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This brief overview stresses the importance of laboratory data and theory in analyzing astronomical observations and understanding the physical and chemical processes that drive the astrophysical phenomena in our Universe. This includes basic atomic and molecular data such as spectroscopy and collisional rate coefficients, but also an improved understanding of nuclear, plasma and particle physics, as well as reactions and photoprocesses in the gaseous and solid state that lead to chemical complexity and building blocks for life. Systematic laboratory collision experiments have provided detailed insight into the steps that produce pebbles, bricks and ultimately planetesimals starting from sub-μ-sized grains. Sample return missions and meteoritic studies benefit from increasingly sophisticated laboratory machines to analyze materials and provide compositional images on nanometer scales. Prioritization of future data requirements will be needed to cope with the increasing data streams from a diverse range of future astronomical facilities within a constrained laboratory astrophysics budget.
The surfaces of interstellar and circumstellar dust grains are the sites of molecule formation, most of which, except H2, stick and form ice mantles. The study of ice evolution thus seems directly relevant for understanding our own origins, although the relation between interstellar and solar system ices remains a key question. The comparison of interstellar and solar system ices relies evidently on an accurate understanding of the composition and processes in both environments. With the accurate in situ measurements available for the comet 67P/Churyumov-Gerasimenko with the Rosetta mission, improving our understanding of interstellar ices is the more important. Here, I will address three specific questions. First, while laboratory experiments have made much progress in understanding complex organic molecule (COM) formation in the ices, the question remains, how does COM formation depend on environment and time? Second, what is the carrier of sulfur in the ices? And third, can ice absorption bands trace the processing history of the ices? Laboratory experiments, ranging from infrared spectroscopy to identify interstellar ice species, to surface experiments to determine reaction parameters in ice formation scenarios, to heating and irradiation experiments to simulate space environments, are essential to address these questions and analyze the flood of new observational data that will become available with new facilities in the next 2-10 years.
The goal of this contribution is to illustrate how spatially resolved spectroscopic observations of the infrared emission of UV irradiated regions, from star forming regions to the diffuse ISM, can be used to rationalize the chemical evolution of carbonaceous macromolecules in space, with the help of astrophysical models. For instance, observations with the Spitzer space telescope lead to the idea that fullerenes (including C60 can form top-down from Polycyclic Aromatic Hydrocarbons in the interstellar medium. The possibility that this process can occur in space was tested using a photochemical model which includes the key molecular parameters derived from experimental and theoretical studies. This approach allows to test the likelihood that the proposed path is realistic, but, more importantly, it allows to isolate the key physical processes and parameters that are required to capture correctly the evolution of carbonaceous molecules in space. In this specific case, we found that relaxation through thermally excited electronic states (a physical mechanism that is largely unexplored, except by few a teams) is one of the keys to model the photochemistry of the considered species. Subsequent quantum chemical studies stimulated by the (limited) astrophysical model showed that a detailed mapping of the energetics of isomerization and de-hydrogenation is necessary to understand the competition between these processes in space.
Such approaches, involving experimentalists and theoreticians, are particularly promising in the context of the upcoming JWST mission, which will provide access to the signatures of carbonaceous species in emission and in absorption at an angular resolution that will enable to reach new chemical frontiers in star and even in planet forming regions.
The existence of cosmic dust is attested by the interstellar extinction and polarization, IR emission and absorption spectra, and elemental depletion patterns. Dust grains are efficiently processed or even destroyed in shocks, molecular clouds, or protoplanetary disks. A considerable amount of dust has to be re-formed in the ISM. In various astrophysical environments, dust grains are covered by molecular ices and therefore contribute or catalytically influence the chemical reactions in these layers. Laboratory experiments are desperately required to understand the evolution of grains and grain/ice mixtures in molecular clouds and early planetary disks. This review considers recent progress in laboratory approaches to dust/ice experiments.
Recent experimental and theoretical works concerning gas-phase radical-neutral reactions involving Complex Organic Molecules are reviewed in the context of cold interstellar objects with a special emphasis on the OH + CH3OH reaction and its potential impact on the formation of CH3O.
Two laboratory emission spectrometers have been designed and described previously. Here, we present a follow-up study with special focus on absolute intensity calibration of the new SURFER-spectrometer (SUbmillimeter Receiver For Emission spectroscopy of Rotational transitions), operational between 300 and 400 GHz and coincident with ALMA (Atacama Large Millimeter/submillimeter Array) Band 7.
Furthermore, we present a feasibility study to extend the detection frequencies up to 2 THz. First results have been obtained using the SOFIA (Stratospheric Observatory for IR Astronomy) upGREAT laboratory setup which is located at the University of Cologne. Pure rotational spectra of the complex molecule vinyl cyanide have been obtained and are used to give an estimate on the sensitivity to record ro-vibrational transitions of molecules with astrophysical importance at 2 THz.
Complex organic molecules (COMs) have been detected in the gas-phase in cold and lightless molecular cores. Recent solid-state laboratory experiments have provided strong evidence that COMs can be formed on icy grains through ‘non-energetic’ processes. In this contribution, we show that propanal and 1-propanol can be formed in this way at the low temperature of 10 K. Propanal has already been detected in space. 1-propanol is an astrobiologically relevant molecule, as it is a primary alcohol, and has not been astronomically detected. Propanal is the major product formed in the C2H2 + CO + H experiment, and 1-propanol is detected in the subsequent propanal + H experiment. ALMA observations towards IRAS 16293-2422B are discussed and provide a 1-propanol:propanal upper limit of < 0.35–0.55, which are complemented by computationally-derived activation barriers in addition to the performed laboratory experiments.
A key element when modeling dust in any astrophysical environment is a self-consistent treatment of the evolution of the dust material properties (size distribution, chemical composition and structure) as they react to and adjust to the local radiation field intensity and hardness and to the gas density and dynamics. The best way to achieve this goal is to anchore as many model parameters as possible to laboratory data. In this paper, I present two examples to illustrate how outstanding questions in dust modeling have been/are being moved forward by recent advances in laboratory astrophysics and what laboratory data are still needed to further advance dust evolution models.
An exotic molecular inventory exists in space. While some species have well-known terrestrial analogs, others are very reactive and can hardly survive in the laboratory timely to allow for their characterization. With an eye toward these latter, we highlight in this contribution the role of quantum chemistry in providing astrochemically relevant data where experiment struggles. Special attention is given to the concept of molecular potential energy surfaces (PESs), a key aspect in theoretical chemical physics, and the possible dynamical attributes taken therefrom. As case studies, we outline our current efforts in obtaining global PESs of carbon clusters. It is thus hoped that, with such an active synergy between theoretical chemistry and state-of-the-art experimental/observational techniques (the pillars to the modern laboratory astrophysics), scientists may gather the required knowledge to explain the origins, abundances and the driving force toward molecular complexity in the Universe.
The starting point for the development of any astrochemical model is the knowledge of whether a molecule is present in the astrophysical environment considered, with the astronomical observations of spectroscopic signatures providing the unequivocal proof of its presence. Among the goals of astrochemistry, the detection of potential prebiotic molecules in the interstellar medium and planetary atmospheres is fundamental in view of possibly understanding the origin of life. The detection of new molecules in space requires the spectroscopic signatures (mostly, rotational transition frequencies) to be accurately determined over a large frequency range. This task is more and more often the result of a synergic interplay of experiment and theory.
Recent observations revealed that there is a difference in the spatial distribution of both nitrogen and oxygen bearing species towards massive star forming regions. These differences can be explained under different temperature regimes in hot cores. In this study, we attempt to model the chemistry of few nitrogen species; namely, vinyl cyanide (CH2CHCN), ethyl cyanide (CH3CH2CN), and formamide (NH2CHO), using gas-grain chemical models. A special attention is given to the role and efficiency of surface chemistry as it is suggested to play one of the main key roles in manufacturing these species.
The James Webb Space Telescope (JWST) is expected to be launched in 2021. The JWST’s science instruments will provide high quality spectra acquired in the line of sight to young stellar objects whose interpretation will require a robust database of laboratory data. With this in mind, an experimental work is in progress in the Laboratory for Experimental Astrophysics in Catania to study the profile (shape, width, and peak position) of the main infrared bands of molecular species expected to be present in icy grain mantles. Our study also takes into account the modifications induced on icy samples by low-energy cosmic ray bombardment and by thermal processing. Here we present some recent results on deuterium hydrogen monoxide (HDO), N-bearing species, and carbon dioxide (CO2).
Dust particles covered by icy mantles play a crucial role in the formation of molecules in the Interstellar Medium (ISM). These icy mantles are mainly composed of water but many other chemical species are also contained in these ices. These compounds can diffuse and meet each other to react. It is through these surface reactions that new saturated species are formed. Photodissociation reactions are also thought to play a crucial role in the formation of radical species. Complex organic molecules are formed through an intricated network of photodissociation and surface reactions.
Both type of reactions release energy. Surface reactions are typically exothermic by a few eV, whereas photodissociation reactions are triggered by the absorption of a UV photon, resulting in the formation of highly excited products. The excited reaction products can apply this energy for desorption or diffusion, making products more mobile than predicted when considering only thermal hopping. The energy could further lead to annealing or deformation of the ice structure.
Here we would like to quantify the relative importance of these different energy dissipation routes. For this we performed thousands of Molecular Dynamics simulations for three different species (CO2, H2O and CH4) on top of a water ice surface. We consider different types of excitation such as translational, rotational, and/or vibrational excitation. The applied substrate is an amorphous solid water surface (ASW).
The initial chemical composition of a proto-planetary nebula depends upon the degree to which 1) organic and ice components form on dust grains, 2) organic and molecular species form in the gas phase, 3) organics and ices are exchanged between the gas and solid state, and 4) the precursor and newly formed (more complex) materials survive and are modified in the developing planetary system. Infrared and radio observations of star-forming regions reveal that complex chemistry occurs on icy grains, often before stars even form. Additional processing, through the proto-planetary disk (PPD) further modifies most, but not all, of the initial materials. In fact, the modern Solar System still carries a fraction of its interstellar inheritance (Alexander et al.2017). Here we focus on three examples of small bodies in our Solar System, each containing chemical and dynamical clues to its origin and evolution: the small-cold classical Kuiper Belt object (KBO) 2014 MU69, Pluto, and Saturn’s moon, Phoebe. The New Horizons flyby of 2014 MU69 has given the first view of an unaltered body composed of material originally in the solar nebula at ~45 AU. The spectrum of MU69 reveals methanol ice (not commonly found), a possible detection of water ice, and the noteworthy absence of methane ice (Stern et al. 2019). Pluto’s internal and surface inventory of volatiles and complex organics, together with active geological processes including cryo-volcanism, indicate a surprising level of activity on a body in the outermost region of the Solar System, and the fluid that emerges from subsurface reservoirs may contain material inherited from the solar nebula (Cruikshank et al.2019a,b). Meanwhile, Saturn’s captured moon, Phoebe, carries high D/H in H2O (Clark et al. 2019) and complex organics (Cruikshank et al. 2008), both consistent with its formation in, and inheritance from, the outer region of the solar nebula. Together, these objects provide windows on the origin and evolution of our Solar System and constraints to be considered in future chemical and physical models of PPDs.
The search for complex organic molecules in the interstellar medium (ISM) has revealed species of ever greater complexity. This search relies on the progress made in the laboratory to characterize their rotational spectra. Our understanding of the processes that lead to molecular complexity in the ISM builds on numerical simulations that use chemical networks fed by laboratory and theoretical studies. The advent of ALMA and NOEMA has opened a new door to explore molecular complexity in the ISM. Their high angular resolution reduces the spectral confusion of star-forming cores and their increased sensitivity allows the detection of low-abundance molecules that could not be probed before. The complexity of the recently-detected molecules manifests itself not only in terms of number of atoms but also in their molecular structure. We discuss these developments and report on ReMoCA, a new spectral line survey performed with ALMA toward the high-mass star-forming region Sgr B2(N).
Increasing evidences suggest that the building blocks of Ca-Al-rich inclusions (CAIs) could have formed with the Sun, during the collapse of the parent cloud. However, determination of the relative age of CAIs relies on the homogeneous distribution of their short-lived radionuclide 26Al that is used as a chronometer. Some CAIs show evidence of 26Al/27 Al variation that is independent of decay.
We investigate the dynamical and chemical evolution of refractories from the collapsing cloud to their transport in the protoplanetary disk focusing to the predicted isotopic anomalies resulting from 26Al heterogeneities.
The interplay between the thermal properties of the dust, the isotopic zoning in the cloud and disk dynamics produce aggregates that resemble chondrites. An abrupt raise of 26Al close the center of the cloud followed by a plateau throughout the cloud best matches the observations. As a consequence, the 26Al -chronometer retains validity from the formation of canonical CAIs onward.
We present a new experimental setup called AROMA (The Aromatic Research of Organics with Molecular Analyzer) based on the use of laser mass spectrometry techniques. We demonstrate the potential of AROMA for the analysis of meteoritic samples and cosmic dust analogues. Tens of peaks are identified in the mass spectra with notable discrepancies across the different samples. These discrepancies provide clues on the chemical history of each sample and are not a bias of our analysis. A double bound-equivalent (DBE) method is applied to sort the detected carbonaceous molecules into families of compounds. It reveals in addition of polycyclic aromatic hydrocarbons, the presence of other populations such as mixed aromatic-aliphatic species and carbon clusters.
We present the results of an experimental study on the interaction of D atoms with Mg-rich amorphous silicates. The effects of D irradiation have been analyzed by infrared spectroscopy. The results indicate that HD forms by abstraction of hydrogen atoms chemisorbed in the hydroxyl groups of silicate grains. The formation process occurs for grain and atom temperatures relevant to photodissociation regions.
H2D+ and D2H+ are important chemical tracers of prestellar cores due to their pure rotational spectra that can be excited at the ~20 K temperature of these environments. The use of these molecules as probes of prestellar cores requires understanding the chemistry that forms and destroys these molecules. Of the eight key reactions that have been identified (Albertssonet al. 2013), five are thought to be well understood. The remaining three are the isotope exchange reactions of atomic D with H
$${ + \over 3}$$
, H2D+, and D2H+. Semi-classical results differ from the classical Langevin calculations by an order of magnitude (Moyano et al. 2004). To resolve this discrepancy, we have carried out laboratory measurements for these three reactions. Absolute cross sections were measured using a dual-source, merged fast-beams apparatus for relative collision energies between ~10 meV to ~10 eV (Hillenbrand et al. 2019). A semi-empirical model was developed incorporating high level quantum mechanical ab initio calculations for the zero-point-energy-corrected potential energy barrier in order to generate thermal rate coefficients for astrochemical models. Based on our studies, we find that these three reactions proceed too slowly at prestellar core temperatures to play a significant role in the deuteration of H
$${ + \over 3}$$
isotopologues.