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1.
  • Bianchi, F., et al. (författare)
  • The SALTENA Experiment : Comprehensive Observations of Aerosol Sources, Formation, and Processes in the South American Andes
  • 2022
  • Ingår i: Bulletin of The American Meteorological Society - (BAMS). - 0003-0007 .- 1520-0477. ; 103:2, s. E212-E229
  • Tidskriftsartikel (refereegranskat)abstract
    • This paper presents an introduction to the Southern Hemisphere High Altitude Experiment on Particle Nucleation and Growth (SALTENA). This field campaign took place between December 2017 and June 2018 (wet to dry season) at Chacaltaya (CHC), a GAW (Global Atmosphere Watch) station located at 5,240 m MSL in the Bolivian Andes. Concurrent measurements were conducted at two additional sites in El Alto (4,000 m MSL) and La Paz (3,600 m MSL). The overall goal of the campaign was to identify the sources, understand the formation mechanisms and transport, and characterize the properties of aerosol at these stations. State-of-the-art instruments were brought to the station complementing the ongoing permanent GAW measurements, to allow a comprehensive description of the chemical species of anthropogenic and biogenic origin impacting the station and contributing to new particle formation. In this overview we first provide an assessment of the complex meteorology, airmass origin, and boundary layer-free troposphere interactions during the campaign using a 6-month high-resolution Weather Research and Forecasting (WRF) simulation coupled with Flexible Particle dispersion model (FLEXPART). We then show some of the research highlights from the campaign, including (i) chemical transformation processes of anthropogenic pollution while the air masses are transported to the CHC station from the metropolitan area of La Paz-El Alto, (ii) volcanic emissions as an important source of atmospheric sulfur compounds in the region, (iii) the characterization of the compounds involved in new particle formation, and (iv) the identification of long-range-transported compounds from the Pacific or the Amazon basin. We conclude the article with a presentation of future research foci. The SALTENA dataset highlights the importance of comprehensive observations in strategic high-altitude locations, especially the undersampled Southern Hemisphere.
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2.
  • Pasquier, J. T., et al. (författare)
  • The Ny-Ålesund Aerosol Cloud Experiment (NASCENT) : Overview and First Results
  • 2022
  • Ingår i: Bulletin of The American Meteorological Society - (BAMS). - 0003-0007 .- 1520-0477. ; 103:11, s. e2533-E2558
  • Tidskriftsartikel (refereegranskat)abstract
    • The Arctic is warming at more than twice the rate of the global average. This warming is influenced by clouds, which modulate the solar and terrestrial radiative fluxes and, thus, determine the surface energy budget. However, the interactions among clouds, aerosols, and radiative fluxes in the Arctic are still poorly understood. To address these uncertainties, the Ny-Ålesund Aerosol Cloud Experiment (NASCENT) study was conducted from September 2019 to August 2020 in Ny-Ålesund, Svalbard. The campaign’s primary goal was to elucidate the life cycle of aerosols in the Arctic and to determine how they modulate cloud properties throughout the year. In situ and remote sensing observations were taken on the ground at sea level, at a mountaintop station, and with a tethered balloon system. An overview of the meteorological and the main aerosol seasonality encountered during the NASCENT year is introduced, followed by a presentation of first scientific highlights. In particular, we present new findings on aerosol physicochemical and molecular properties. Further, the role of cloud droplet activation and ice crystal nucleation in the formation and persistence of mixed-phase clouds, and the occurrence of secondary ice processes, are discussed and compared to the representation of cloud processes within the regional Weather Research and Forecasting Model. The paper concludes with research questions that are to be addressed in upcoming NASCENT publications.  
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3.
  • Fanourgakis, George S., et al. (författare)
  • Evaluation of global simulations of aerosol particle and cloud condensation nuclei number, with implications for cloud droplet formation
  • 2019
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:13, s. 8591-8617
  • Tidskriftsartikel (refereegranskat)abstract
    • A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011-2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of -24% and -35% for particles with dry diameters >50 and >120nm, as well as -36% and -34% for CCN at supersaturations of 0.2% and 1.0%, respectively. However, they seem to behave differently for particles activating at very low supersaturations (<0.1%) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N3 (number concentration of particles with dry diameters larger than 3nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2% (CCN0.2) compared to that for N3, maximizing over regions where new particle formation is important. An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter. Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated on average by the models by 40% during winter and 20% in summer. In contrast to the large spread in simulated aerosol particle and CCN number concentrations, the CDNC derived from simulated CCN spectra is less diverse and in better agreement with CDNC estimates consistently derived from the observations (average NMB -13% and -22% for updraft velocities 0.3 and 0.6ms-1, respectively). In addition, simulated CDNC is in slightly better agreement with observationally derived values at lower than at higher updraft velocities (index of agreement 0.64 vs. 0.65). The reduced spread of CDNC compared to that of CCN is attributed to the sublinear response of CDNC to aerosol particle number variations and the negative correlation between the sensitivities of CDNC to aerosol particle number concentration (Nd=Na) and to updraft velocity (Nd=w). Overall, we find that while CCN is controlled by both aerosol particle number and composition, CDNC is sensitive to CCN at low and moderate CCN concentrations and to the updraft velocity when CCN levels are high. Discrepancies are found in sensitivities Nd=Na and Nd=w; models may be predisposed to be too "aerosol sensitive" or "aerosol insensitive" in aerosol-cloud-climate interaction studies, even if they may capture average droplet numbers well. This is a subtle but profound finding that only the sensitivities can clearly reveal and may explain intermodel biases on the aerosol indirect effect.
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4.
  • Tatzelt, C., et al. (författare)
  • Circum-Antarctic abundance and properties of CCN and INPs
  • 2022
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:14, s. 9721-9745
  • Tidskriftsartikel (refereegranskat)abstract
    • Aerosol particles acting as cloud condensation nuclei (CCN) or ice-nucleating particles (INPs) play a major role in the formation and glaciation of clouds. Thereby they exert a strong impact on the radiation budget of the Earth. Data on abundance and properties of both types of particles are sparse, especially for remote areas of the world, such as the Southern Ocean (SO). In this work, we present unique results from ship-borne aerosol-particle-related in situ measurements and filter sampling in the SO region, carried out during the Antarctic Circumnavigation Expedition (ACE) in the austral summer of 2016-2017. An overview of CCN and INP concentrations over the Southern Ocean is provided and, using additional quantities, insights regarding possible CCN and INP sources and origins are presented. CCN number concentrations spanned 2 orders of magnitude, e.g. for a supersaturation of 0.3% values ranged roughly from 3 to 590 cm(-3). CCN showed variable contributions of organic and inorganic material (inter-quartile range of hygroscopicity parameter kappa from 0.2 to 0.9). No distinct size dependence of kappa was apparent, indicating homogeneous composition across sizes (critical dry diameter on average between 30 and 110 nm). The contribution of sea spray aerosol (SSA) to the CCN number concentration was on average small. Ambient INP number concentrations were measured in the temperature range from -5 to -27 degrees C using an immersion freezing method. Concentrations spanned up to 3 orders of magnitude, e.g. at -16 degrees C from 0.2 to 100 m(-3). Elevated values (above 10 m(-3) at 16 degrees C) were measured when the research vessel was in the vicinity of land (excluding Antarctica), with lower and more constant concentrations when at sea. This, along with results of backward-trajectory analyses, hints towards terrestrial and/or coastal INP sources being dominant close to ice-free (non-Antarctic) land. In pristine marine areas INPs may originate from both oceanic sources and/or long-range transport. Sampled aerosol particles (PM10) were analysed for sodium and methanesulfonic acid (MSA). Resulting mass concentrations were used as tracers for primary marine and secondary aerosol particles, respectively. Sodium, with an average mass concentration around 2.8 mu gm(-3), was found to dominate the sampled, identified particle mass. MSA was highly variable over the SO, with mass concentrations up to 0.5 mu g m(-3) near the sea ice edge. A correlation analysis yielded strong correlations between sodium mass concentration and particle number concentration in the coarse mode, unsurprisingly indicating a significant contribution of SSA to that mode. CCN number concentration was highly correlated with the number concentration of Aitken and accumulation mode particles. This, together with a lack of correlation between sodium mass and Aitken and accumulation mode number concentrations, underlines the important contribution of non-SSA, probably secondarily formed particles, to the CCN population. INP number concentrations did not significantly correlate with any other measured aerosol physico-chemical parameter.
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