A QM/MM study of HCl adsorption at ice surface defect sites

Bolton, Kim

doi:10.1016/s0166-1280(03)00295-1

Cited by 31 publications

(46 citation statements)

References 63 publications

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“…18,31 If one assumes that the proton comes solely from surface defects, the experimental yield at 90 K indicates an intrinsic CI surface defect density of ∼10 12 cm À2 . Assuming ∼10 15 sites/cm À2 for a hexagonal bilayer, this is 10 À3 of the total surface sites available.…”

Section: Iva Mechanisms For Cation Esdmentioning

confidence: 99%

Probing the Interaction of Hydrogen Chloride with Low-Temperature Water Ice Surfaces Using Thermal and Electron-Stimulated Desorption

et al. 2011

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The interaction and autoionization of HCl on low-temperature (80-140 K) water ice surfaces has been studied using low-energy (5-250 eV) electron-stimulated desorption (ESD) and temperature programmed desorption (TPD). There is a reduction of H(+) and H(2)(+) and a concomitant increase in H(+)(H(2)O)(n=1-7) ESD yields due to the presence of submonolayer quantities of HCl. These changes are consistent with HCl induced reduction of dangling bonds required for H(+) and H(2)(+) ESD and increased hole localization necessary for H(+)(H(2)O)(n=1-7) ESD. For low coverages, this can involve nonactivated autoionization of HCl, even at temperatures as low as 80 K; well below those typical of polar stratospheric cloud particles. The uptake and autoionization of HCl is supported by TPD studies which show that for HCl doses ≤0.5 ± 0.2 ML (ML = monolayer) at 110 K, desorption of HCl begins at 115 K and peaks at 180 K. The former is associated with adsorption of a small amount of molecular HCl and is strongly dependent on the annealing history of the ice. The latter peak at 180 K is commensurate with desorption of HCl via recombinative desorption of solvated separated ion pairs. The activation energy for second-order desorption of HCl initially in the ionized state is 43 ± 2 kJ/mol. This is close to the zero-order activation energy for ice desorption.

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Section: Iva Mechanisms For Cation Esdmentioning

confidence: 99%

Probing the Interaction of Hydrogen Chloride with Low-Temperature Water Ice Surfaces Using Thermal and Electron-Stimulated Desorption

et al. 2011

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“…Most of the published experiments suggest a thermal activated HCl ionization [5,16]. From a theoretical point of view, calculations predict a dissociation mechanism that depends strongly either on the arrangement of the dangling bonds [7,17,18] or on defective sites on the surface [19,20] or on the possibility for HCl to be inserted in the uppermost layer [9,10]. All these processes are actually favored by a high surface temperature.…”

Section: Introductionmentioning

confidence: 99%

Photodissociation of a HCl molecule adsorbed on ice at T=210K

et al. 2007

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“…[3][4][5][6][7] Experiments which explore this transition are still quite rare. The HX dissociation has been theoretically studied on model ice surfaces, [12][13][14][15][16][17] and it has also been the subject of extensive experimental investigations using temperaturecontrolled desorption, x-ray absorption spectroscopy, reac-tive Cs + ion scattering, low energy sputtering, and Fourier transform infrared spectroscopy. 8 A pump-probe photoionization experiment with HBr͑H 2 O͒ n clusters confirmed the transition for n =5.…”

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confidence: 99%

Photodissociation of hydrogen halide molecules on free ice nanoparticles

Poterya

Fárnı́k

Slavı́ček

et al. 2007

The Journal of Chemical Physics

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Photodissociation of water clusters doped with HX(X=Br,Cl), molecules has been studied in a molecular beam experiment. The HX(H2O)n clusters are dissociated with 193 nm laser pulses, and the H fragments are ionized at 243.07 nm and their time-of-flight distributions are measured. Experiments with deuterated species DBr(H2O)n and HBr(D2O)n suggest that the photodissociation signal originates from the presence of the HX molecule on the water cluster, but does not come directly from a photolysis of the HX molecule. The H fragment is proposed to originate from the hydronium molecule H3O. Possible mechanisms of the H3O production are discussed. Experimental evidence suggests that acidic dissociation takes place in the cluster, but the H3O+ ion remains rather immobile.

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A QM/MM study of HCl adsorption at ice surface defect sites

Cited by 31 publications

References 63 publications

Probing the Interaction of Hydrogen Chloride with Low-Temperature Water Ice Surfaces Using Thermal and Electron-Stimulated Desorption

Probing the Interaction of Hydrogen Chloride with Low-Temperature Water Ice Surfaces Using Thermal and Electron-Stimulated Desorption

Photodissociation of a HCl molecule adsorbed on ice at T=210K

Photodissociation of hydrogen halide molecules on free ice nanoparticles

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