Acetaldehyde binding energies: a coupled experimental and theoretical study

Ferrero, Stefano; Grieco, Francesco; Mohamed, A-S Ibrahim; Dulieu, F.; Rimola, Albert; Ceccarelli, C.; Nervi, Carlo; Minissale, Marco; Ugliengo, Piero

doi:10.1093/mnras/stac2358

Cited by 24 publications

(15 citation statements)

References 88 publications

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“…Although most of the molecules desorb in the “trapped” peak, the eventual appearance of the “volcano” TPD peak at higher laser fluence indicates that the molecule’s interaction with water is not too strong. This fits with the assignment to acetaldehyde, which can form one hydrogen bond with water, but still prefers to form clusters at the interface when deposited on water–ice surface . Some hydrogen bonds are formed between water and acetaldehyde resulting in the codesorption of the two molecules.…”

Section: Results and Discussionsupporting

confidence: 83%

“…This fits with the assignment to acetaldehyde, which can form one hydrogen bond with water, but still prefers to form clusters at the interface when deposited on water–ice surface. 53 Some hydrogen bonds are formed between water and acetaldehyde resulting in the codesorption of the two molecules. Acetaldehyde molecules that do not form hydrogen bonds with water due to unfavorable relative orientation are ejected in the “volcano” peak.…”

Section: Results and Discussionmentioning

confidence: 99%

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Chemical Reactivity of Strongly Interacting, Hydrogen-Bond-Forming Molecules Following 193 nm Photon Irradiation: Methanol in Amorphous Solid Water at Low Temperatures

et al. 2023

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Mixtures of methanol and amorphous solid water (ASW) ices are observed in the interstellar medium (ISM), where they are subject to irradiation by UV photons and bombardment by charged particles. The charged particles, if at high enough density, induce a local electric field in the ice film that potentially affects the photochemistry of these ices. When CD 3 OD@ASW ices grown at 38 K on a Ru(0001) substrate are irradiated by 193 nm (6.4 eV) photons, products such as HD, D 2 , CO, and CO 2 are formed in large abundances relative to the initial amount of CD 3 OD. Other molecules such as D 2 O, CD 4 , acetaldehyde, and ethanol and/or dimethyl ether are also observed, but in smaller relative abundances. The reactivity cross sections range from (2.6 ± 0.3) × 10 −21 to (3.8 ± 0.3) × 10 −25 cm 2 /photon. The main products are formed through two competing mechanisms: direct photodissociation of methanol and water and dissociative electron attachment (DEA) by photoelectrons ejected from the Ru(0001) substrate. An electric field of 2 × 10 8 V/m generated within the ASW film during Ne + ions bombardment is apparently not strong enough to affect the relative abundances (selectivity) of the photochemical products observed in this study.

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Section: Results and Discussionsupporting

confidence: 83%

Section: Results and Discussionmentioning

confidence: 99%

Chemical Reactivity of Strongly Interacting, Hydrogen-Bond-Forming Molecules Following 193 nm Photon Irradiation: Methanol in Amorphous Solid Water at Low Temperatures

et al. 2023

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“…This fact could be inferred from previous studies (Garrod, R. T. et al 2007;Minissale, M. et al 2016;Fredon & Cuppen 2018;Fredon et al 2021) where the efficiency of chemical desorption is a function of BE. However, as previously indicated for thermal desorption studies Ferrero et al 2022a;Molpeceres, G. et al 2022), we must emphasize that considering the whole distribution of binding sites is essential to unravel the role of non-thermal mechanisms. Here we found that the binding energy anticorrelates with the fraction of energy dissipated into the lattice and the acquired translational energy of the nascent molecule.…”

Section: Extended Samplingmentioning

confidence: 89%

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

Molpeceres¹,

Zaverkin²,

Furuya³

et al. 2023

Preprint

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Context. 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. Aims. Our goal with this study is to use state-of-the-art methods to determine the fate of the chemical energy in the simplest phosphorous hydride reaction. Methods. We studied the reaction dynamics of the P + H − −− → PH reaction on amorphous solid water, a reaction of astrophysical interest, using ab-initio molecular dynamics with atomic forces evaluated by a neural network interatomic potential. Results. 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 %. Conclusions. 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.

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“…As pointed out by previous articles (Ferrero et al 2022;Minissale et al 2022;Tinacci et al 2022), attention should be given to the way in which the prefactor in the desorption rate (k thdes in Equation (1)) is computed. As in the aforementioned articles, we here adopt the Tait et al (2005) formula:…”

Section: The Desorption Rate Prefactormentioning

confidence: 99%

Theoretical Water Binding Energy Distribution and Snowline in Protoplanetary Disks

Tinacci

Germain

Pantaleone

et al. 2023

ApJ

Self Cite

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Water is one of the most important and abundant molecules in star-forming regions. In protoplanetary disks, where planets and comets form, H2O is in a gas or solid form, depending on the dust temperature, i.e., the distance from the center and its binding energy (BE). Not surprisingly, several experimental and theoretical studies of the H2O BE have been published. We report new ab initio calculations carried out on a large model of interstellar ice, where we identified 144 different adsorption sites. The BE associated with those sites ranges between 14.2 kJ mol−1 (1705 K) and 61.6 kJ mol−1 (7390 K). The distribution of the computed BEs as a function of BE follows a Gaussian peaked at 35.4 kJ mol−1 (4230 K) with a standard deviation of 9.7 kJ mol−1 (1160 K). The computed pre-exponential factor (ν) ranges between 9 × 1012 and 6 × 1014 s−1. We evaluated the impact of the newly calculated BE and ν distributions on the snowline of a generic protoplanetary disk. We found that the region where water is frozen onto the ice is much smaller (a factor of 10 smaller radius) than that computed with the single BE (5600 K) and ν (2 × 1012 s−1) values commonly adopted by astrochemical models. Besides, ∼10% of water remains frozen in relatively warm (∼150 K) regions, where the single BE and ν model would predict a full release of the ice in the gas phase. This last aspect may have an impact on the quantity trapped in the planetesimals eventually forming rocky planets.

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Acetaldehyde binding energies: a coupled experimental and theoretical study

Cited by 24 publications

References 88 publications

Chemical Reactivity of Strongly Interacting, Hydrogen-Bond-Forming Molecules Following 193 nm Photon Irradiation: Methanol in Amorphous Solid Water at Low Temperatures

Chemical Reactivity of Strongly Interacting, Hydrogen-Bond-Forming Molecules Following 193 nm Photon Irradiation: Methanol in Amorphous Solid Water at Low Temperatures

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

Theoretical Water Binding Energy Distribution and Snowline in Protoplanetary Disks

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