| 1. |
- Andersson, Patrik U, 1970, et al.
(författare)
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Carbon dioxide interactions with crystalline and amorphous ice surfaces
- 2004
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Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 108:21, s. 4627-4631
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Tidskriftsartikel (refereegranskat)abstract
- Carbon dioxide interactions with crystalline and amorphous water ice have been studied by time-resolved molecular beam techniques. CO2 collisions at thermal kinetic energies with ice in the temperature range 100-160 K result in efficient trapping on the ice surface followed by desorption. The desorption kinetics on crystalline ice at 100-125 K are well described by the Arrhenius equation with an activation energy of 0.22 +/- 0.02 eV and a preexponential factor of 10(13.32+/-0.57) s(-1). Below 120 K, CO2 populates strongly bonded sites on amorphous ice, resulting in surface residence times on the order of minutes at 100 K, and the desorption data can in this case not be explained by a simple first-order process. The results are compared to previous studies of gas-ice interactions, and the implications for heterogeneous processes in the terrestrial atmosphere are discussed.
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| 2. |
- Andersson, Patrik U, 1970, et al.
(författare)
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Formation of Highly Rovibrationally Excited Ammonia from Dissociative Recombination of NH4
- 2010
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Ingår i: Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 1:17, s. 2519-2523
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Tidskriftsartikel (refereegranskat)abstract
- The internal energy distribution of ammonia formed in the dissociative recombination (DR) of NH4+ with electrons has been studied by an imaging technique at the ion storage ring CRYRING. The DR process resulted in the formation of NH3 + H (0.90 ± 0.01), with minor contributions from channels producing NH2 + H2 (0.05 ± 0.01) and NH2 + 2H (0.04 ± 0.02). The formed NH3 molecules were highly internally excited, with a mean rovibrational energy of 3.3 ± 0.4 eV, which corresponds to 70% of the energy released in the neutralization process. The internal energy distribution was semiquantitatively reproduced by ab initio direct dynamics simulations, and the calculations suggested that the NH3 molecules are highly vibrationally excited while rotational excitation is limited. The high internal excitation and the translational energy of NH3 and H will influence their subsequent reactivity, an aspect that should be taken into account when developing detailed models of the interstellar medium and ammonia-containing plasmas.
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| 3. |
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| 4. |
- Andersson, Patrik U, 1970, et al.
(författare)
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Water Condensation on Graphite Studied by Elastic Helium Scattering and Molecular Dynamics Simulations
- 2007
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Ingår i: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 111:42, s. 15258-15266
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Tidskriftsartikel (refereegranskat)abstract
- Formation of water/ice layers on graphite has been studied in the temperature range from 90 to 180 K by elastic helium scattering, light scattering, and molecular dynamics simulations. Combined helium- and light-scattering experiments show that an ice film that wets the graphite surface is formed at surface temperatures of 100-140 K, whereas three-dimensional ice structures are formed at 140-180 K. Desorption of adsorbed water molecules competes with water incorporation into the ice film, and the ice formation rate is strongly temperature dependent. At 150 K, ice-layer formation takes place at the same time scale as layer reconstruction, and its properties are sensitive to the water deposition rate. The experimental results are compared with kinetics models, and the Johnston-Mehl-Avrami-Kolmogorov model is concluded to well describe the ice-layer formation kinetics in the whole temperature range. Molecular dynamics simulations of water-cluster formation on graphite at 90-180 K show that water molecules and small clusters are highly mobile on the surface, which rapidly results in the nucleation of large and less mobile clusters on the surface. Clusters formed at low temperature tend to have the most molecules in direct contact with the uppermost graphite layer, while multilayer cluster structures are preferred at high temperatures. The results are discussed and compared with earlier studies of water ice formation on solid surfaces.
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| 5. |
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| 6. |
- Janhäll, Sara, 1965, et al.
(författare)
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Evolution of the urban aerosol during winter temperature inversion episodes
- 2006
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Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310. ; 40:28, s. 5355-5366
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Tidskriftsartikel (refereegranskat)abstract
- Winter temperature inversions are for Nordic urban sites a major cause for exceeding air-quality legislation thresholds for most primary pollutants. In this study, number particle size distributions have been measured and compared to other tracers for traffic emissions. Concentrations during winter days with and without morning temperature inversion were compared. Morning temperature inversion resulted in high concentrations of traffic-related pollutants, including CO, NO and NO2 together with ultrafine particles, while the pollution levels where considerably lower during mornings without temperature inversion. The specific time trends of NOx species could be well understood when considering the reaction with O-3. The two different particle measures used in this study, i.e. the number concentration of ultrafine particles (10-100 nm) and the mass of particles below 10 pm (PM10), both increased during morning rush hours. When the morning inversion broke up and ground-level air mixed with air aloft, the number of particles decreased more rapidly than PM10 concentrations. LIDAR measurements were used to follow the vertical distribution of particles, and they clearly showed how the mixing processes started after the morning inversion and resulted in rising of the inversion followed by a relatively well-mixed boundary layer with a height of I kin around 14:00. (c) 2006 Elsevier Ltd. All rights reserved.
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| 7. |
- Kong, Xiangrui, et al.
(författare)
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Environmental molecular beam studies of ice surface processes
- 2011
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Ingår i: Physics and Chemistry of Ice 2010 (The 12th International Conference on the Physics and Chemistry of Ice, Sapporo, Japan, September 5-10, 2010, Eds. Y. Furukawa, G. Sazaki, T. Uchida, N. Watanabe, Hokkaido University Press, Sapporo, Japan, 2011). - 9784832903616 ; , s. 79-88
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Konferensbidrag (refereegranskat)abstract
- The development and application of a new molecular beam setup for studies of gas-ice interactions at pressures in the 0.001 mbar range is described. Direct simulation Monte Carlo calculations have been applied to optimize the experimental design with respect to gas transmission through the high pressure zone outside the ice surface and pressure along the surface plane. In a first application of the new setup elastic helium scattering and light scattering have been used to study the formation of water, methanol and water-methanol ice on a graphite surface in the temperature range from 180 to 215 K. Water does not wet the graphite surface under these conditions, in agreement with earlier results obtained below 180 K, while methanol readily forms a thin layer on the surface. Methanol enhances water ice nucleation and influences the properties of the ice formed, but does not have a major impact on ice growth or evaporation once a thick water-containing ice layer has formed. The potential for further development of the molecular beam technique are discussed.
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| 8. |
- Kong, Xiangrui, et al.
(författare)
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Ice Formation via Deposition Mode Nucleation on Bare and Alcohol-Covered Graphite Surfaces
- 2012
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Ingår i: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 116:16, s. 8964-8974
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Tidskriftsartikel (refereegranskat)abstract
- Deposition of water on aerosol particles contributes to ice cloud formation in the atmosphere with implications for the water cycle and climate on Earth. The heterogeneous ice nucleation process is influenced by physicochemical properties of the substrate, but the mechanisms remain incompletely understood. Here, we report on ice formation on bare and alcohol-covered graphite at temperatures from 175 to 213 K, probed by elastic helium and light scattering. Water has a low wettability on bare and butanol-covered graphite resulting in the growth of rough ice surfaces. In contrast, preadsorbed methanol provides hydrophilic surface sites and results in the formation of smooth crystalline ice; an effect that is pronounced also for submonolayer methanol coverages. The alcohols primarily reside at the ice surface and at the ice–graphite interface with a minor fraction being incorporated into the growing ice structures. Methanol has no observable effect on gas/solid water vapor exchange, whereas butanol acts as a transport barrier for water resulting in a reduction in ice evaporation rate at 185 K. Implications for the description of deposition mode freezing are discussed.
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| 9. |
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| 10. |
- Olofson, K. Frans G., 1976, et al.
(författare)
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Urban aerosol evolution and particle formation during wintertime temperature inversions
- 2009
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Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310. ; 43, s. 340-346
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Tidskriftsartikel (refereegranskat)abstract
- Aerosol temporal and spatial distributions during wintertime temperature inversions in Gothenburg, Sweden, have been characterized by ground-based and airborne particle measurements combined with lidar measurements. Ground inversions frequently developed during evenings and nights with stable cold conditions, and the low wintertime insolation often resulted in near neutral boundary layer conditions during day-time. Under these conditions ground level aerosol concentrations peaked during morning rush hours and often remained relatively high throughout the day due to inefficient ventilation. The particle number concentrations decreased slowly with increasing altitude within the boundary layer, and measurements slightly above the boundary layer suggested limited entrainment of polluted air into the free troposphere. High concentrations of ultrafine particles were observed throughout the boundary layer up to altitudes of 1100 m, which suggested that nucleation took place within the residual layer during the night and early morning. Recently formed particles were also observed around midday when the layer near ground was ventilated by mixing into the boundary layer, which indicated that ultrafine particles were either transported down from the residual layer to ground level or formed when the polluted surface layer mixed with the cleaner air above.
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