Surface processes on cosmic solids in cold astrophysical environments lead to gas phase depletion and molecular complexity. Most astrophysical models assume that the molecular ice forms a thick multilayer substrate, not interacting with the dust surface. In contrast, we present experimental results demonstrating the importance of the surface for porous grains. We show that cosmic dust grains may be covered by a few monolayers of ice only. This implies that the role of dust surface structure, composition, and reactivity in models describing surface processes in cold interstellar, protostellar, and protoplanetary environments has to be reevaluated.
The physical evolution of Young Stellar Objects (YSOs) is accompanied by an enrichment of the molecular complexity, mainly triggered by the heating and energetic processing of the astrophysical ices. In this paper, a study of how the ice column density varies across the protostellar evolution has been performed. Tabulated data of H$_2$O, CO$_2$, CH$_3$OH, HCOOH observed by ground- and space-based telescopes toward 27 early-stage YSOs were taken from the literature. The observational data shows that ice column density and spectral index ($α$), used to classify the evolutionary stage, are well c…
Water ice has a strong spectral feature at a wavelength of approximately $3~μ$m, which plays a vital role in our understanding of the icy universe. In this study, we investigate the scattering polarization of this water-ice feature. The linear polarization degree of light scattered by $μ$m-sized icy grains is known to be enhanced at the ice band; however, the dependence of this polarization enhancement on various grain properties is unclear. We find that the enhanced polarization at the ice band is sensitive to the presence of $μ$m-sized grains as well as their ice abundance. We demonstrate th…
Ice mantles on dust grains play a central role in astrochemistry. Water and complex organic molecules (COMs) are thought to first form on the ice mantles and subsequently are released into the gas phase due to star formation activity. However, the critical question is whether ice mantles can survive stellar radiation when grains are being heated from $T_{d}\sim 10\rm K$ to $\gtrsim 100$ K. In this paper, we first study the effect of suprathermal grain rotation driven by the intense radiation of young stellar objects (YSOs) on the ice mantles. We find that the entire ice mantles can be disrupte…
Dust is an essential component of the interstellar medium (ISM) and plays an important role in many different astrophysical processes and phenomena. Traditionally, dust grains are known to be destroyed by thermal sublimation, Coulomb explosions, sputtering, and shattering. The first two mechanisms arise from the interaction of dust with intense radiation fields and high-energy photons (extreme UV), which work in a limited astrophysical environment. The present review is focused on a new destruction mechanism present in the {\it dust-radiation interaction} that is effective in a wide range of r…
In dense and cold regions of the interstellar medium (ISM), molecules may be adsorbed onto dust grains to form the ice mantles. Once formed, they can be processed by ionizing radiation coming from stellar or interstellar medium leading to formation of several new molecules in the ice. Among the different kind of ionizing radiation, cosmic rays play an important role in the solid-phase chemistry because of the large amount of energy deposited in the ices. The physicochemical changes induced by the energetic processing of astrophysical ices are recorded in a intrinsic parameter of the matter cal…
Widespread detection of amorphous and crystalline water (H${}_{2}$O) ice in the outer solar system bodies and the interstellar medium has been confirmed over the past decades. Radiative transfer models (RTMs) are used to estimate the grain sizes of H${}_{2}$O ice from near-infrared (NIR) wavelengths. Wide discrepancies in the estimation of H${}_{2}$O ice grain size on the Saturnian moons (Hansen, 2009), as well as nitrogen (N${}_{2}$) and methane (CH${}_{4}$) ices on Kuiper belt objects have been reported owing to different scattering models used (Emran and Chevrier, 2022). We assess the discr…
Interstellar dust grain growth in dense clouds and protoplanetary disks, even moderate, affects the observed interstellar ice profiles as soon as a significant fraction of dust grains is in the size range close to the wave vector at the considered wavelength. The continuum baseline correction made prior to analysing ice profiles influences the subsequent analysis and hence the estimated ice composition, typically obtained by band fitting using thin film ice mixture spectra. We model the effect of grain growth on ice mantle spectroscopic profiles, focusing on CO2 to see how it can affect inters…
Computational models of interstellar gas-grain chemistry have historically adopted a single dust-grain size of 0.1 micron, assumed to be representative of the size distribution present in the interstellar medium. Here, we investigate the effects of a broad grain-size distribution on the chemistry on dust-grain surfaces and the subsequent build-up of molecular ices on the grains, using a three-phase gas-grain chemical model of a quiescent dark cloud. We include an explicit treatment of the grain temperatures, governed both by the visual extinction of the cloud and the size of each individual gr…
We present an argument that radio galaxies (active galaxies with mis-aligned jets) are likely to be the primary sources of the high-energy astrophysical neutrinos observed by IceCube. In particular, if the gamma-ray emission observed from radio galaxies is generated through the interactions of cosmic-ray protons with gas, these interactions can also produce a population of neutrinos with a flux and spectral shape similar to that measured by IceCube. We present a simple physical model in which high-energy cosmic rays are confined within the volumes of radio galaxies, where they interact with ga…
Comets provide unique information about the physical and chemical properties of the environment in which the Solar system was formed. Understanding how cometary dust and ice evolve under the effect of sunlight is essential for constraining nuclear structure and triggering mechanism of comet activity. In this paper, we first study rotational disruption of dust grains lifted by outgassing from comet nuclei by radiative torques (RATs). We find that composite grains could be rapidly disrupted into small fragments by the Radiative Torque Disruption (RATD) mechanism. We then study rotational desorpt…
Understanding the history and evolution of small bodies, such as dust grains and comets, in planet-forming disks is very important to reveal the architectural laws responsible for the creation of planetary systems. These small bodies in cold regions of the disks are typically considered as mixtures of dust particles with molecular ices, where ices cover the surface of a dust core or are actually physically mixed with dust. Whilst the first case, ice-on-dust, has been intensively studied in the laboratory in recent decades, the second case, ice-mixed-with-dust, present uncharted territory. This…
We present a new gas-grain chemical model to constrain the effect of grain size distribution on molecular abundances in starless and pre-stellar cores. We introduce grain-size dependence simultaneously for cosmic-ray (CR)-induced desorption efficiency and for grain equilibrium temperatures. We keep explicit track of ice abundances on a set of grain populations. We find that the size-dependent CR desorption efficiency affects ice abundances in a highly non-trivial way that depends on the molecule. Species that originate in the gas phase follow a simple pattern where the ice abundance is highest…
Cosmic-ray-induced sputtering is one of the important desorption mechanisms at work in astrophysical environments. The chemical evolution observed in high-density regions, from dense clouds to protoplanetary disks, and the release of species condensed on dust grains, is one key parameter to be taken into account in interpretations of both observations and models. This study is part of an ongoing systematic experimental determination of the parameters to consider in astrophysical cosmic ray sputtering. As was already done for water ice, we investigated the sputtering yield as a function of ice …
The Ice Chamber for Astrophysics-Astrochemistry (ICA) is a new laboratory end-station located at the Institute for Nuclear Research (Atomki) in Debrecen, Hungary. The ICA has been specifically designed for the study of the physico-chemical properties of astrophysical ice analogues and their chemical evolution when subjected to ionising radiation and thermal processing. The ICA is an ultra-high vacuum compatible chamber containing a series of IR-transparent substrates mounted in a copper holder connected to a closed-cycle cryostat capable of being cooled down to 20 K, itself mounted on a 360° r…
The degree of porosity in interstellar dust-grain material is poorly defined, although recent work has suggested that the grains could be highly porous. Aside from influencing the optical properties of the dust, porosity has the potential to affect the chemistry occurring on dust-grain surfaces, via increased surface area, enhanced local binding energies, and the possibility of trapping of molecules within the pores as ice mantles build up on the grains. Through computational kinetics simulations, we investigate how interstellar grain-surface chemistry and ice composition are affected by the p…
We study the effects of grain surface reactions on the chemistry of protoplanetary disks where gas, ice surface layers and icy mantles of dust grains are considered as three distinct phases. Gas phase and grain surface chemistry is found to be mainly driven by photo-reactions and dust temperature gradients. The icy disk interior has three distinct chemical regions: (i) the inner midplane with low FUV fluxes and warm dust ($\gtrsim 15$K) that lead to the formation of complex organic molecules, (ii) the outer midplane with higher FUV from the ISM and cold dust where hydrogenation reactions domin…
A new experimental set-up INterStellar Ice-Dust Experiment (INSIDE), was designed for studying cosmic grain analogues represented by ice-coated carbon- and silicate-based dust grains. In the new instrument, we can simulate physical and chemical conditions prevailing in interstellar and circumstellar environments. The set-up combines ultrahigh vacuum and low temperature conditions with infrared spectroscopy and mass spectrometry. Using INSIDE, we plan to investigate physical and chemical processes, such as adsorption, desorption, and formation of molecules, on the surface of dust/ice samples. F…
Grain surfaces play a central role in the formation and desorption of molecules in space. To form molecules on a grain surface, adsorbed species trapped in binding sites must be mobile and migrate to adjacent sites. Thermal hopping is a popular mechanism for the migration of adsorbed species when the grain surface is warmed up by stellar radiation. However, previous studies disregarded the fact that grains can be spun-up to suprathermal rotation by radiative torques (RATs) during grain heating process. To achieve an accurate model of surface astrochemistry, in this paper, we study the effect o…
Broadband spectroscopy of astrophysical ice analogues: IV. Optical constants of N$_2$ ice in the terahertz and mid-infrared ranges
Leiden University（莱顿大学）；Max-Planck-Institut für Extraterrestrische Physik（马克斯·普朗克地外物理研究所）；Aix Marseille Univ, CNRS, CNES, LAM（艾克斯-马赛大学）；Prokhorov General Physics Institute of the Russian Academy of Sciences（俄罗斯科学院普罗霍洛夫普通物理研究所）；Federal Institute of Education, Science and Technology of Rio de Janeiro (IFRJ)（里约热内卢联邦教育、科学与技术学院）；University of Stuttgart（斯图加特大学）；University of Perugia（佩鲁贾大学）
Laboratory studies of the radiation chemistry occurring in astrophysical ices have demonstrated the dependence of this chemistry on a number of experimental parameters. One experimental parameter which has received significantly less attention is that of the phase of the solid ice under investigation. In this present study, we have performed systematic 2 keV electron irradiations of the amorphous and crystalline phases of pure CH3OH and N2O astrophysical ice analogues. Radiation-induced decay of these ices and the concomitant formation of products were monitored in situ using FT-IR spectroscop…
Interstellar ices are layers of molecules deposited on !ne dust grains in dark and dense molecular cloud cores. Subsurface ice has been considered in a few astrochemical models, which have shown that it can be of great importance. The aim of this work is to introduce an established subsurface ice description into the state-of-the-art astrochemical model ALCHEMIC. The model has been developed by the Heidelberg astrochemistry group. The result is an up-to-date model for interstellar molecular cloud research with possible application for protoplanetary disks.
Abundances and partitioning of ices and gases produced by gas-grain chemistry are governed by adsorption and desorption on grains. Understanding astrophysical observations rely on laboratory measurements of adsorption and desorption rates on dust grains analogs. On flat surfaces, gas adsorption probabilities (or sticking coefficients) have been found close to unity for most gases. Here we report a strong decrease of the sticking coefficients of H2O and CO2 on substrates more akin to cosmic dust, such as submicrometer-sized particles of carbon and olivine, bare or covered with ice. This effect …
Whether ice in cold cosmic environments is physically separated from the silicate dust or mixed with individual silicate moieties is not known. However, different grain models give very different compositions and temperatures of grains. The aim of the present study is a comparison of the mid-IR spectra of laboratory silicate-grains/water-ice mixtures with astronomical observations to evaluate the presence of dust/ice mixtures in interstellar and circumstellar environments. The laboratory data can explain the observations assuming reasonable mass-averaged temperatures for the protostellar envel…
The first off-lattice Monte Carlo kinetics model of interstellar dust-grain surface chemistry is presented. The positions of all surface particles are determined explicitly, according to the local potential minima resulting from the pair-wise interactions of contiguous atoms and molecules, rather than by a pre-defined lattice structure. The model is capable of simulating chemical kinetics on any arbitrary dust-grain morphology, as determined by the user-defined positions of each individual dust-grain atom. A simple method is devised for the determination of the most likely diffusion pathways a…
In cold core of dark molecular clouds, where the UV radiation from external sources is strongly attenuated, cosmic rays can induce chemical reactions on the surface of ice-covered grains promoting the ejection of the processed material to the gas phase. We report the positive and negative secondary ion emission from pure CH3CN, C2H3CN and i-C3H7CN ices due to the bombardment of heavy ions (252Cf fission fragments), simulating the incidence of cosmic rays onto icy surfaces. The secondary ions emitted from each sample were analysed by time-of-flight mass spectrometry (TOF-MS), using Plasma Desor…
Cosmic rays are ubiquitous in interstellar environments, and their bombardment of dust-grain ice mantles is a possible driver for the formation of complex, even prebiotic molecules. Yet, critical data that are essential for accurate modeling of this phenomenon, such as the average radii of cosmic-ray tracks in amorphous solid water (ASW) remain unconstrained. It is shown that cosmic ray tracks in ASW can be approximated as a cylindrical volume with an average radius that is mostly independent of the initial particle energy. Interactions between energetic ions and both a low-density amorphous (…
The astrochemistry of CO2 ice analogues has been a topic of intensive investigation due to the prevalence of CO2 throughout the interstellar medium and the Solar System, as well as the possibility of it acting as a carbon feedstock for the synthesis of larger, more complex organic molecules. In order to accurately discern the physico-chemical processes in which CO2 plays a role, it is necessary to have laboratory-generated spectra to compare against observational data acquired by ground- and space-based telescopes. A key factor which is known to influence the appearance of such spectra is temp…
A new, more comprehensive model of gas-grain chemistry in hot molecular cores is presented, in which nondiffusive reaction processes on dust-grain surfaces and in ice mantles are implemented alongside traditional diffusive surface/bulk-ice chemistry. We build on our nondiffusive treatments used for chemistry in cold sources, adopting a standard collapse/warm-up physical model for hot cores. A number of other new chemical model inputs and treatments are also explored in depth, culminating in a final model that demonstrates excellent agreement with gas-phase observational abundances for many mol…
The properties of dust change during the transition from diffuse to dense clouds as a result of ice formation and dust coagulation, but much is still unclear about this transformation. We present 2-20 micron spectra of 49 field stars behind the Perseus and Serpens Molecular Clouds and establish relationships between the near-infrared continuum extinction (AK) and the depths of the 9.7 micron silicate (tau97) and 3.0 micron H2O ice (tau30) absorption bands. The tau97/AK ratio varies from large, diffuse interstellar medium-like values (~0.55), to much lower ratios (~0.26). Above extinctions of A…
Context: Observations of scattered light in the 1-5 $μ$m range have revealed dust grains in molecular cores with sizes larger than commonly inferred for the diffuse interstellar medium. It is currently unclear whether these grains are grown within the molecular cores or are an ubiquitous component of the interstellar medium. Aims: We investigate whether the large grains necessary for efficient scattering at 1-5 mum are associated with the abundance of water-ice within molecular clouds and cores. Methods: We combined water-ice abundance measurements for sight lines through the Lupus IV molecula…
Cosmic rays are able to heat interstellar dust grains. This may enhance molecule mobility in icy mantles that have accumulated on the grains in dark cloud cores. A three-phase astrochemical model was used to investigate the molecule mobility in interstellar ices. Specifically, diffusion through pores in ice between the subsurface mantle and outer surface, assisted by whole-grain heating, was considered. It was found that the pores can serve as an efficient transport route for light species. The diffusion of chemical radicals from the mantle to the outer surface are most effective. These specie…
We compute the desorption rate of icy mantles on dust grains as a function of the size and composition of both the grain and the mantle. We combine existing models of cosmic ray (CR) related desorption phenomena with a model of CR transport to accurately calculate the desorption rates in dark regions of molecular clouds. We show that different desorption mechanisms dominate for grains of different sizes, and in different regions of the cloud. We then use these calculations to investigate a simple model of the growth of mantles, given a distribution of grain sizes. We find that modest variation…
The observed gas-phase molecular inventory of hot cores is believed to be significantly impacted by the products of chemistry in interstellar ices. In this study, we report the construction of a full macroscopic Monte Carlo model of both the gas-phase chemistry and the chemistry occurring in the icy mantles of interstellar grains. Our model treats icy grain mantles in a layer-by-layer manner, which incorporates laboratory data on ice desorption correctly. The ice treatment includes a distinction between a reactive ice surface and an inert bulk. The treatment also distinguishes between zeroth a…
Two different silicate/water ice mixtures representing laboratory analogues of interstellar and circumstellar icy grains were produced in the laboratory. For the first time, optical constants, the real and imaginary parts of the complex refractive index, of such silicate/water ice mixtures were experimentally determined in the mid-infrared spectral region at low temperatures. In addition, optical constants of pure water ice and pure silicates were derived in the laboratory. Two sets of constants were compared, namely, measured constants calculated from the transmission spectra of silicate/wate…
Massive young stellar objects in the Magellanic Clouds show infrared absorption features corresponding to significant abundances of CO, CO$_2$ and H$_2$O ice along the line of sight, with the relative abundances of these ices differing between the Magellanic Clouds and the Milky Way. CO ice is not detected towards sources in the Small Magellanic Cloud, and upper limits put its relative abundance well below sources in the Large Magellanic Cloud and the Milky Way. We use our gas-grain chemical code MAGICKAL, with multiple grain sizes and grain temperatures, and further expand it with a treatment…
The catalytic role of dust grain surfaces in the thermal reaction CO2 + 2NH3 $\rightarrow$ NH4+NH2COO was recently demonstrated by our group. The rate coefficients for the reaction at 80 K on the surface of nanometre-sized carbon and silicate grains were measured to be up to three times higher compared to the reaction rate coefficients measured on KBr. In this study, the reaction was performed on carbon grains and on KBr in the extended temperature range of 50 - 80 K and with the addition of water ice. The reaction activation energy was found to be about 3 times lower on grains compared to the…
Infrared photometry and spectroscopy (1-25 um) of background stars reddened by the Lupus molecular cloud complex are used to determine the properties of the grains and the composition of the ices before they are incorporated into circumstellar envelopes and disks. H2O ices form at extinctions of Ak=0.25+/-0.07 mag (Av=2.1+/-0.6). Such a low ice formation threshold is consistent with the absence of nearby hot stars. Overall, the Lupus clouds are in an early chemical phase. The abundance of H2O ice (2.3+/-0.1*10^-5 relative to Nh) is typical for quiescent regions, but lower by a factor of 3-4 co…
UV ice photodesorption is an important non-thermal desorption pathway in many interstellar environments that has been invoked to explain observations of cold molecules in disks, clouds and cloud cores. Systematic laboratory studies of the photodesorption rates, between 7 and 14 eV, from CO:N2 binary ices, have been performed at the DESIRS vacuum UV beamline of the synchrotron facility SOLEIL. The photodesorption spectral analysis demonstrates that the photodesorption process is indirect, i.e. the desorption is induced by a photon absorption in sub-surface molecular layers, while only surface m…
Context. Cosmic ray particles that hit interstellar grains in dark molecular cores may induce whole-grain heating. The high temperature of a CR-heated grain allows energy barriers for bulk diffusion and reactions to be overcome. Additionally, ice molecules are destroyed by direct cosmic-ray induced dissociation. Aims. We provide a justified estimate of the significance of cosmic-ray induced surface-mantle diffusion, chemical reactions in ice, and dissociation of ice species in a star-forming interstellar cloud core. Methods. We considered a gas clump in a collapsing low-mass prestellar core an…
