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Register a new userVacuum ultraviolet photoabsorption spectroscopy of space-related ices: 1 keV electron irradiation of nitrogen- and oxygen-rich ices
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Molecular oxygen, nitrogen, and ozone have been detected in the Solar System. They are also expected to be present in ice-grain mantles within star-forming regions. Laboratory experiments that simulate energetic processing (ions, photons, and electrons) of ices are essential for interpreting and directing future astronomical observations. We provide VUV photoabsorption spectroscopic data of energetically processed nitrogen- and oxygen-rich ices that will help to identify absorption bands and/or spectral slopes observed on icy objects in the Solar System and on ice-grain mantles of the interstellar medium. We present VUV photoabsorption spectra of frozen O2 and N2, a 1:1 mixture of both, and a new systematic set of pure and mixed nitrogen oxide ices. Spectra were obtained at 22 K before and after 1 keV electron bombardment of the ice sample. Ices were then annealed to higher temperatures to study their thermal evolution. In addition, Fourier-transform infrared spectroscopy was used as a secondary probe of molecular synthesis to better identify the physical and chemical processes at play. Our VUV data show that ozone and the azide radical (N3) are observed in our experiments after electron irradiation of pure O2 and N2 ices, respectively. Energetic processing of an O2:N2 = 1:1 ice mixture leads to the formation of ozone along with a series of nitrogen oxides. The electron irradiation of solid nitrogen oxides, pure and in mixtures, induces the formation of new species such as O2, N2 , and other nitrogen oxides not present in the initial ice. Results are discussed here in light of their relevance to various astrophysical environments. Finally, we show that VUV spectra of solid NO2 and water can reproduce the observational VUV profile of the cold surface of Enceladus, Dione, and Rhea, strongly suggesting the presence of nitrogen oxides on the surface of the icy Saturn moons.
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Carbonic acid (H2CO3) is a weak acid relevant to astrobiology which, to date, remains undetected in space. Experimental work has shown that the beta-polymorph of H2CO3 forms under space relevant conditions through energetic (UV photon, electron, and cosmic ray) processing of CO2- and H2O-rich ices. We present a systematic set of VUV photoabsorption spectra of pure and mixed CO2 and H2O ices exposed to 1 keV electrons at 20 and 80 K to simulate different interstellar and Solar System environments. Ices were then annealed to obtain a layer of pure H2CO3 which was further exposed to 1 keV electrons at 20 and 80 K to monitor its destruction pathway. Fourier-transform infrared (FT-IR) spectroscopy was used as a secondary probe providing complementary information on the physicochemical changes within an ice. Our laboratory work shows that the formation of solid H2CO3, CO, and O3 upon the energetic processing of CO2:H2O ice mixtures is temperature-dependent in the range between 20 and 80 K. The amorphous to crystalline phase transition of H2CO3 ice is investigated for the first time in the VUV spectral range by annealing the ice at 200 and 225 K. We have detected two photoabsorption bands at 139 and 200 nm, and we assigned them to beta-H2CO3 and gamma-H2CO3, respectively. We present VUV spectra of the electron irradiation of annealed H2CO3 ice at different temperatures leading to its decomposition into CO2, H2O, and CO ice. Laboratory results are compared to Cassini UltraViolet Imaging Spectrograph observations of the 70-90 K ice surface of Saturns satellites Enceladus, Dione, and Rhea.
Non-thermal desorption from icy grains containing H$_2$CO has been invoked to explain the observed H$_2$CO gas phase abundances in ProtoPlanetary Disks (PPDs) and Photon Dominated Regions (PDRs). Photodesorption is thought to play a key role, however no absolute measurement of the photodesorption from H$_2$CO ices were performed up to now, so that a default value is used in the current astrophysical models. As photodesorption yields differ from one molecule to the other, it is crucial to experimentally investigate photodesorption from H$_2$CO ices. We measured absolute wavelength-resolved photodesorption yields from pure H$_2$CO ices, H$_2$CO on top of a CO ice (H$_2$CO/CO), and H$_2$CO mixed with CO ice (H$_2$CO:CO) irradiated in the Vacuum UltraViolet (VUV) range (7-13.6~eV). Photodesorption from a pure H$_2$CO ice releases H$_2$CO in the gas phase, but also fragments, such as CO and H$_2$. Energy-resolved photodesorption spectra, coupled with InfraRed (IR) and Temperature Programmed Desorption (TPD) diagnostics, showed the important role played by photodissociation and allowed to discuss photodesorption mechanisms. For the release of H$_2$CO in the gas phase, they include Desorption Induced by Electronic Transitions (DIET), indirect DIET through CO-induced desorption of H$_2$CO and photochemical desorption. We found that H$_2$CO photodesorbs with an average efficiency of $sim 4-10 times 10^{-4}$ molecule/photon, in various astrophysical environments. H$_2$CO and CO photodesorption yields and photodesorption mechanisms, involving photofragmentation of H$_2$CO, can be implemented in astrochemical codes. The effects of photodesorption on gas/solid abundances of H$_2$CO and all linked species from CO to Complex Organic Molecules (COMs), and on the H$_2$CO snowline location, are now on the verge of being unravelled.
Oxygen atom addition and insertion reactions may provide a pathway to chemical complexity in ices that are too cold for radicals to diffuse and react. We have studied the ice-phase reactions of photo-produced oxygen atoms with C2 hydrocarbons under ISM-like conditions. The main products of oxygen atom reactions with ethane are ethanol and acetaldehyde; with ethylene are ethylene oxide and acetaldehyde; and with acetylene is ketene. The derived branching ratio from ethane to ethanol is ~0.74 and from ethylene to ethylene oxide is ~0.47. For all three hydrocarbons there is evidence of an effectively barrierless reaction with O(^1D) to form oxygen-bearing organic products; in the case of ethylene, there may be an additional barriered contribution of the ground-state O(^3P) atom. Thus, oxygen atom reactions with saturated and unsaturated hydrocarbons are a promising pathway to chemical complexity even at very low temperatures where the diffusion of radical species is thermally inaccessible.
Sensitive 5-38 um Spitzer Space Telescope (SST) and ground based 3-5 um spectra of the embedded low mass protostars B5 IRS1 and HH46 IRS show deep ice absorption bands superposed on steeply rising mid-infrared continua. The ices likely originate in the circumstellar envelopes. The CO2 bending mode at 15 um is a particularly powerful tracer of the ice composition and processing history. Toward these protostars, this band shows little evidence for thermal processing at temperatures above 50 K. Signatures of lower temperature processing are present in the CO and OCN- bands, however. The observed CO2 profile indicates an intimate mixture with H2O, but not necessarily with CH3OH, in contrast to some high mass protostars. This is consistent with the low CH3OH abundance derived from the ground based L band spectra. The CO2/H2O column density ratios are high in both B5 IRS1 and HH46 IRS (~35%). Clearly, the SST spectra are essential to study ice evolution in low mass protostellar environments, and to eventually determine the relation between interstellar and solar system ices.
Ices are an important constituent of protoplanetary disks. New observational facilities, notably JWST, will greatly enhance our view of disk ices by measuring their infrared spectral features. We present a suite of models to complement these upcoming observations. Our models use a kinetics-based gas-grain chemical evolution code to simulate the distribution of ices in a disk, followed by a radiative transfer code using a subset of key ice species to simulate the observations. We present models reflecting both molecular inheritance and chemical reset initial conditions. We find that H$_2$O, CO$_2$, and CH$_3$OH near-to-mid-IR absorption features are readily observable in disk-integrated spectra of highly-inclined disks while CO, NH$_3$, and CH$_4$ ice do not show prominent features. CH$_3$OH ice has low abundance and is not observable in the reset model, making this species an excellent diagnostic of initial chemical conditions. CO$_2$ ice features exhibit the greatest change over disk lifetime: decreasing and increasing for the inheritance and reset models, respectively. Spatially-resolved spectra of edge-on disks, possible with JWSTs integral field unit observing modes, are ideal for constraining the vertical distribution of ices and may be able to isolate features from ices closer to the midplane (e.g., CO) given sufficient sensitivity. Spatially-resolved spectra of face-on disks can trace scattered-light features from H$_2$O, CO$_2$, and CH$_3$OH, plus CO and CH$_4$ from the outermost regions. We additionally simulate far-IR H$_2$O ice emission features and find they are strongest for disks viewed face-on.
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