Molecular Simulations of Halomethanes at the Air/Ice Interface

Habartová, Alena; Hormain, Laureline; Pluhařová, Eva; Briquez, Stéphane; Monnerville, Maurice; Toubin, Céline; Roeselová, Martina

doi:10.1021/acs.jpca.5b06071

Cited by 7 publications

(14 citation statements)

References 31 publications

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“…6, agrees perfectly with what was previously found to be preferred by CH 3 F, 59 and agrees also well with the earlier finding of Harper et al concerning the preferred orientation of CH 3 Cl at the free water surface. 64 It should also be noted that this orientational preference is somewhat different from what was claimed to be the preferred orientation of CH 3 Cl and CH 3 Br by Habartová et al 63 In the case of CHCl 3 , we have found two preferred orientations, both corresponding to slightly negative cos values. The first of these orientations, denoted here as I CHCl3 , corresponds to  = 0 o , while in the case of the second one, marked here as II CHCl3 , the value of  is close to 60 o .…”

Section: Orientation Of the Adsorbed Moleculescontrasting

confidence: 85%

Adsorption of Chlorinated Methane Derivatives at the Ice Surface: A Grand Canonical Monte Carlo Simulation Study

2017

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The adsorption behavior of three chlorinated methane derivative molecules, namely CH 3 Cl, CHCl 3 , and CCl 4 is investigated at the (0001) surface of I h ice at the tropospheric temperature of 200 K by means of grand canonical Monte Carlo simulations. This study completes our earlier investigations concerning the adsorption of CH 4 , CH 2 Cl 2 , and fluorinated methane derivatives. Our results show that neither CHCl 3 nor CCl 4 exhibits any adsorption. This complete lack of adsorption is attributed to the interplay of the very strong cohesion acting between the adsorbate molecules, and their relatively weak interaction with the ice phase. By contrast, CH 3 Cl does exhibit noticeable adsorption on ice, and the adsorbed molecules prefer to turn towards the ice surface by their H atoms, forming weak, C-H …. O type hydrogen bonds with surface waters. The lateral (i.e., adsorbate-adsorbate) contribution to the total interaction energy of the adsorbed molecules is always considerably larger (in magnitude) than in the case of the corresponding fluorinated analogs, making also the total adsorption energy lower for the chlorinated molecules than for their fluorinated counterpart. As a consequence of this strong attraction between the chlorinated adsorbate molecules, their condensation occurs at lower chemical potential (and, hence, pressure) values than that of the fluorinated analogs, which prevents the formation or completion of the adsorption layer of the chlorinated molecules.

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Section: Orientation Of the Adsorbed Moleculescontrasting

confidence: 85%

Adsorption of Chlorinated Methane Derivatives at the Ice Surface: A Grand Canonical Monte Carlo Simulation Study

2017

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“…To achieve a better understanding of the interaction between halogenated compounds and ice surface, we have recently performed a set of GCMC simulations investigating the adsorption of all the fluorinated and chlorinated methane derivatives (CH n X 4-n , n ranging from 0 to 4, X=Cl, F) at the (0001) surface of I h ice [40][41][42]. These studies well complement well the partial results obtained from previous MD simulations on some of these molecules interacting with ice surface [39,80,81]. Because the results of our GCMC studies have been reviewed in a recent publication [43], only the main conclusions are recalled here.…”

Section: Adsorption Of Halogenated Methane Derivatives On Crystallinesupporting

confidence: 61%

Molecular-scale simulations of organic compounds on ice: application to atmospheric and interstellar sciences

Picaud

Jedlovszky

2018

Molecular Simulation

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In this paper, we present a brief review of what has been learned about the adsorption characteristics of various organic molecules at the surface of ice, from more than 15 years of computer simulation studies at the molecular scale. In particular, grand canonical Monte Carlo and molecular dynamics calculations were performed to determine the adsorption isotherms, the saturation coverage of the first molecular layer at the ice surface, the preferred orientations of the molecules in their adsorption sites, and the corresponding adsorption energies. The results of the simulations indicated that the main driving force for trace gas adsorption on ice is hydrogen bonding not only between the adsorbate and the water molecules of the ice surface, but also within the adsorbate. When possible, the comparison with available experimental data showed a close agreement, supporting thus the methodology used in the modelling. Finally, the present review demonstrates how computer simulation can nicely complement experimental approaches for studying interactions between trace gases and ice under tropospheric and interstellar condition

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“…[23][24][25][26][27][28][29][30][31][32] In addition, Grand Canonical Monte Carlo (GCMC) simulations 17,33 have also been performed to simulate the adsorption isotherms of various classes of volatile organic compounds and atmospheric pollutants on ice at low temperatures. [34][35][36][37][38][39][40][41][42][43][44] Indeed, the GCMC method is particularly suitable for studying adsorption, because in this method the chemical potential rather than the number of the adsorbate molecules is fixed in the simulation.…”

Section: Introductionmentioning

confidence: 99%

Adsorption of Methylamine at the Surface of Ice. A Grand Canonical Monte Carlo Simulation Study

et al. 2016

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Abstract:A series of 41 Monte Carlo simulations are performed in the grand canonical ensemble at 200 K to determine the adsorption isotherm and study in detail the adsorption of methylamine at the surface of I h ice. The adsorption isotherm exhibits a plateau, corresponding to the saturated adsorption monolayer, in a broad range of chemical potentials and pressures.However, even this part of the adsorption isotherm deviates noticeably from the Langmuir shape. Shortly before condensation of methylamine occurs outer molecular layers also start building up. The remarkable stability of the adsorption monolayer is caused by the interplay of hydrogen bonding interaction between the adsorbed methylamine and surface water molecules and dipolar interaction between neighboring adsorbed methylamines. As a consequence, the adsorbed methylamine molecules exhibit a rich orientational distribution relative to the ice surface and the adsorption is accompanied by rather large energy variations.3

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Molecular Simulations of Halomethanes at the Air/Ice Interface

Cited by 7 publications

References 31 publications

Adsorption of Chlorinated Methane Derivatives at the Ice Surface: A Grand Canonical Monte Carlo Simulation Study

Adsorption of Chlorinated Methane Derivatives at the Ice Surface: A Grand Canonical Monte Carlo Simulation Study

Molecular-scale simulations of organic compounds on ice: application to atmospheric and interstellar sciences

Adsorption of Methylamine at the Surface of Ice. A Grand Canonical Monte Carlo Simulation Study

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