Reaction dynamics on amorphous solid water surfaces using interatomic machine learned potentials. Microscopic energy partition revealed from the P + H -> PH reaction

Abstract

Energy redistribution after a chemical reaction is one of the few mechanisms to explain the diffusion and desorption of molecules which require more energy than the thermal energy available in quiescent molecular clouds (10 K). This energy distribution can be important in phosphorous hydrides, elusive yet fundamental molecules for interstellar prebiotic chemistry. We studied the reaction dynamics of the \ce{P + H -> PH} reaction on amorphous solid water, a reaction of astrophysical interest, using \emph{ab-initio} molecular dynamics with atomic forces evaluated by a neural network interatomic potential. We found that the exact nature of the initial phosphorous binding sites is less relevant for the energy dissipation process because the nascent PH molecule rapidly migrates to sites with higher binding energy after the reaction. Non-thermal diffusion and desorption-after-reaction were observed and occurred early in the dynamics, essentially decoupled from the dissipation of the chemical reaction energy. From an extensive sampling of reactions on sites, we constrained the average dissipated reaction energy within the simulation time (50 ps) to be between 50 and 70 %. Most importantly, the fraction of translational energy acquired by the formed molecule was found to be mostly between 1 and 5 %. Including these values, specifically for the test cases of 2% and 5% of translational energy conversion, in astrochemical models, reveals very low gas-phase abundances of PH${}_x$ molecules and reflects that considering binding energy distributions is paramount for correctly merging microscopic and macroscopic modelling of non-thermal surface astrochemical processes. Finally, we found that PD molecules dissipate more of the reaction energy. This effect can be relevant for the deuterium fractionation and preferential distillation of molecules in the interstellar medium.

arXiv commentAccepted for publication in Astronomy and Astrophysics

References in corpus (28)

• A KInetic Database for Astrochemistry (KIDA)
• Non-thermal desorption from interstellar dust grains via exothermic surface reactions
• A three-phase chemical model of hot cores: the formation of glycine
• Gas and grain chemical composition in cold cores as predicted by the Nautilus 3-phase model
• Dust as interstellar catalyst I. Quantifying the chemical desorption process
• Binding energies of interstellar molecules on crystalline and amorphous models of water ice by ab-initio calculations
• Confirmation of circumstellar phosphine
• Gas-grain chemistry in cold interstellar cloud cores with a microscopic Monte Carlo approach to surface chemistry
• ALMA and ROSINA detections of phosphorus-bearing molecules: the interstellar thread between star-forming regions and comets
• Gaussian Moments as Physically Inspired Molecular Descriptors for Accurate and Scalable Machine Learning Potentials
• Phosphorus-bearing molecules in solar-type star forming regions: First PO detection
• First detections of the key prebiotic molecule PO in star-forming regions
• Benzonitrile as a proxy for benzene in the cold ISM: low temperature rate coefficients for CN + C${}_6$H${}_6$
• Phosphorus-bearing molecules in the Galactic Center
• An Approach to Estimate the Binding energy of Interstellar Species
• Chemical desorption versus energy dissipation: insights from ab-initio molecular dynamics of HCO formation
• H2 formation on interstellar grains and the fate of reaction energy
• Phosphorus-bearing molecules in massive dense cores
• The first steps of Interstellar Phosphorus Chemistry
• Where does the energy go during the interstellar NH${}_3$ formation on water ice? A computational study
• The Case of H${}_2$C${}_3$O Isomers, Revisited: Solving the Mystery of the Missing Propadienone
• Binding Energy Evaluation Platform: A database of quantum chemical binding energy distributions for the astrochemical community
• Isomers in Interstellar Environments (I): The Case of Z- and E-Cyanomethanimine
• Predicting Properties of Periodic Systems from Cluster Data: A Case Study of Liquid Water
• Fast and Sample-Efficient Interatomic Neural Network Potentials for Molecules and Materials Based on Gaussian Moments
• Neural-Network Assisted Study of Nitrogen Atom Dynamics on Amorphous Solid Water. I. Adsorption & Desorption
• Acetaldehyde binding energies: a coupled experimental and theoretical study
• Quantifying the chemical desorption of H${}_2$S and PH${}_3$ from amorphous water ice surfaces

Cited by in corpus (7)

• Cracking the Puzzle of CO2 Formation on Interstellar Ices. Quantum Chemical and Kinetic Study of the CO + OH -> CO2 + H Reaction
• Proposed importance of HOCO chemistry: Inefficient formation of CO${}_2$ from CO and OH reactions on ice dust
• A multigrain-multilayer astrochemical model with variable desorption energy for surface species
• CO Adsorption Sites on Interstellar Water Ices Explored with Machine Learning Potentials. Binding energy distributions and snowline
• Diffusive vs. non-diffusive paths to interstellar hydrogen peroxide. A machine learning-based molecular dynamics study
• Piecing together formic acid isomerism in dark clouds. Detection of cis-formic acid in TMC-1 and astrochemical modeling
• A sensitivity analysis of interstellar ice chemistry in astrochemical models