Lack of Aggregation of Molecules on Ice Nanoparticles

Pysanenko, Andriy; Habartová, Alena; Svrčková, P.; Lengyel, Jozef; Poterya, Viktoriya; Roeselová, Martina; Fedor, Juraj; Fárnı́k, Michal

doi:10.1021/acs.jpca.5b05368

Cited by 29 publications

(55 citation statements)

References 51 publications

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“…The first is a cluster beam (CLUB) apparatus located in Prague, Czech Republic [ 12 , 15 ]. The clusters were produced by a supersonic expansion into vacuum, and the beam was skimmed and passed through three differentially pumped chambers (one containing a pickup cell) into an interaction chamber where it was crossed with an electron beam of variable energy.…”

Section: Methodsmentioning

confidence: 99%

Suppression of low-energy dissociative electron attachment in Fe(CO)₅ upon clustering

Lengyel¹,

Papp²,

Matejčík³

et al. 2017

Beilstein J. Nanotechnol.

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In this work, we probe anion production upon electron interaction with Fe(CO)5 clusters using two complementary cluster-beam setups. We have identified two mechanisms that lead to synthesis of complex anions with mixed Fe/CO composition. These two mechanisms are operative in distinct electron energy ranges. It is shown that the elementary decomposition mechanism that has received perhaps the most attention in recent years (i.e., dissociative electron attachment at energies close to 0 eV) becomes suppressed upon increasing aggregation of iron pentacarbonyl. We attribute this suppression to the electrostatic shielding of a long-range interaction that strongly enhances the dissociative electron attachment in isolated Fe(CO)5.

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Section: Methodsmentioning

confidence: 99%

Suppression of low-energy dissociative electron attachment in Fe(CO)₅ upon clustering

Lengyel¹,

Papp²,

Matejčík³

et al. 2017

Beilstein J. Nanotechnol.

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“…A similar result was obtained later by Pysanenko et al considering CH 3 Cl molecules adsorbed on ice, who concluded that the interaction with the polar water molecules inhibits the mobility of the adsorbed molecules. 20 Moreover, it was also shown by means of metastable impact electron spectroscopy that CHCl 3 molecules are adsorbed at the ice surface with their H atom oriented towards the substrate below 120 K, 21 and for all chlorinated methane derivatives (CH 4-x Cl x ) that their interaction with water occurs through the oxygen atom. 22 Finally, Vysokikh et al…”

Section: Introductionmentioning

confidence: 99%

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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“…Aoki et al showed, using metastable impact electron spectroscopy that CH 3 Cl molecules adsorbed at the ice surface turn their H atoms towards the ice phase below 120 K [26]. It was also shown that both CHCl 3 [24,25] and CH 3 Cl [27] remain immobile at the ice surface in the entire temperature range below desorption due to their interaction with the surface water molecules [24,25,27], and that the interaction of all chlorinated methane derivatives with water involves the water O atom [28].…”

Section: Introductionmentioning

confidence: 99%

Dependence of the adsorption of halogenated methane derivatives at the ice surface on their chemical structure

Sumi

Picaud

Jedlovszky

2017

Journal of Molecular Liquids

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The adsorption of all the fluorinated and chlorinated methane derivatives as well as methane itself at the surface of I h ice is studied at the tropospheric temperature of 200 K by grand canonical Monte Carlo simulations. The general behaviour of the obtained isotherms is in good accordance with existing experimental data, giving us confidence in the models used. The shape of the adsorption isotherms is discussed in terms of the interplay of adhesive and cohesive interactions. It is found that in cases when the former of the two interactions is clearly the stronger one, multilayer adsorption occurs; when the latter interaction is the dominant one, no considerable adsorption is observed, while in cases when the two interactions are of roughly the same strength, the formation of a saturated monolayer occurs. The isotherms exhibit the Langmuir shape, at least up to the pressures where multilayer adsorption starts to occur, given that the cohesion acting between the adsorbate molecules is only moderately strong. Too strong cohesion, on the other hand, leads to the deviation of the isotherm from the Langmuir shape. While the strength of cohesion depends on the properties of the adsorbate molecules, that of adhesion is determined by hydrogen bond formation between the adsorbed molecules and surface waters. Our results show that while CH 3 F and CH 3 Cl form several weak, C-H donated hydrogen bonds with the surface molecules of the ice phase, the adsorbates containing more than one halogen atom form only one, though strong, O-H donated hydrogen bond with them.

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Lack of Aggregation of Molecules on Ice Nanoparticles

Cited by 29 publications

References 51 publications

Suppression of low-energy dissociative electron attachment in Fe(CO)₅ upon clustering

Suppression of low-energy dissociative electron attachment in Fe(CO)₅ upon clustering

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

Dependence of the adsorption of halogenated methane derivatives at the ice surface on their chemical structure

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Lack of Aggregation of Molecules on Ice Nanoparticles

Cited by 29 publications

References 51 publications

Suppression of low-energy dissociative electron attachment in Fe(CO)5 upon clustering

Suppression of low-energy dissociative electron attachment in Fe(CO)5 upon clustering

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

Dependence of the adsorption of halogenated methane derivatives at the ice surface on their chemical structure

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Product

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Suppression of low-energy dissociative electron attachment in Fe(CO)₅ upon clustering

Suppression of low-energy dissociative electron attachment in Fe(CO)₅ upon clustering