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Register a new userThermal and energetic processing of astrophysical ice analogues rich in SO$_2$
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Sulfur is an abundant element in the cosmos and it is thus an important contributor to astrochemistry in the interstellar medium and in the Solar System. Astronomical observations of the gas and of the solid phases in the dense interstellar/circumstellar regions have evidenced that sulfur is underabundant. The hypothesis to explain such a circumstance is that it is incorporated in some species in the solid phase (i.e. as frozen gases and/or refractory solids) and/or in the gas phase, which for different reasons have not been observed so far. Here we wish to give a contribution to the field by studying the chemistry induced by thermal and energetic processing of frozen mixtures of sulfur dioxide (one of the most abundant sulfur-bearing molecules observed so far) and water. We present the results of a series of laboratory experiments concerning thermal processing of different H2O:SO2 mixtures and ion bombardment 30 keV He$^+$ of the same mixtures. We used in situ FTIR spectroscopy to investigate the induced effects. The results indicate that ionic species such as HSO$_{3}^{-}$, HSO$_{4}^{-}$, and S$_2$O$_{5}^{2-}$ are easily produced. Energetic processing also produces SO$_3$ polymers and a sulfurous refractory residue. The produced ionic species exhibit spectral features in a region that, in astronomical spectra of dense molecular clouds, is dominated by strong silicate absorption. However, such a dominant feature is associated with some spectral features, some of which have not yet been identified. We suggest adding the sulfur-bearing ionic species to the list of candidates to help explain some of those features.
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Formic acid (HCOOH) has been extensively detected in space environments, including interstellar medium (gas and grains), comets and meteorites. Such environments are often subjected to the action of ionizing agents, which may cause changes in the molecular structure, thus leading to formation of new species. Formic acid is a possible precursor of pre-biotic species, such as Glycine (NH2CH2COOH). This work investigates experimentally the physicochemical effects resulting from interaction of heavy and energetic cosmic ray analogues (46MeV 58Ni11+) in H2O:HCOOH (1:1) ice, at 15 K, in ultrahigh vacuum regime, using Fourier transform infrared spectrometry in the mid-infrared region (4000-600 cm-1 or 2.5-12.5 microns). After the bombardment, the sample was slowly heated to room temperature. The results show the dissociation cross-section for the formic acid of 2.4x10^-13 cm2, and half-life due to galactic cosmic rays of 8x10^7 yr. The IR spectra show intense formation of CO and CO2, and small production of more complex species at high fluences.
2-aminooxazole (2AO), a N-heterocyclic molecule, has been proposed as an intermediate in prebiotic syntheses. It has been demonstrated that it can be synthesized from small molecules such as cyanamide and glycoaldehyde, which are present in interstellar space. The aim of this work is to provide infrared spectra, in the solid phase for conditions typical of astrophysical environments and to estimate its stability toward UV photons and cosmic rays. Infrared (4000-600 cm$^{-1}$) absorption spectra at 20 K, 180 K, and 300 K, IR band strengths, and room temperature UV (120-250 nm) absorption spectra are given for the first time for this species. Destruction cross-sections of 9.5 10$^{-18}$ cm$^2$ and 2 10$^{-16}$ cm$^2$ were found in the irradiation at 20 K of pure 2AO and 2AO:H$_2$O ices with UV (6.3-10.9 eV) photons or 5 keV electrons, respectively. These data were used for the estimate of half-life times for the molecule in different environments. It is estimated that 2AO could survive UV radiation and cosmic rays in the ice mantles of dense clouds beyond cloud collapse. In contrast, it would be very unstable at the surface of cold Solar System bodies like Kuiper belt objects, but the molecule could still survive within dust grain agglomerates or cometesimals.
HCN is a molecule central to interstellar chemistry, since it is the simplest molecule containing a carbon-nitrogen bond and its solid state chemistry is rich. The aim of this work was to study the NH3 + HCN -> NH4+CN- thermal reaction in interstellar ice analogues. Laboratory experiments based on Fourier transform infrared spectroscopy and mass spectrometry were performed to characterise the NH4+CN- reaction product and its formation kinetics. This reaction is purely thermal and can occur at low temperatures in interstellar ices without requiring non-thermal processing by photons, electrons or cosmic rays. The reaction rate constant has a temperature dependence of k(T) = 0.016+0.010-0.006 s-1.exp((-2.7+-0.4 kJmol-1)/(RT)) when NH3 is much more abundant than HCN. When both reactants are diluted in water ice, the reaction is slowed down. We have estimated the CN- ion band strength to be A_CN- = 1.8+-1.5 x10-17 cm molec-1 at both 20 K and 140 K. NH4+CN- exhibits zeroth-order multilayer desorption kinetics with a rate of k_des(T) = 10^28 molecules cm-2 s-1.exp((-38.0+-1.4 kJmol-1)/(RT)). The NH3 + HCN -> NH4+CN- thermal reaction is of primary importance because (i) it decreases the amount of HCN available to be hydrogenated into CH2NH, (ii) the NH4+ and CN- ions react with species such as H2CO, or CH2NH to form complex molecules, and (iii) NH4+CN- is a reservoir of NH3 and HCN, which can be made available to a high temperature chemistry.
Millimeter and centimeter observations are discovering an increasing number of interstellar complex organic molecules (iCOMs) in a large variety of star forming sites, from the earliest stages of star formation to protoplanetary disks and in comets. In this context it is pivotal to understand how the solid phase interactions between iCOMs and grain surfaces influence the thermal desorption process and, therefore, the presence of molecular species in the gas phase. In laboratory, it is possible to simulate the thermal desorption process deriving important parameters such as the desorption temperatures and energies. We report new laboratory results on temperature-programmed desorption (TPD) from olivine dust of astrophysical relevant ice mixtures of water, acetonitrile, and acetaldehyde. We found that in the presence of grains, only a fraction of acetaldehyde and acetonitrile desorbs at about 100 K and 120 K respectively, while 40% of the molecules are retained by fluffy grains of the order of 100 {mu}m up to temperatures of 190-210 K. In contrast with the typical assumption that all molecules are desorbed in regions with temperatures higher than 100 K, this result implies that about 40% of the molecules can survive on the grains enabling the delivery of volatiles towards regions with temperatures as high as 200 K and shifting inwards the position of the snowlines in protoplanetary disks. These studies offer a necessary support to interpret observational data and may help our understanding of iCOMs formation providing an estimate of the fraction of molecules released at various temperatures.
Enceladus, a small icy moon of Saturn, is one of the most remarkable bodies in the solar system. This moon is a geologically active object, and despite the lower temperatures on most of its surface, the geothermally heated south polar region presents geysers that spouts a plume made of water (approximately ninety percent), carbon dioxide, methane, ammonia, and methanol, among other molecules. Most of the upward-moving particles do not have the velocity to escape from the gravitational influence of the moon and fall back to the surface. The molecules in the ice are continuously exposed to ionizing radiation, such as UV and X-rays photons, cosmic rays, and electrons. Over time, the ionizing radiation promotes molecular bond rupture, destroying and also forming molecules, radicals, and fragments. We analyse the processing of an ice mixture analogue to the Enceladus fallout ice in cold resurfaced areas (north pole) by 1 keV electrons. The main goal is to search for complex species that have not yet been detected in this moon, and to determine relevant physico-chemical parameters, such as destruction and formation cross-sections and the half-life of the studied molecules in the ice. The experiment consisted of the electron irradiation of an Enceladus-like ice mixture (H2O,CO2,CH4,NH3, and CH3OH) in an ultra-high vacuum chamber at 20 K. The analysis was made by infrared spectrometry in the mid-infrared region (4000-800 cm-1 or 2.5-12.5 microns).The absolute dissociation cross-sections of the parent molecules, the formation cross-section of daughter species, and the half-life of the parental species in a simulated Enceladus irradiation scenario were determined. Among the produced species, CO (carbon monoxide), OCN- (cyanate anion), HCONH2 (formamide), and H2CO (formaldehyde) were tentatively detected.
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