Items

Advanced search

Mesoscale modeling of smoke transport over the Southeast Asian Maritime Continent: coupling of smoke direct radiative effect below and above the low-level clouds

The online-coupled Weather Research and Forecasting model with Chemistry (WRF-Chem) is used to simulate the direct and semi-direct radiative impacts of smoke particles over the Southeast Asian Maritime Continent (MC, 10° S–10° N, 90–150° E) during October 2006 when a significant El Niño event caused the highest biomass burning activity since 1997. With the use of an OC (organic carbon) / BC (black carbon) ratio of 10 in the smoke emission inventory, the baseline simulation shows that the clouds can reverse the negative smoke forcing in cloud-free conditions to a positive value. The net absorption of the atmosphere is largely enhanced when smoke resides above a cloud. This led to a warming effect at the top of the atmosphere (TOA) with a domain and monthly average forcing value of ~ 20 W m−2 over the islands of Borneo and Sumatra. Smoke-induced monthly average daytime heating (0.3 K) is largely confined above the low-level clouds, and results in a local convergence over the smoke source region. This heating-induced convergence transports more smoke particles above the planetary boundary layer height (PBLH), hence rendering a positive effect. This positive effect contrasts with a decrease in the cloud fraction resulting from the combined effects of smoke heating within the cloud layer and the more stable boundary layer; the latter can be considered as a negative effect in which a decrease of the cloud fraction weakens the heating by smoke particles above the clouds. During the nighttime, the elevated smoke layer lying above the clouds in the daytime is decoupled from the boundary layer, and the enhanced downdraft and shallower boundary layer lead to the accumulation of smoke particles near the surface. Because of monthly smoke radiative extinction, the amount of solar input at the surface is reduced by as much as 60 W m−2, which leads to a decrease in sensible heat, latent heat, 2 m air temperature, and PBLH by a maximum of 20 W m−2, 20 W m−2, 1 K, and 120 m, respectively. During daytime, the cloud changes over continents mostly occur over the islands of Sumatra and Borneo where the low-level cloud fraction decreases more than 10%. However, the change of local wind, including sea breeze, induced by the smoke direct radiative effect leads to more convergence over the Karimata Strait and the south coastal area of Kalimantan during both daytime and nighttime; consequently, the cloud fraction there is increased up to 20%. The sensitivities with different OC / BC ratios show the importance of the smoke single-scattering albedo for the smoke semi-direct effects. Lastly, a conceptual model is used to summarize the responses of clouds, smoke, temperature, and water vapor fields to the coupling of smoke direct effect below and above clouds over the Southeast Asian Maritime Continent.
Model study on the dependence of primary marine aerosol emission on the sea surface temperature

Primary marine aerosol composed of sea salt and organic material is an important contributor to the global aerosol load. By comparing measurements from two EMEP (co-operative programme for monitoring and evaluation of the long-range transmissions of air-pollutants in Europe) intensive campaigns in June 2006 and January 2007 with results from an atmospheric transport model this work shows that accounting for the influence of the sea surface temperature on the emission of primary marine aerosol improves the model results towards the measurements in both months. Different sea surface temperature dependencies were evaluated. Using correction functions based on Sofiev et al. (2011) and Jaeglé et al. (2011) improves the model results for coarse mode particles. In contrast, for the fine mode aerosols no best correction function could be found. The model captures the low sodium concentrations at the marine station Virolahti II (Finland), which is influenced by air masses from the low salinity Baltic Sea, as well as the higher concentrations at Cabauw (Netherlands) and Auchencorth Moss (Scotland). These results indicate a shift towards smaller sizes with lower salinity for the emission of dry sea salt aerosols. Organic material was simulated as part of primary marine aerosol assuming an internal mixture with sea salt. A comparison of the model results for primary organic carbon with measurements by a Berner-impactor at Sao Vincente (Cape Verde) indicated that the model underpredicted the observed organic carbon concentration. This leads to the conclusion that the formation of secondary organic material needs to be included in the model to improve the agreement with the measurements.
Combined assimilation of IASI and MLS observations to constrain tropospheric and stratospheric ozone in a global chemical transport model

Accurate and temporally resolved fields of free-troposphere ozone are of major importance to quantify the intercontinental transport of pollution and the ozone radiative forcing. We consider a global chemical transport model (MOdèle de Chimie Atmosphérique à Grande Échelle, MOCAGE) in combination with a linear ozone chemistry scheme to examine the impact of assimilating observations from the Microwave Limb Sounder (MLS) and the Infrared Atmospheric Sounding Interferometer (IASI). The assimilation of the two instruments is performed by means of a variational algorithm (4D-VAR) and allows to constrain stratospheric and tropospheric ozone simultaneously. The analysis is first computed for the months of August and November 2008 and validated against ozonesonde measurements to verify the presence of observations and model biases. Furthermore, a longer analysis of 6 months (July–December 2008) showed that the combined assimilation of MLS and IASI is able to globally reduce the uncertainty (root mean square error, RMSE) of the modeled ozone columns from 30 to 15% in the upper troposphere/lower stratosphere (UTLS, 70–225 hPa). The assimilation of IASI tropospheric ozone observations (1000–225 hPa columns, TOC – tropospheric O3 column) decreases the RMSE of the model from 40 to 20% in the tropics (30° S–30° N), whereas it is not effective at higher latitudes. Results are confirmed by a comparison with additional ozone data sets like the Measurements of OZone and wAter vapour by aIrbus in-service airCraft (MOZAIC) data, the Ozone Monitoring Instrument (OMI) total ozone columns and several high-altitude surface measurements. Finally, the analysis is found to be insensitive to the assimilation parameters. We conclude that the combination of a simplified ozone chemistry scheme with frequent satellite observations is a valuable tool for the long-term analysis of stratospheric and free-tropospheric ozone.
Corrigendum to "Chemical characterization and source apportionment of PM2.5 in Beijing: seasonal perspective" published in Atmos. Chem. Phys., 13, 7053–7074, 2013
Field measurements of trace gases emitted by prescribed fires in southeastern US pine forests using an open-path FTIR system

We report trace-gas emission factors from three pine-understory prescribed fires in South Carolina, US measured during the fall of 2011. The fires were more intense than many prescribed burns because the fuels included mature pine stands not subjected to prescribed fire in decades that were lit following an extended drought. Emission factors were measured with a fixed open-path Fourier transform infrared (OP-FTIR) system that was deployed on the fire control lines. We compare these emission factors to those measured with a roving, point sampling, land-based FTIR and an airborne FTIR deployed on the same fires. We also compare to emission factors measured by a similar OP-FTIR system deployed on savanna fires in Africa. The data suggest that the method used to sample smoke can strongly influence the relative abundance of the emissions that are observed. The majority of fire emissions were lofted in the convection column and were sampled by the airborne FTIR. The roving, ground-based, point sampling FTIR measured the contribution of individual residual smoldering combustion fuel elements scattered throughout the burn site. The OP-FTIR provided a ~ 30 m path-integrated sample of emissions transported to the fixed path via complex ground-level circulation. The OP-FTIR typically probed two distinct combustion regimes, "flaming-like" (immediately after adjacent ignition and before the adjacent plume achieved significant vertical development) and "smoldering-like." These two regimes are denoted "early" and "late", respectively. The path-integrated sample of the ground-level smoke layer adjacent to the fire from the OP-FTIR provided our best estimate of fire-line exposure to smoke for wildland fire personnel. We provide a table of estimated fire-line exposures for numerous known air toxics based on synthesizing results from several studies. Our data suggest that peak exposures are more likely to challenge permissible exposure limits for wildland fire personnel than shift-average (8 h) exposures.
Direct estimation of the rate constant of the reaction ClO + HO2 → HOCl + O2 from SMILES atmospheric observations

Diurnal variations of ClO, HO2, and HOCl were simultaneously observed by the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) between 12 October 2009 and 21 April 2010. These were the first global observations of the diurnal variation of HOCl in the upper atmosphere. A major reaction for the production of HOCl is ClO + HO2 → HOCl + O2 (Reaction (R1)) in extra-polar regions. A model study suggested that in the mesosphere, this is the only reaction influencing the amount of HOCl during the night. The evaluation of the pure reaction period, when only Reaction (R1) occurred in the Cly chemical system, was performed by checking the consistency of the HOCl production rate with the ClO loss rate from SMILES observation data. It turned out that the SMILES data at the pressure level of 0.28 hPa (about 58 km) in the autumn mid-latitude region (20–40°, February–April 2010) during night (between modified local time 18:30 and 04:00) were suitable for the estimation of the rate constant, k1. The rate constant obtained from SMILES observations was k1(245 K) = (7.75 ± 0.25) × 10−12 cm3 molecule−1 s−1. This result is consistent with results from a laboratory experiment and ab initio calculations for similar low-pressure conditions.
Heterogeneous reaction of N2O5 with illite and Arizona test dust particles

The heterogeneous reaction of N2O5 with airborne illite and Arizona test dust (ATD) particles was investigated at room temperature and at different relative humidities using an atmospheric pressure aerosol flow tube. N2O5 at concentrations in the range 8 to 24 × 1012 molecule cm−3 was monitored using thermal-dissociation cavity ring-down spectroscopy at 662 nm. At zero relative humidity a large uptake coefficient of N2O5 to illite was obtained, γ(N2O5) = 0.09, which decreased to 0.04 as relative humidity was increased to 67%. In contrast, the uptake coefficient derived for ATD is much lower (~0.006) and displays a weaker (if any) dependence on relative humidity (0–67%). Potential explanations are given for the significant differences between the uptake behaviour for ATD and illite and the results are compared with uptake coefficients for N2O5 on other mineral surfaces.
Global stratospheric fluorine inventory for 2004–2009 from Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) measurements and SLIMCAT model simulations

Fluorine-containing species can be extremely effective atmospheric greenhouse gases. We present fluorine budgets using organic and inorganic species retrieved by the ACE-FTS satellite instrument supplemented with output from the SLIMCAT 3-D chemical transport model. The budgets are calculated between 2004 and 2009 for a number of latitude bands: 70–30° N, 30–00° N, 00° N–30° S, and 30–70° S. At lower altitudes total fluorine profiles are dominated by the contribution from CFC-12, up to an altitude of 20 km in the extra-tropics and 29 km in the tropics; above these altitudes the profiles are dominated by hydrogen fluoride (HF). Our data show that total fluorine profiles at all locations have a negative slope with altitude, providing evidence that overall fluorine emissions (measured by their F content) have been increasing with time. Total stratospheric fluorine is increasing at a similar rate in the tropics: 32.5 ± 4.9 ppt yr−1 (1.31 ± 0.20% per year) in the Northern Hemisphere (NH) and 29.8 ± 5.3 ppt yr−1 (1.21 ± 0.22% per year) in the Southern Hemisphere (SH). Extra-tropical total stratospheric fluorine is also increasing at a similar rate in both the NH and SH: 28.3 ± 2.7 ppt per year (1.12 ± 0.11% per year) in the NH and 24.3 ± 3.1 ppt per year (0.96 ± 0.12% per year) in the SH. The calculation of radiative efficiency-weighted total fluorine allows the changes in radiative forcing between 2004 and 2009 to be calculated. These results show an increase in radiative forcing of between 0.23 ± 0.11% per year and 0.45 ± 0.11% per year, due to the increase in fluorine-containing species during this time. The decreasing trends in the mixing ratios of halons and chlorofluorocarbons (CFCs), due to their prohibition under the Montreal Protocol, have suppressed an increase in total fluorine caused by increasing mixing ratios of hydrofluorocarbons (HFCs). This has reduced the impact of fluorine-containing species on global warming.
Airborne measurements of gas and particle pollutants during CAREBeijing-2008

Measurements of gaseous pollutants – including ozone (O3), sulfur dioxide (SO2), nitrogen oxides (NOX = NO + NO2), carbon monoxide (CO), particle number concentrations (5.6–560 nm and 0.47–30 μm) – and meteorological parameters (T, RH, P) were conducted during the Campaigns of Air Quality Research in Beijing and Surrounding Regions in 2008 (CAREBeijing-2008), from 27 August through 13 October 2008. The data from a total 18 flights (70 h flight time) from near the surface to 2100 m altitude were obtained with a Yun-12 aircraft in the southern surrounding areas of Beijing (38–40° N, 114–118° E). The objectives of these measurements were to characterize the regional variation of air pollution during and after the Olympics of 2008, determine the importance of air mass trajectories and to evaluate of other factors that influence the pollution characteristics. The results suggest that there are primarily four distinct sources that influenced the magnitude and properties of the pollutants in the measured region based on back-trajectory analysis: (1) southerly transport of air masses from regions with high pollutant emissions, (2) northerly and northeasterly transport of less pollutant air from further away, (3) easterly transport from maritime sources where emissions of gaseous pollutant are less than from the south but still high in particle concentrations, and (4) the transport of air that is a mixture from different regions; that is, the air at all altitudes measured by the aircraft was not all from the same sources. The relatively long-lived CO concentration is shown to be a possible transport tracer of long-range transport from the northwesterly direction, especially at the higher altitudes. Three factors that influenced the size distribution of particles – i.e., air mass transport direction, ground source emissions and meteorological influences – are also discussed.
Antarctic ozone variability inside the polar vortex estimated from balloon measurements

Thirteen years of ozone soundings at the Antarctic Belgrano II station (78° S, 34.6° W) have been analysed to establish a climatology of stratospheric ozone and temperature over the area. The station is inside the polar vortex during the period of development of chemical ozone depletion. Weekly periodic profiles provide a suitable database for seasonal characterization of the evolution of stratospheric ozone, especially valuable during wintertime, when satellites and ground-based instruments based on solar radiation are not available. The work is focused on ozone loss rate variability (August–October) and its recovery (November–December) at different layers identified according to the severity of ozone loss. The time window selected for the calculations covers the phase of a quasi-linear ozone reduction, around day 220 (mid-August) to day 273 (end of September). Decrease of the total ozone column over Belgrano during spring is highly dependent on the meteorological conditions. Largest depletions (up to 59%) are reached in coldest years, while warm winters exhibit significantly lower ozone loss (20%). It has been found that about 11% of the total O3 loss, in the layer where maximum depletion occurs, takes place before sunlight has arrived, as a result of transport to Belgrano of air from a somewhat lower latitude, near the edge of the polar vortex, providing evidence of mixing inside the vortex. Spatial homogeneity of the vortex has been examined by comparing Belgrano results with those previously obtained for South Pole station (SPS) for the same altitude range and for 9 yr of overlapping data. Results show more than 25% higher ozone loss rate at SPS than at Belgrano. The behaviour can be explained taking into account (i) the transport to both stations of air from a somewhat lower latitude, near the edge of the polar vortex, where sunlight reappears sooner, resulting in earlier depletion of ozone, and (ii) the accumulated hours of sunlight, which become much greater at the South Pole after the spring equinox. According to the variability of the ozone hole recovery, a clear connection between the timing of the breakup of the vortex and the monthly ozone content was found. Minimum ozone concentration of 57 DU in the 12–24 km layer remained in November, when the vortex is more persistent, while in years when the final stratospheric warming took place "very early", mean integrated ozone rose by up to 160–180 DU.