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Gabriela Silva-Vera

Publications and source records attributed to Gabriela Silva-Vera.

3 recordsLinked to original sources

Theoretical determination of the binding energies of methanol and related species onto amorphous solid water ice

The formation and survival of complex organic molecules (COMs) in cold interstellar environments depends on their interactions with icy dust grain surfaces. Methanol, a key COM detected in cold cores and protoplanetary disks, is believed to form on amorphous solid water (ASW) through surface reactions and reside there until it is desorbed into the gas phase. We present a theoretical study of the binding energies (BEs) of methanol and its photolysis-derived species on ASW clusters by means of dispersion-corrected density functional theory (DFT) using a refined protocol implemented in the Binding Energy Evaluation Platform (BEEP). Molecules capable of hydrogen bonding, such as H2O, CH3OH, HCOOH, and OH, exhibit high BEs and broad BE distributions that reflect the structural heterogeneity of the ASW surface. In contrast, weakly interacting volatiles including CO, CO2, CH4, and CH3 display narrower distributions dominated by dispersion interactions. Open-shell radicals such as CH2OH and OH bind more strongly than HCO and CH3 due to their ability to form directional hydrogen bonds. Incorporation of our BEs into an astrochemical model, in conjunction with a recalculation of the pre-exponential factor using transition state theory, demonstrates the sensitivity of model results to the method of calculation of the grain-surface reaction rates. The new approach generally predicts a higher abundance of radicals on the ice that are key reactants for the formation of COMs when surface diffusion is assumed to be efficient. These findings emphasize the importance of incorporating BEs that have been determined in a self-consistent manner into astrochemical models, and provide reliable theoretical benchmarks for species with limited experimental data.

astro-ph.GA↗

Pathways to Interstellar Amides via Carbamoyl (NH2CO) Isomers by Radical-Neutral Reactions on Ice Grain Mantles

Explaining the formation pathways of amides on ice-grain mantels is crucial to understanding the prebiotic chemistry in an interstellar medium. In this computational study, we explore different radical-neutral formation pathways for some of the observed amides (formamide, acetamide, urea, and N-methylformamide) via intermediate carbamoyl (NH2CO) radical precursors and their isomers. We assess the relative energy of four NH2CO isomers in the gas phase and evaluate their binding energy on small water clusters to discern the affinity that the isomers present to an ice model. We consider three possible reaction pathways for the formation of the carbamoyl radicals, namely, the OH + HCN, CN + H2O, and NH2 + CO reaction channels. We computed the binding energy distribution for the HCN and CH3CN precursors on an ice model consisting of a set of clusters of 22 water molecules each to serve as a starting point for the reactivity study on the ice surface. The computations revealed that the lowest barrier to the formation of an NH2CO isomer corresponds to the NH2 + CO reaction (12.6 kJ/mol). The OH + HCN reaction pathway results in the exothermic formation of the N-radical form of carbamoyl HN(C=O)H with a reaction barrier of 26.7 kJ/mol. We found that the CN + H2O reaction displays a high energy barrier of 70.6 kJ/mol. Finally, we also probed the direct formation of the acetamide radical precursor via the OH + CH3CN reaction and found that the most probable outcome on interstellar ices is the H-abstraction reaction to yield CH2CN and H2O. Based on these results, we believe that including alternative reaction pathways, leading to the formation of amides via the N-radical form of carbamoyl, would provide an improvement in the prediction of the amide abundances in astrochemical models, especially regarding the chemistry of star-forming regions.

astro-ph.GA↗

In-Depth Exploration of Catalytic Sites on Amorphous Solid Water: I. The Astrosynthesis of Aminomethanol

Chemical processes taking place on ice-grain mantles are pivotal to the complex chemistry of interstellar environments. In this study, we conducted a comprehensive analysis of the catalytic effects of an amorphous solid water (ASW) surface on the reaction between ammonia (NH$_3$) and formaldehyde (H$_2$CO) to form aminomethanol (NH$_2$CH$_2$OH) using density functional theory. We identified potential catalytic sites based on the binding energy distribution of NH$_3$ and H$_2$CO reactants, on a set-of-clusters surface model composed of 22 water molecules and found a total of 14 reaction paths. Our results indicate that the catalytic sites can be categorized into four groups, depending on the interactions of the carbonyl oxygen and the amino group with the ice surface in the reactant complex. A detailed analysis of the reaction mechanism using Intrinsic Reaction Coordinate and reaction force analysis revealed three distinct chemical events for this reaction: formation of the C--N bond, breaking of the N--H bond, and formation of the O--H hydroxyl bond. Depending on the type of catalytic site, these events can occur within a single, concerted, albeit asynchronous, step, or can be isolated in a step-wise mechanism, with the lowest overall transition state energy observed at 1.3 kcal mol$^{-1}$. A key requirement for the low-energy mechanism is the presence of a pair of dangling OH bonds on the surface, found at 5\% of the potential catalytic sites on an ASW porous surface.

astro-ph.GA↗