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Register a new userNeural-Network Assisted Study of Nitrogen Atom Dynamics on Amorphous Solid Water. I. Adsorption & Desorption
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Dynamics of adsorption and desorption of (4S)-N on amorphous solid water are analyzed using molecular dynamics simulations. The underlying potential energy surface was provided by machine-learned interatomic potentials. Binding energies confirm the latest available theoretical and experimental results. The nitrogen sticking coefficient is close to unity at dust temperatures of 10 K but decreases at higher temperatures. We estimate a desorption time scale of 1 {mu}s at 28 K. The estimated time scale allows chemical processes mediated by diffusion to happen before desorption, even at higher temperatures. We found that the energy dissipation process after a sticking event happens on the picosecond timescale at dust temperatures of 10 K, even for high energies of the incoming adsorbate. Our approach allows the simulation of large systems for reasonable time scales at an affordable computational cost and ab-initio accuracy. Moreover, it is generally applicable for the study of adsorption dynamics of interstellar radicals on dust surfaces.
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We investigated the behavior of H$_2$, main constituent of the gas phase in dense clouds, after collision with amorphous solid water (ASW) surfaces, one of the most abundant chemical species of interstellar ices. We developed a general framework to study the adsorption dynamics of light species on interstellar ices. We provide binding energies and their distribution, sticking probabilities for incident energies between 1 meV and 60 meV, and thermal sticking coefficients between 10 and 300 K for surface temperatures from 10 to 110 K. We found that the sticking probability depends strongly on the adsorbate kinetic energy and the surface temperature, but hardly on the angle of incidence. We observed finite sticking probabilities above the thermal desorption temperature. Adsorption and thermal desorption should be considered as separate events with separate time scales. Laboratory results for these species have shown a gap in the trends attributed to the differently employed experimental techniques. Our results complement observations and extend them, increasing the range of gas temperatures under consideration. We plan to employ our method to study a variety of adsorbates, including radical and charged species.
Core-excitation of water ice releases many different molecules and ions in the gas phase. Studying these desorbed species and the underlying mechanisms can provide useful information on the effects of X-ray irradiation in ice. We report a detailed study of the X-ray induced desorption of a number of neutral, cationic and anionic species from amorphous solid water. We discuss the desorption mechanisms, and the relative contributions of Auger and secondary electrons (X-ray induced Electron Stimulated Desorption) and initial excitation (rev{direct desorption}) as well as the role of photochemistry. Anions are shown to desorb not just through processes linked with secondary electrons but also through direct dissociation of the core-excited molecule. The desorption spectra of oxygen ions (O$^+$, OH$^+$, H$_2$O$^+$, O$^-$, OH$^-$) give a new perspective on their previously reported very low desorption yields for most types of irradiation of water, showing that they mostly originate from the dissociation of photoproducts such as H$_2$O$_2$.
Carbonyl sulfide (OCS) is an abundant sulfur (S)-bearing species in the interstellar medium. It is present not only in the gas phase, but also on interstellar grains as as solid; therefore, OCS very likely undergoes physico-chemical processes on icy surfaces at very low temperatures. The present study experimentally and computationally investigates the reaction of solid OCS with hydrogen (H) atoms on amorphous solid water at low temperatures. The results show that H addition to OCS proceeds via quantum tunneling, and further H addition leads to the formation of carbon monoxide (CO), hydrogen sulfide (H2S), formaldehyde (H2CO), methanol (CH3OH) and thioformic acid (HC(O)SH). These experimental results are explained by our quantum chemical calculations, which demonstrate that the initial H addition to the S atom of OCS is the most predominant, leading to the formation of OCS-H radicals. Once the formed OCS-H radical is stabilized on ices, further H addtion to the S atom yields CO and H2S, while that to the C atom yields HC(O)SH. We have also confirmed, in a separate experiment, the HCOSH formation by the HCO reactions with the SH radicals. The present results would have an important implication for the recent detection of HC(O)SH toward H+0.693-0.027.
In this paper, we investigate the adsorption of water monomer on fluorinated graphene using state-of-the-art first principles methods within the framework of density functional theory (DFT). Four different methods are employed to describe the interactions between water and the carbon surface: The traditional DFT calculations within the generalized gradient approximation (GGA), and three types of calculations using respectively the semi-empirical DFT-D2method, the original van der Waals density functional (vdW-DF) method, and one of its variants. Compared with the adsorption on pristine graphene, the adsorption energies of water on fluorinated graphene are significantly increased, and the orientations of water diploe moment are notably changed. The most stable configuration is found to stay right above the top site of the C atom which is bonded with F, and the dipole moment of water molecule aligns spontaneously along the surface normal.
Two approximations used by Sengupta [Phys. Rev. B {bf 100}, 075429 (2019)] in numerically computing the adsorption rate of cold hydrogen atoms on suspended graphene are critically examined. The independent boson model approximation (IBMA) was used to compute the atom self-energy, and the single-pole approximation (SPA) was used to obtain the adsorption rate from the self-energy. It is shown explicitly that there are additional contributions to the self-energy appearing at the same order of the atom-phonon coupling as the IBMA terms that alter the value of the real part of the self-energy at low energies by several orders of magnitude in the regime of interest. This shift in the self-energy consequently renders the use of SPA invalid.
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