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Impacts of dust on West African climate during 2005 and 2006

The aim of this study is to understand the impacts of Saharan dust outbreaks on West African climate using a 3-dimensional, hydrostatic, sigma vertical coordinate regional climate model (RegCM). We performed a simulation with the non aerosol version of the model (control case) followed by another simulation using the desert dust module (dust case) implemented in RegCM which includes emission, transport, gravitational settling, wet and dry removal and calculation of dust optical properties for 2005 and 2006. Dynamic and thermodynamic parameters obtained from both versions of the model are intercompared and validated with NCEP/NCAR reanalysis, African Monsoon Multidisciplinary Analysis (AMMA) program data and the Global Precipitation Climatology Project (GPCP) rainfall products. The spatial and temporal distribution of the Aerosol optical depth derived from the desert dust run is compared to available observed aerosol data such as the Aerosol Robotic Network (AERONET) program and satellites data. Using radiosounding data and RegCM outputs, a case study of a strong dust outbreak showed the presence of a stable environment at Dakar, Sal and Nouadhibou stations.
Ice nucleation and cloud microphysical properties in tropical tropopause layer cirrus

In past modeling studies, it has generally been assumed that the predominant mechanism for nucleation of ice in the uppermost troposphere is homogeneous freezing of aqueous aerosols. However, recent in situ and remote-sensing measurements of the properties of cirrus clouds at very low temperatures in the tropical tropopause layer (TTL) are broadly inconsistent with theoretial predictions based on the homogeneous freezing assumption. The nearly ubiquitous occurence of gravity waves in the TTL makes the predictions from homogeneous nucleation theory particularly difficult to reconcile with measurements. These measured properties include ice number concentrations, which are much lower than theory predicts; ice crystal size distributions, which are much broader than theory predicts; and cloud extinctions, which are much lower than theory predicts. Although other explanations are possible, one way to limit ice concentrations is to have on the order of 50 L−1 effective ice nuclei (IN) that could nucleate ice at relatively low supersaturations. We suggest that ammonium sulfate particles, which would be dry much of the time in the cold TTL, are a potential IN candidate for TTL cirrus. However, this mechanism remains to be fully quantified for the size distribution of ammonium sulfate (possibly internally mixed with organics) actually present in the upper troposphere. Possible implications of the observed cloud microphysical properties for ice sedimentation, dehydration, and cloud persistence are also discussed.
Technical Note: Measuring condensation sink and ion sink of atmospheric aerosols with the electrical low pressure impactor (ELPI)

We investigate the suitability of ELPI for condensation sink and ion sink measurements. The aim is to find the simple calibration factors by which the measured ELPI current can be converted to condensation or ion sinks. The calibration is based on DMPS and ELPI measurements within the period 15–25 May 2005 at a boreal forest site in Southern Finland. The values of condensation sink and ion sink were calculated from the DMPS size distributions using their theoretical definitions. After that the values were compared to theoretical and measured ELPI current, and calibration factors were specified. For condensation sink the calibration factor was found to be 7.27E-06 s−1 fA−1 and for ion sink 8.55E-06 s−1 fA−1. Simply by multiplying the total current of the outdoor ELPI by these factors, the values of condensation sink and ion sink can be measured.
Variability of springtime transpacific pollution transport during 2000–2006: the INTEX-B mission in the context of previous years

We analyze the transport of pollution across the Pacific during the NASA INTEX-B (Intercontinental Chemical Transport Experiment Part B) campaign in spring 2006 and examine how this year compares to the time period for 2000 through 2006. In addition to aircraft measurements of carbon monoxide (CO) collected during INTEX-B, we include in this study multi-year satellite retrievals of CO from the Measurements of Pollution in the Troposphere (MOPITT) instrument and simulations from the chemistry transport model MOZART-4. Model tracers are used to examine the contributions of different source regions and source types to pollution levels over the Pacific. Additional modeling studies are performed to separate the impacts of inter-annual variability in meteorology and dynamics from changes in source strength. Interannual variability in the tropospheric CO burden over the Pacific and the US as estimated from the MOPITT data range up to 7% and a somewhat smaller estimate (5%) is derived from the model. When keeping the emissions in the model constant between years, the year-to-year changes are reduced (2%), but show that in addition to changes in emissions, variable meteorological conditions also impact transpacific pollution transport. We estimate that about 1/3 of the variability in the tropospheric CO loading over the contiguous US is explained by changes in emissions and about 2/3 by changes in meteorology and transport. Biomass burning sources are found to be a larger driver for inter-annual variability in the CO loading compared to fossil and biofuel sources or photochemical CO production even though their absolute contributions are smaller. Source contribution analysis shows that the aircraft sampling during INTEX-B was fairly representative of the larger scale region, but with a slight bias towards higher influence from Asian contributions.
Quantitative assessment of Southern Hemisphere ozone in chemistry-climate model simulations

Stratospheric ozone recovery in the Southern Hemisphere is expected to drive pronounced trends in atmospheric temperature and circulation from the stratosphere to the troposphere in the 21st century; therefore ozone changes need to be accounted for in future climate simulations. Many climate models do not have interactive ozone chemistry and rely on prescribed ozone fields, which may be obtained from coupled chemistry-climate model (CCM) simulations. However CCMs vary widely in their predictions of ozone evolution, complicating the selection of ozone boundary conditions for future climate simulations. In order to assess which models might be expected to better simulate future ozone evolution, and thus provide more realistic ozone boundary conditions, we assess the ability of twelve CCMs to simulate observed ozone climatology and trends and rank the models according to their errors averaged across the individual diagnostics chosen. According to our analysis no one model performs better than the others in all the diagnostics; however, combining errors in individual diagnostics into one metric of model performance allows us to objectively rank the models. The multi-model average shows better overall agreement with the observations than any individual model. Based on this analysis we conclude that the multi-model average ozone projection presents the best estimate of future ozone evolution and recommend it for use as a boundary condition in future climate simulations. Our results also demonstrate a sensitivity of the analysis to the choice of reference data set for vertical ozone distribution over the Antarctic, highlighting the constraints that large observational uncertainty imposes on such model verification.
A laboratory based experimental study of mercury emission from contaminated soils in the River Idrijca catchment

Results obtained by a laboratory flux measurement system (LFMS) focused on investigating the kinetics of the mercury emission flux (MEF) from contaminated soils of the Idrija Hg-mine region, Slovenia are presented. Representative soil samples with respect to total Hg concentrations (4–417 μg g−1) and land cover (forest, meadow and alluvial soil) alongside the River Idrijca were analysed to determine the variation in MEF versus distance from the source, regulating three major environmental parameters comprising soil temperature, soil moisture and solar radiation. MEFs ranged from less than 2 to 530 ng m−2 h−1, with the highest emissions from contaminated alluvial soils and soils near the mining district in the town of Idrija. A significant decrease of MEF was then observed with increasing distance from these sites. The results revealed a strong positive effect of all three parameters investigated on momentum MEF. The light-induced flux was shown to be independent of the soil temperature, while the soil aqueous phase seems to be responsible for recharging the pool of mercury in the soil available for both the light- and thermally-induced flux. The overall flux response to simulated environmental conditions depends greatly on the form of Hg in the soil. Higher activation energies are required for the overall process to occur in soils where insoluble cinnabar prevails compared to soils where more mobile Hg forms and forms available for transformation processes are dominant.
Biomass burning aerosol emissions from vegetation fires: particle number and mass emission factors and size distributions

Aerosol emissions from vegetation fires have a large impact on air quality and climate. In this study, we use published experimental data and different fitting procedures to derive dynamic particle number and mass emission factors (EFPN, EFPM) related to the fuel type, burning conditions and the mass of dry fuel burned, as well as characteristic CO-referenced emission ratios (PN/CO, PM/CO). Moreover, we explore and characterize the variability of the particle size distribution of fresh smoke, which is typically dominated by a lognormal accumulation mode with count median diameter around 120 nm (depending on age, fuel and combustion efficiency), and its effect on the relationship between particle number and mass emission factors. For the particle number emission factor of vegetation fires, we found no dependence on fuel type and obtained the following parameterization as a function of modified combustion efficiency (MCE): EFPN=34×1015×(1−MCE) kg−1±1015 kg−1 with regard to dry fuel mass (d.m.). For the fine particle mass emission factors (EFPM) we obtained (86–85×MCE) g kg−1±3 g kg−1 as an average for all investigated fires; (93–90×MCE) g kg−1±4 g kg−1 for forest; (67–65×MCE) g kg−1±2 g kg−1 for savanna; (63–62×MCE) g kg−1±1 g kg−1 for grass. For the PN/CO emission ratio we obtained an average of (34±16) cm−3 ppb−1 exhibiting no systematic dependence on fuel type or combustion efficiency. The average PM/CO emission ratios were (0.09±0.04) g g−1 for all investigated fires; (0.13±0.05) g g−1 for forest; (0.08±0.03) g g−1 for savanna; and (0.07±0.03) g g−1 for grass. The results are consistent with each other, given that particles from forest fires are on average larger than those from savanna and grass fires. This assumption and the above parameterizations represent the current state of knowledge, but they are based on a rather limited amount of experimental data which should be complemented by further measurements. Nevertheless, the presented parameterizations appear sufficiently robust for exploring the influence of vegetation fires on aerosol particle number and mass concentrations in regional and global model studies.
Measurements of OH and HO2 yields from the gas phase ozonolysis of isoprene

The reactions of ozone with alkenes are an important source of hydroxyl (OH) radicals; however, quantification of their importance is hindered by uncertainties in the absolute OH yield. Hydroxyl radical yields for the gas-phase ozonolysis of isoprene are determined in this paper by four different methods: (1) The use of cyclohexane as an OH scavenger, and the production of cyclohexanone, (2) The use of 1,3,5-trimethylbenzene as an OH tracer, and the diminution in its concentration, (3) A kinetic method in which the OH yield was obtained by performing a series of pseudo-first-order experiments in the presence or absence of an OH scavenger (cyclohexane), (4) The OH and HO2 yields were determined by fitting the temporal OH and HO2 profiles following direct detection of absolute OH and HO2 concentrations by laser induced fluorescence at low pressure (Fluorescence Assay by Gas Expansion- FAGE). The following OH yields for the ozonolysis of isoprene were obtained, relative to alkene consumed, for each method: (1) Scavenger (0.25±0.04), (2) Tracer (0.25±0.03), (3) Kinetic study (0.27±0.02), and (4) Direct observation (0.26±0.02), the error being one standard deviation. An averaged OH yield of 0.26±0.02 is recommended at room temperature and atmospheric pressure and this result is compared with recent literature determinations. The HO2 yield was directly determined for the first time using FAGE to be 0.26±0.03.
The 16-day wave in the Arctic and Antarctic mesosphere and lower thermosphere

The 16-day planetary wave in the polar mesosphere and lower thermosphere has been investigated using meteor radars at Esrange (68° N, 21° E) in the Arctic and Rothera (68° S, 68° W) in the Antarctic. The measurements span the 10-year interval from October 1999 to July 2009 and the 5-year interval February 2005 to July 2009, respectively. The height range covered is about 80–100 km. In both polar regions the wave is seen to occur in intermittent bursts, where wave amplitudes typically reach a maximum of about 15 m s−1, and never more than about 20 m s−1. Horizontal wind variance within a wave-period range of 12 to 20 days is used as a proxy for the activity of the 16-day wave. Wave activity is strong for 3 to 4 months in winter, where it is present across the entire height range observed and monthly wave variance reaches about 65 m2 s−2. Some weak and intermittent activity is observed throughout the other seasons including summer. However, there is a high degree of inter-annual variability and in some individual years wave activity is almost absent. The data are used to construct a representative climatology for the Arctic and Antarctic. The seasonal cycle of the 16-day wave is found to be very similar in both polar regions. The 16-day wave has slightly greater amplitudes in the zonal component of the winds than in the meridional. Mesospheric temperatures measured by the radars were used to further investigate the 16-day wave. The temperatures reveal a clear signature of the 16-day wave. Temperature amplitudes are generally only a few Kelvin but occasional bursts of up to 10 K have been observed. Observations of the wave in summer are sometimes consistent with the suggestion of ducting from the winter hemisphere.
A review of natural aerosol interactions and feedbacks within the Earth system

The natural environment is a major source of atmospheric aerosols, including dust, secondary organic material from terrestrial biogenic emissions, carbonaceous particles from wildfires, and sulphate from marine phytoplankton dimethyl sulphide emissions. These aerosols also have a significant effect on many components of the Earth system such as the atmospheric radiative balance and photosynthetically available radiation entering the biosphere, the supply of nutrients to the ocean, and the albedo of snow and ice. The physical and biological systems that produce these aerosols can be highly susceptible to modification due to climate change so there is the potential for important climate feedbacks. We review the impact of these natural systems on atmospheric aerosol based on observations and models, including the potential for long term changes in emissions and the feedbacks on climate. The number of drivers of change is very large and the various systems are strongly coupled. There have therefore been very few studies that integrate the various effects to estimate climate feedback factors. Nevertheless, available observations and model studies suggest that the regional radiative perturbations are potentially several Watts per square metre due to changes in these natural aerosol emissions in a future climate. Taking into account only the direct radiative effect of changes in the atmospheric burden of natural aerosols, and neglecting potentially large effects on other parts of the Earth system, a global mean radiative perturbation approaching 1 W m−2 is possible by the end of the century. The level of scientific understanding of the climate drivers, interactions and impacts is very low.