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During the eruption of the Eyjafjallajökull volcano in the south of Iceland in April/May 2010, about 40 Tg of ash mass were emitted into the atmosphere. It was unclear whether volcanic ash particles with <i>d</i> < 10 μm facilitate the glaciation of clouds. Thus, ice nucleation properties of volcanic ash particles were investigated in AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber experiments simulating atmospherically relevant conditions. The ash sample that was used for our experiments had been collected at a distance of 58 km from the Eyjafjallajökull during the eruption period in April 2010. The temperature range covered by our ice nucleation experiments extended from 219 to 264 K, and both ice nucleation via immersion freezing and deposition nucleation could be observed. Immersion freezing was first observed at 252 K, whereas the deposition nucleation onset lay at 242 K and RH<sub>ice</sub> =126%. About 0.1% of the volcanic ash particles were active as immersion freezing nuclei at a temperature of 249 K. For deposition nucleation, an ice fraction of 0.1% was observed at around 233 K and RH<sub>ice</sub> =116%. Taking ice-active surface site densities as a measure for the ice nucleation efficiency, volcanic ash particles are similarly efficient ice nuclei in immersion freezing mode (<i>n</i><sub>s,imm</sub> ~ 10<sup>9</sup> m<sup>−2</sup> at 247 K) compared to certain mineral dusts. For deposition nucleation, the observed ice-active surface site densities <i>n</i><sub>s,dep</sub> were found to be 10<sup>11</sup> m<sup>−2</sup> at 224 K and RH<sub>ice</sub> =116%. Thus, volcanic ash particles initiate deposition nucleation more efficiently than Asian and Saharan dust but appear to be poorer ice nuclei than ATD particles. Based on the experimental data, we have derived ice-active surface site densities as a function of temperature for immersion freezing and of relative humidity over ice and temperature for deposition nucleation.
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In order to improve the surface ozone forecast over Beijing and surrounding regions, data assimilation method integrated into a high-resolution regional air quality model and a regional air quality monitoring network are employed. Several advanced data assimilation strategies based on ensemble Kalman filter are designed to adjust O<sub>3</sub> initial conditions, NO<sub>x</sub> initial conditions and emissions, VOCs initial conditions and emissions separately or jointly through assimilating ozone observations. As a result, adjusting precursor initial conditions demonstrates potential improvement of the 1-h ozone forecast almost as great as shown by adjusting precursor emissions. Nevertheless, either adjusting precursor initial conditions or emissions show deficiency in improving the short-term ozone forecast at suburban areas. Adjusting ozone initial values brings significant improvement to the 1-h ozone forecast, and its limitations lie in the difficulty in improving the 1-h forecast at some urban site. A simultaneous adjustment of the above five variables is found to be able to reduce these limitations and display an overall better performance in improving both the 1-h and 24-h ozone forecast over these areas. The root mean square errors of 1-h ozone forecast at urban sites and suburban sites decrease by 51% and 58% respectively compared with those in free run. Through these experiments, we found that assimilating local ozone observations is determinant for ozone forecast over the observational area, while assimilating remote ozone observations could reduce the uncertainty in regional transport ozone.
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The condensational growth rate of aerosol particles formed in atmospheric new particle formation events is one of the most important factors influencing the lifetime of these particles and their ability to become climatically relevant. Diameter growth rates (GR) of nucleation mode particles were studied based on almost 7 yr of data measured during the years 2003–2009 at a boreal forest measurement station SMEAR II in Hyytiälä, Finland. The particle growth rates were estimated using particle size distributions measured with a Differential Mobility Particle Sizer (DMPS), a Balanced Scanning Mobility Analyzer (BSMA) and an Air Ion Spectrometer (AIS). Two GR analysis methods were tested. The particle growth rates were also compared to an extensive set of ambient meteorological parameters and trace gas concentrations to investigate the processes/constituents limiting the aerosol growth. The median growth rates of particles in the nucleation mode size ranges with diameters of 1.5–3 nm, 3–7 nm and 7–20 nm were 1.9 nm h<sup>−1</sup>, 3.8 nm h<sup>−1</sup>, and 4.3 nm h<sup>−1</sup>, respectively. The median relative uncertainties in the growth rates due to the size distribution instrumentation in these size ranges were 25%, 19%, and 8%, respectively. For the smallest particles (1.5–3 nm) the AIS data yielded on average higher growth rate values than the BSMA data, and higher growth rates were obtained from positively charged size distributions as compared with negatively charged particles. For particles larger than 3 nm in diameter no such systematic differences were found. For these particles the uncertainty in the growth rate related to the analysis method, with relative uncertainty of 16%, was similar to that related to the instruments. The growth rates of 7–20 nm particles showed positive correlation with monoterpene concentrations and their oxidation rate by ozone. The oxidation rate by OH did not show a connection with GR. Our results indicate that the growth of nucleation mode particles in Hyytiälä is mainly limited by the concentrations of organic precursors.
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Secondary new particle formation affects atmospheric aerosol and cloud droplet numbers and thereby, the aerosol effects on climate. In this paper, the frequency of nucleation events and the associated particle formation and growth rates, along with their seasonal variation, was analysed based on over ten years of aerosol measurements conducted at the Pallas GAW station in northern Finland. The long-term measurements also allowed a detailed examination of factors possibly favouring or suppressing particle formation. Effects of meteorological parameters and air mass properties as well as vapour sources and sinks for particle formation frequency and event parameters were inspected. In addition, the potential of secondary particle formation to increase the concentration of cloud condensation nuclei (CCN) sized particles was examined. Findings from these long-term measurements confirmed previous observations: event frequency peaked in spring and the highest growth rates were observed in summer, affiliated with increased biogenic activity. Events were almost exclusively observed in marine air masses on sunny cloud-free days. A low vapour sink by the background particle population as well as an elevated sulphuric acid concentration were found to favour particle formation. These were also conditions taking place most likely in marine air masses. Inter-annual trend showed a minimum in event frequency in 2003, when also the smallest annual median of growth rate was observed. This gives further evidence of the importance and sensitivity of particle formation for the condensing vapour concentrations at Pallas site. The particle formation was observed to increase CCN<sub>80</sub> (>80 nm particle number) concentrations especially in summer and autumn seasons when the growth rates were the highest. When the growing mode exceeded the selected 80 nm limit, on average in those cases, 211 ± 114% increase of CCN<sub>80</sub> concentrations was observed.
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The evolution of organic aerosols (OA) in Mexico City and its outflow is investigated with the nearly explicit gas phase photochemistry model GECKO-A (Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere), wherein precursor hydrocarbons are oxidized to numerous intermediate species for which vapor pressures are computed and used to determine gas/particle partitioning in a chemical box model. Precursor emissions included observed C3-10 alkanes, alkenes, and light aromatics, as well as larger <i>n</i>-alkanes (up to C25) not directly observed but estimated by scaling to particulate emissions according to their volatility. Conditions were selected for comparison with observations made in March 2006 (MILAGRO). The model successfully reproduces the magnitude and diurnal shape for both primary (POA) and secondary (SOA) organic aerosols, with POA peaking in the early morning at 15–20 μg m<sup>−3</sup>, and SOA peaking at 10–15 μg m<sup>−3</sup> during mid-day. The majority (≥75%) of the model SOA stems from reaction products of the large <i>n</i>-alkanes, used here as surrogates for all emitted hydrocarbons of similar volatility, with the remaining SOA originating mostly from the light aromatics. Simulated OA elemental composition reproduces observed H/C and O/C ratios reasonably well, although modeled ratios develop more slowly than observations suggest. SOA chemical composition is initially dominated by δ-hydroxy ketones and nitrates from the large alkanes, with contributions from peroxy acyl nitrates and, at later times when NOx is lower, organic hydroperoxides. The simulated plume-integrated OA mass continues to increase for several days downwind despite dilution-induced particle evaporation, since oxidation chemistry leading to SOA formation remains strong. In this model, the plume SOA burden several days downwind exceeds that leaving the city by a factor of >3. These results suggest significant regional radiative impacts of SOA.
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We describe and evaluate the NMMB/BSC-Dust, a new dust aerosol cycle model embedded online within the NCEP Non-hydrostatic Multiscale Model (NMMB). NMMB is a further evolution of the operational Non-hydrostatic Mesoscale Model (WRF-NMM), which together with other upgrades has been extended from meso to global scales. Its unified non-hydrostatic dynamical core is prepared for regional and global simulation domains. The new NMMB/BSC-Dust is intended to provide short to medium-range weather and dust forecasts from regional to global scales and represents a first step towards the development of a unified chemical-weather model. This paper describes the parameterizations used in the model to simulate the dust cycle including sources, transport, deposition and interaction with radiation. We evaluate monthly and annual means of the global configuration of the model against the AEROCOM dust benchmark dataset for year 2000 including surface concentration, deposition and aerosol optical depth (AOD), and we evaluate the daily AOD variability in a regional domain at high resolution covering Northern Africa, Middle East and Europe against AERONET AOD for year 2006. The NMMB/BSC-Dust provides a good description of the horizontal distribution and temporal variability of the dust. Daily AOD correlations at the regional scale are around 0.6–0.7 on average without dust data assimilation. At the global scale the model lies within the top range of AEROCOM dust models in terms of performance statistics for surface concentration, deposition and AOD. This paper discusses the current strengths and limitations of the modeling system and points towards future improvements.
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Continuous condensation particle (CP) observations were conducted from 1984 through 2009 at Neumayer Station under stringent contamination control. During this period, the CP concentration (median 258 cm<sup>−3</sup>) showed no significant long term trend but exhibited a pronounced seasonality characterized by a stepwise increase starting in September and reaching its annual maximum of around 10<sup>3</sup> cm<sup>−3</sup> in March. Minimum values below 10<sup>2</sup> cm<sup>–3</sup> were observed during June/July. Dedicated time series analyses in the time and frequency domain revealed no significant correlations between inter-annual CP concentration variations and atmospheric circulation indices like Southern Annular Mode (SAM) or Southern Ocean Index (SOI). The impact of the Pinatubo volcanic eruption and strong El Niño events did not affect CP concentrations. From thermodenuder experiments we deduced that the portion of volatile (at 125 °C) and semi-volatile (at 250 °C) particles which could be both associated with biogenic sulfur aerosol, was maximum during austral summer, while during winter non-volatile sea salt particles dominated. During September through April we could frequently observe enhanced concentrations of ultrafine particles within the nucleation mode (between 3 nm and 7 nm particle diameter), preferentially in the afternoon.
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Calculations of the absorptive partitioning of secondary organic aerosol components were carried out using a number of methods to estimate vapour pressure and non-ideality. The sensitivity of predicted condensed component masses, volatility, O:C ratio, molar mass and functionality distribution to the choice of estimation methods was investigated in mixtures of around 2700 compounds generated by a near explicit mechanism of atmospheric VOC degradation. The sensitivities in terms of all metrics were comparable to those previously reported (using 10 000 semi-randomly generated compounds). In addition, the change in predicted aerosol properties and composition with changing VOC emission scenario was investigated showing key dependencies on relative anthropogenic and biogenic contributions. Finally, the contribution of non-ideality to the changing distribution of condensed components was explored in terms of the shift in effective volatility by virtue of component activity coefficients, clearly demonstrating both enhancement and reduction of component masses associated with negative and positive deviations from ideality.
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As a part of EUCAARI activities, the annual cycle of cloud condensation nuclei (CCN) concentrations and critical diameter for cloud droplet activation as a function of supersaturation were measured using a CCN counter and a HTDMA (hygroscopicity tandem differential mobility analyzer) at SMEAR II station, Hyytiälä, Finland. The critical diameters for CCN activation were estimated from (i) the measured CCN concentration and particle size distribution data, and (ii) the hygroscopic growth factors by applying κ-Köhler theory, in both cases assuming an internally mixed aerosol. The critical diameters derived by these two methods were in good agreement with each other. The effect of new particle formation on the diurnal variation of CCN concentration and critical diameters was studied. New particle formation was observed to increase the CCN concentrations by 70–110%, depending on the supersaturation level. The average value for the κ-parameter determined from hygroscopicity measurements was κ = 0.18 and it predicted well the CCN activation in boreal forest conditions in Hyytiälä. The derived critical diameters and κ-parameter confirm earlier findings with other methods, that aerosol particles at CCN sizes in Hyytiälä are mostly organic, but contain also more hygrosopic, probably inorganic salts like ammonium sulphate, making the particles more CCN active than pure secondary organic aerosol.
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The interaction between breezes and synoptic gradient winds, and surface friction increase in transition from sea to land can create persistent convergence zones nearby coastlines. The low level convergence of moist air promotes the dynamical and microphysical processes responsible for the formation of clouds and precipitation. <br><br> Our work focuses on the winter seasons of 1998–2011 in the Eastern Mediterranean. During the winter the Mediterranean sea is usually warmer than the adjacent land, resulting in frequent occurrence of land breeze that opposes the common synoptic winds. Using rain-rate vertical profiles from the Tropical Rainfall Measurement Mission (TRMM) satellite, we examined the spatial and temporal distribution of average hydrometeor mass in clouds as a function of the distance from coastlines. <br><br> Results show that coastlines in the Eastern Mediterranean are indeed favored areas for precipitation formation. The intra-seasonal and diurnal changes in the distribution of hydrometeor mass indicate that the land breeze may likely be the main responsible mechanism behind our results.
