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Creators/Authors contains: "Garrod, Robin T"

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  1. Abstract Despite the organic molecule inventory detected in the Orion Kleinmann–Low Nebula (Orion KL), acetaldehyde (CH3CHO)—one of the most ubiquitous interstellar aldehydes—has not been firmly identified with millimeter-wave interferometry. We analyze extensive Atacama Large Millimeter/submillimeter Array archival data sets (142–355 GHz) to search for acetaldehyde, revealing two distinct acetaldehyde emission peaks and one component with more complex kinematic structures. One peak aligns with MF10/IRc2, where emissions of other O-bearing complex organic molecules are rarely reported, while the other is coincident with the ethanol peak in the southwest region of the hot core. The MF10/IRc2 detection suggests unique chemistry, possibly influenced by repeated heating events. In contrast, codetection with ethanol indicates an ice origin and suggests a potential chemical relationship between the two species. We determine acetaldehyde column densities and kinetic temperatures toward these two peaks under local thermodynamic equilibrium assumptions and compare its distribution with ethanol and other molecules that have an aldehyde (HCO) group, such as methyl formate, glycolaldehyde, and formic acid. Toward the ethanol peak, the observed abundance ratios between HCO-containing species are analyzed using a chemical model. The model suggests two key points: (1) the destruction of ethanol to form acetaldehyde in the ice may contribute to the observed correlation between the two species; and (2) a long cold-collapse timescale and a methyl formate binding energy similar to or lower than water are needed to explain the observations. The relative abundance ratios obtained from the model are highly sensitive to the assumed kinetic temperature, which accounts for the high spatial variability of the aldehyde ratios observed toward Orion KL. 
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    Free, publicly-accessible full text available July 1, 2026
  2. Abstract Phosphorus is a key element that plays an essential role in biological processes important for living organisms on Earth. The origin and connection of phosphorus-bearing molecules to early solar system objects and star-forming molecular clouds is therefore of great interest, yet there are limited observations throughout different stages of low-mass (M < a few solar masses) star formation. Observations from the Yebes 40 m and IRAM 30 m telescopes detect for the first time in the 7 mm, 3 mm, and 2 mm bands multiple transitions of PN and PO, as well as a single transition of PO+, toward a low-mass starless core. The presence of PN, PO, and PO+is kinematically correlated with bright SiO(1–0) emission. Our results reveal not only that shocks are the main driver of releasing phosphorus from dust grains and into the gas phase but that the emission originates from gas not affiliated with the shock itself but quiescent gas that has been shocked in the recent past. From radiative transfer calculations, the PO/PN abundance ratio is found to be 3 . 1 0.6 + 0.4 , consistent with other high-mass and low-mass star-forming regions. This first detection of PO+toward any low-mass star-forming region reveals a PO+/PO ratio of 0.011 5 0.0009 + 0.0008 , a factor of 10 lower than previously determined from observations of a Galactic center molecular cloud, suggesting its formation can occur under more standard Galactic cosmic-ray ionization rates. These results motivate the need for additional observations that can better disentangle the physical mechanisms and chemical drivers of this precursor of prebiotic chemistry. 
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    Free, publicly-accessible full text available May 21, 2026
  3. Context. The solid-state reaction C + H2O → H2CO has recently been studied experimentally and claimed as a new ‘non-energetic’ pathway to complex organic and prebiotic molecules in cold astrophysical environments. Aims. We compared results of astrochemical network modelling with and without the C + H2O surface reaction. Methods. A typical, generic collapse model in which a dense core forms from initially diffuse conditions was used along with the astrochemical kinetics model MAGICKAL. Results. The inclusion of the reaction does not notably enhance the abundance of formaldehyde itself; however, it significantly enhances the abundance of methanol (formed by the hydrogenation of formaldehyde) on the dust grains at early times, when the high gas-phase abundance of atomic C leads to relatively rapid adsorption onto the grain surfaces. As a result, the gas-phase abundance of methanol is also increased due to chemical desorption, quickly reaching abundances close to ∼10−9nH, which decline strongly under late-time, high-density conditions. The reaction also influences the abundances of simple ice species, with the CO2abundance increased in the earliest, deepest ice layers, while the water-ice abundance is somewhat depressed. The abundances of various complex organic molecules are also affected, with some species becoming more abundant and others less. When gas-phase atomic carbon becomes depleted, the grain-surface chemistry returns to behaviour that would be expected if there had been no new reaction. Conclusions. Our results show that fundamental reactions involving the simplest atomic and molecular species can be of great importance for the evolution of astrochemical reaction networks, thus providing motivation for future experimental and theoretical studies. 
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    Free, publicly-accessible full text available December 1, 2025
  4. Context.Recent JWST observations have measured the ice chemical composition towards two highly extinguished background stars, NIR38 and J110621, in the Chamaeleon I molecular cloud. The observed excess of extinction on the long-wavelength side of the H2O ice band at 3 μm has been attributed to a mixture of CH3OH with ammonia hydrates NH3·H2O), which suggests that CH3OH ice in this cloud could have formed in a water-rich environment with little CO depletion. Laboratory experiments and quantum chemical calculations suggest that CH3OH could form via the grain surface reactions CH3+ OH and/or C + H2O in water-rich ices. However, no dedicated chemical modelling has been carried out thus far to test their efficiency. In addition, it remains unexplored how the efficiencies of the proposed mechanisms depend on the astrochemical code employed. Aims.We modelled the ice chemistry in the Chamaeleon I cloud to establish the dominant formation processes of CH3OH, CO, CO2, and of the hydrides CH4and NH3(in addition to H2O). By using a set of state-of-the-art astrochemical codes (MAGICKAL, MONACO, Nautilus, UCLCHEM, and KMC simulations), we can test the effects of the different code architectures (rate equation vs. stochastic codes) and of the assumed ice chemistry (diffusive vs. non-diffusive). Methods.We consider a grid of models with different gas densities, dust temperatures, visual extinctions, and cloud-collapse length scales. In addition to the successive hydrogenation of CO, the codes’ chemical networks have been augmented to include the alternative processes for CH3OH ice formation in water-rich environments (i.e. the reactions CH3+ OH → CH3OH and C + H2O → H2CO). Results.Our models show that the JWST ice observations are better reproduced for gas densities ≥105cm−3and collapse timescales ≥105yr. CH3OH ice formation occurs predominantly (>99%) via CO hydrogenation. The contribution of reactions CH3+ OH and C + H2O is negligible. The CO2ice may form either via CO + OH or CO + O depending on the code. However, KMC simulations reveal that both mechanisms are efficient despite the low rate of the CO + O surface reaction. CH4is largely underproduced for all codes except for UCLCHEM, for which a higher amount of atomic C is available during the translucent cloud phase of the models. Large differences in the predicted abundances are found at very low dust temperatures (Tdust<12 K) between diffusive and non-diffusive chemistry codes. This is due to the fact that non-diffusive chemistry takes over diffusive chemistry at such low Tdust. This could explain the rather constant ice chemical composition found in Chamaeleon I and other dense cores despite the different visual extinctions probed. 
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    Free, publicly-accessible full text available March 1, 2026
  5. The observation and synthesis of organic molecules in interstellar space is one of the most exciting and rapidly growing topics in astrochemistry. Spectroscopic observations especially with millimeter and submillimeter waves have resulted in the detection of more than 250 molecules in the interstellar clouds from which stars and planets are ultimately formed. In this review, we focus on the diverse suggestions made to explain the formation of Complex Organic Molecules (COMs) in the low-temperature interstellar medium. The dominant mechanisms at such low temperatures are still a matter of dispute, with both gas-phase and granular processes, occurring on and in ice mantles, thought to play a role. Granular mechanisms include both diffusive and nondiffusive processes. A granular explanation is strengthened by experiments at 10 K that indicate that the synthesis of large molecules on granular ice mantles under space-like conditions is exceedingly efficient, with and without external radiation. In addition, the bombardment of carbon-containing ice mantles in the laboratory by cosmic rays, which are mainly high-energy protons, can lead to organic species even at low temperatures. For processes on dust grains to be competitive at low temperatures, however, non-thermal desorption mechanisms must be invoked to explain why the organic molecules are detected in the gas phase. Although much remains to be learned, a better understanding of low-temperature organic syntheses in space will add both to our understanding of unusual chemical processes and the role of molecules in stellar evolution. 
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  6. Abstract Chemical models and experiments indicate that interstellar dust grains and their ice mantles play an important role in the production of complex organic molecules (COMs). To date, the most complex solid-phase molecule detected with certainty in the interstellar medium is methanol, but the James Webb Space Telescope (JWST) may be able to identify still larger organic species. In this study, we use a coupled chemodynamical model to predict new candidate species for JWST detection toward the young star-forming core Cha-MMS1, combining the gas–grain chemical kinetic code MAGICKAL with a 1D radiative hydrodynamics simulation using Athena++ . With this model, the relative abundances of the main ice constituents with respect to water toward the core center match well with typical observational values, providing a firm basis to explore the ice chemistry. Six oxygen-bearing COMs (ethanol, dimethyl ether, acetaldehyde, methyl formate, methoxy methanol, and acetic acid), as well as formic acid, show abundances as high as, or exceeding, 0.01% with respect to water ice. Based on the modeled ice composition, the infrared spectrum is synthesized to diagnose the detectability of the new ice species. The contribution of COMs to IR absorption bands is minor compared to the main ice constituents, and the identification of COM ice toward the core center of Cha-MMS1 with the JWST NIRCAM/Wide Field Slitless Spectroscopy (2.4–5.0 μ m) may be unlikely. However, MIRI observations (5–28 μ m) toward COM-rich environments where solid-phase COM abundances exceed 1% with respect to the column density of water ice might reveal the distinctive ice features of COMs. 
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