature of each population of desorbed molecules is well above the temperature of the ice matrix. The implications for gas-phase chemistry in the interstellar medium are discussed.
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