Aims. The main goal of this work is to compare the effects induced in ices of astrophysical relevance by high-energy ions, simulating cosmic rays, and by vacuum ultraviolet (UV) photons. Methods. ...This comparison relies on in situ infrared spectroscopy of irradiated CH3OH:NH3 ice. Swift heavy ions were provided by the GANIL accelerator. The source of UV was a microwave-stimulated hydrogen flow discharge lamp. The deposited energy doses were similar for ion beams and UV photons to allow a direct comparison. Results. A variety of organic species was detected during irradiation and later during ice warm-up. These products are common to ion and UV irradiation for doses up to a few tens of eV per molecule. Only the relative abundance of the CO product, after ice irradiation, was clearly higher in the ion irradiation experiments. Conclusions. For some ice mixture compositions, the irradiation products formed depend only weakly on the type of irradiation, swift heavy ions, or UV photons. This simplifies the chemical modeling of energetic ice processing in space.
ABSTRACT
Water ices at 15 and 144 K were bombarded by swift heavy ions, 45.8 MeV 58Ni11 + and 606 MeV 64Zn26 +, to measure the induced chemical and physical effects. The column densities of water and ...the synthesized species, hydrogen peroxide (H2O2) and ozone (O3), were monitored via infrared spectroscopy. The formation and destruction cross-sections of precursor and products were determined and compared with literature. The H2O2 formation and destruction cross-sections reveal a linear dependence with electronic stopping power, σ ∝ Se. The sputtering yield (Y0) shows a power law with electronic energy lost, $Y_0\propto S_\mathrm{e}^2$, and an exponential increase with the sample temperature. The findings indicate that the radiolysis rate of water ice is higher at low temperatures while the desorption yield increases at higher temperatures. A large amount of water ice is located in the grain mantles of the circumstellar envelopes and the interstellar medium regions, which are exposed to galactic cosmic rays (GCRs). The synthesis of H2O2 and O3 molecules as a function of absorbed doses of GCR irradiation and their irradiation time is analysed in detail. Besides, the extrapolation of the sputtering yield rates, as a function of time and temperature, for astrophysical conditions can contribute to a better understanding of non-thermal sputtering of water ices.
Context. Under cosmic irradiation, the interstellar water ice mantles evolve towards a compact amorphous state. Crystalline ice amorphisation was previously monitored mainly in the keV to hundreds of ...keV ion energies. Aims. We experimentally investigate heavy ion irradiation amorphisation of crystalline ice, at high energies closer to true cosmic rays, and explore the water-ice sputtering yield. Methods. We irradiated thin crystalline ice films with MeV to GeV swift ion beams, produced at the GANIL accelerator. The ice infrared spectral evolution as a function of fluence is monitored with in-situ infrared spectroscopy (induced amorphisation of the initial crystalline state into a compact amorphous phase). Results. The crystalline ice amorphisation cross-section is measured in the high electronic stopping-power range for different temperatures. At large fluence, the ice sputtering is measured on the infrared spectra, and the fitted sputtering-yield dependence, combined with previous measurements, is quadratic over three decades of electronic stopping power. Conclusions. The final state of cosmic ray irradiation for porous amorphous and crystalline ice, as monitored by infrared spectroscopy, is the same, but with a large difference in cross-section, hence in time scale in an astrophysical context. The cosmic ray water-ice sputtering rates compete with the UV photodesorption yields reported in the literature. The prevalence of direct cosmic ray sputtering over cosmic-ray induced photons photodesorption may be particularly true for ices strongly bonded to the ice mantles surfaces, such as hydrogen-bonded ice structures or more generally the so-called polar ices.
ABSTRACT
The interstellar chemistry of nitrogen is considerably less understood than the chemistry of other common elements, such as carbon and oxygen. Even though a relatively large number of ...species containing nitrogen atoms have already been detected in the interstellar medium, only six of them bear a nitrogen–oxygen (N–O) bond. Some astrophysical and primeval Earth models suggest that N–O species, such as hydroxylamine (NH2OH), are potential precursors of prebiotic amino acids, and even peptides. In this work, we have analyzed an apolar ice mixture of N2:CO of astrophysical interest to investigate possible formation mechanisms of N–O bearing molecules due to processing of the sample by 64Ni24+ 538 MeV ions (8.4 MeV/u) at 14 K. The results show the formation of simple nitrogen oxides ($\rm {N_{1 - 2}}{O_y})$, but no CN–O species of any kind. We have also determined the formation cross-sections of some of the products, as well as the destruction cross-sections of precursors and products. The results presented here are discussed in light of our previous work on the processing of a NH3:CO ice mixture, which have found no N–O bearing molecules at all.
ABSTRACT
Carbon monoxide (CO) plays a vital role in interstellar chemistry, existing abundantly in both gaseous and frozen environments. Understanding the radiation-driven chemistry of CO-rich ices ...is crucial for comprehending the formation and desorption of C-bearing molecules in the interstellar medium (ISM), particularly considering the potential impact of temperature on these processes. We report experimental data on irradiation processing of pure CO ice by cosmic ray analogues (95.2 MeV 136Xe23+ ions) at temperatures of 10, 15, and 20 K, in the IGLIAS set-up coupled to the IRRSUD beamline at GANIL (Caen, France). The evolution of the irradiated frozen samples was monitored by infrared spectroscopy. The computational PROCODA code allows us to quantify the chemical evolution of the samples, determining effective reaction rates coefficients (ERCs), molecular abundances at the chemical equilibrium (CE) phase, and desorption processes. The model integrated 18 chemical species – 8 observed (CO, CO2, C3, O3, C2O, C3O, C3O2, and C5O3) and 10 non-observed but predicted (C, O, C2, O2, CO3, C4O, C5O, C2O2, C2O3, C4O2) – linked via 156 reactions. Our findings reveal temperature-driven influences on molecular abundances at chemical equilibrium, desorption yields and rates, and ERC values. Certain reaction routes exhibit distinct thermochemical behaviours of gas- and ice-phase reactions which may be attributed to the presence of neighbouring molecules within the ice matrix. This study provides pivotal insights into the chemical evolution of CO-enriched ice under irradiation, impacting solid-state astrochemistry, clarifying molecular abundances, and advancing our understanding of ISM chemistry and temperature effects on ionized radiation-processed frozen ices.
ABSTRACT
Experimental results on the processing of NH3:CO ice mixtures of astrophysical relevance by energetic (538 MeV 64Ni24+) projectiles are presented. NH3 and CO are two molecules relatively ...common in interstellar medium and Solar system; they may be precursors of amino acids. 64Ni ions may be considered as representative of heavy cosmic ray analogues. Laboratory data were collected using mid-infrared Fourier transform spectroscopy and revealed the formation of ammonium cation (NH$_4^+$), cyanate (OCN−), molecular nitrogen (N2), and CO2. Tentative assignments of carbamic acid (NH2COOH), formate ion (HCOO−), zwitterionic glycine (NH$_3^+$CH2COO−), and ammonium carbamate (NH$_4^+$NH2COO−) are proposed. Despite the confirmation on the synthesis of several complex species bearing C, H, O, and N atoms, no N–O-bearing species was detected. Moreover, parameters relevant for computational astrophysics, such as destruction and formation cross-sections, are determined for the precursor and the main detected species. Those values scale with the electronic stopping power (Se) roughly as σ ∼ a S$_\mathrm{ e}^n$, where n ∼ 3/2. The power law is helpful for predicting the CO and NH3 dissociation and CO2 formation cross-sections for other ions and energies; these predictions allow estimating the effects of the entire cosmic ray radiation field.
ABSTRACT Radiolysis of α-pinene by 61.3 MeV 84Kr15 + ions was analysed with the scope to simulate the effects of heavy ion cosmic ray bombardment on chiral molecules in the interstellar medium. The ...α-pinene ice samples were irradiated at 10 K and their chemical evolution was monitored by mid-infrared Fourier transform (FTIR) spectroscopy to characterize the reaction products and to determine the extent of racemization. The integrated band strengths have been obtained for all the neutral α-pinene vibrational bands using the experimental band integrated absorbances and the theoretical absolute intensities calculated along the column densities. In the current heavy ion bombardment experiments, small molecules were formed and the precursor, α-pinene, was destroyed instead of being racemized. Twelve hydrocarbons were produced (final fluence of 2.0 × 1012 ions cm−2): methane (CH4), acetylene (C2H2), ethylene (C2H4), propylene (C3H6), propane (C3H8), n-butane (C4H10), butene (C4H8), propyne (C3H4), benzene (C6H6), ethane (C2H6), vinylacetylene (C4H4), and 2-methyl-1,3-butadiene or isoprene (C5H8). The highest formation cross-section (∼ 40 × 10−15 cm2) was observed for the C3H4 and the lowest was for C3H8 (∼ 3 × 10−15 cm2). The radiochemical yields for these molecules follow the same trends as those of their cross-sections. The atom budget calculation confirms that all the expected products have been generated during the radiolysis and supports the conclusion that the proposed A values are accurate. The α-pinene sputtering yield for this ion beam was found to be Y0 = 1.84 × 106 molecules per impact.
Deep inside dense molecular clouds and protostellar disks, interstellar ices are protected from stellar energetic UV photons. However, X-rays and energetic cosmic rays can penetrate inside these ...regions triggering chemical reactions, molecular dissociation, and evaporation processes. We present experimental studies of the interaction of heavy, highly charged, and energetic ions (46 MeV 58Ni13+) with ammonia-containing ices H2O:NH3 (1:0.5) and H2O:NH3:CO (1:0.6:0.4) in an attempt to simulate the physical chemistry induced by heavy-ion cosmic rays inside dense astrophysical environments. The measurements were performed inside a high vacuum chamber coupled to the IRRSUD (IR radiation SUD) beamline at the heavy-ion accelerator GANIL (Grand Accelerateur National d'Ions Lourds) in Caen, France. The gas samples were deposited onto a polished CsI substrate previously cooled to 13 K. In-situ analysis was performed by a Fourier transform infrared spectrometer (FTIR) at different fluences. The average values of the dissociation cross-section of water, ammonia, and carbon monoxide due to heavy-ion cosmic ray analogs are ~$2 \times 10^{-13}$, $1.4 \times 10^{-13}$, and $1.9 \times 10^{-13}$ cm2, respectively. In the presence of a typical heavy cosmic ray field, the estimated half life of the studied species is 2–$3 \times 10^6$ years. The ice compaction (micropore collapse) produced by heavy cosmic rays seems to be at least 3 orders of magnitude higher than that produced by (0.8 MeV) protons. The infrared spectra of the irradiated ice samples exhibit lines of several new species including HNCO, N2O, OCN-, and NH$_4^+$. In the case of the irradiated H2O:NH3:CO ice, the infrared spectrum at room temperature contains five bands that are tentatively assigned to vibration modes of the zwitterionic glycine (NH$_3^+$CH2COO-).
ABSTRACT
H2O:CO, at concentrations of (3:2) and (10:1), was condensed on CsI substrate at 15 K and irradiated with 46-MeV 58Ni11 + ion beam. Radiolysis induced by fast heavy ions was analyzed by ...infrared spectroscopy (FTIR). The formation of nine molecular species: CO2, H2O2, HCOOH, HCO, H2CO, 13CO2, CH3OH, O3, and C3O2 was observed. For both concentrations, carbon dioxide (CO2), formaldehyde (H2CO), formic acid (HCOOH), and hydrogen peroxide (H2O2) are the most abundant products species, and tricarbon dioxide (C3O2) is much less abundant. Precursor destruction cross-sections and formation cross-sections of products are determined. The CO destruction cross-section for the (3:2) concentration is almost five times higher than that of water, while those for the (10:1) concentration are practically the same. Atomic sputtering yields are estimated for the two ice films, the total mass sputtered is approximately 2.5 × 106 u per impact. These results contribute to figure out the chemical pathways of compounds synthesized from the two most abundant organic species (H2O and CO) observed in the ices of grain mantles of the circumstellar envelopes and interstellar medium. In additional, the finding results reveal that molecular astronomical percentages are comparable to those obtained after 15 eV molec−1 of deposited dose in current experiments compared with the relative concentration of molecules in solid phase observed in MYSO, LYSO, BG Stars, and Comets.
ABSTRACT
The processing of H2O:CO2:CH4 (10:1:1) and H2O:CO2:CH4:NH3 (10:1:1:1) ices at 72 K by oxygen ions was studied in an attempt to simulate the physicochemical effects induced by energetic ions ...on the surface of Enceladus (or similar cold surfaces in the outer Solar System). The experiments were carried out at the Grand Accélérateur National d’Ions Lourds (GANIL) in Caen/France. The samples were irradiated with 15.7-MeV O5+ at the IRRadiation SUD (IRRSUD) beamline and with 108-keV O6+ at the Accélérateurs pour les Recherches avec les Ions de Basses Energies (ARIBE) beamline. The frozen samples were monitored by Fourier Transform Infrared Spectroscopy (FTIR) spectroscopy (4000–650 cm−1, 2.5–15.4 μm, at 1 cm−1 resolution). The identified molecular species formed during irradiation were CO, OCN−, CH3OH, HCN, CN−, H2CO3, HNCO, HCO and CO3. The effective formation cross-sections for the synthesis of new species and the effective molecular destruction cross-sections of the parent species in the experiments with MeV ions were found to be of the order of 10−14–10−13 cm2. For the keV ion experiments, these values were of the order of 10−16–10−15 cm2. The fluence at which the sample reaches chemical equilibrium and the molecular abundances in this region (equilibrium branching ratios) were estimated. These experiments suggest that the chemical inventory on the surface of Enceladus can be influenced by the incidence of charged particles on to the moon’s surface.
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