Atmosphere2014, 5(3), 518-535; doi:10.3390/atmos5030518 - published online 29 July 2014 Show/Hide Abstract
Abstract: Ozone and methane are chemically active climate-forcing agents affected by climate–chemistry interactions in the atmosphere. Key chemical reactions and processes affecting ozone and methane are presented. It is shown that climate-chemistry interactions have a significant impact on the two compounds. Ozone, which is a secondary compound in the atmosphere, produced and broken down mainly in the troposphere and stratosphre through chemical reactions involving atomic oxygen (O), NOx compounds (NO, NO2), CO, hydrogen radicals (OH, HO2), volatile organic compounds (VOC) and chlorine (Cl, ClO) and bromine (Br, BrO). Ozone is broken down through changes in the atmospheric distribution of the afore mentioned compounds. Methane is a primary compound emitted from different sources (wetlands, rice production, livestock, mining, oil and gas production and landfills).Methane is broken down by the hydroxyl radical (OH). OH is significantly affected by methane emissions, defined by the feedback factor, currently estimated to be in the range 1.3 to 1.5, and increasing with increasing methane emission. Ozone and methane changes are affected by NOx emissions. While ozone in general increase with increases in NOx emission, methane is reduced, due to increases in OH. Several processes where current and future changes have implications for climate-chemistry interactions are identified. It is also shown that climatic changes through dynamic processes could have significant impact on the atmospheric chemical distribution of ozone and methane, as we can see through the impact of Quasi Biennial Oscillation (QBO). Modeling studies indicate that increases in ozone could be more pronounced toward the end of this century. Thawing permafrost could lead to important positive feedbacks in the climate system. Large amounts of organic material are stored in the upper layers of the permafrost in the yedoma deposits in Siberia, where 2 to 5% of the deposits could be organic material. During thawing of permafrost, parts of the organic material that is deposited could be converted to methane. Furthermore, methane stored in deposits under shallow waters in the Arctic have the potential to be released in a future warmer climate with enhanced climate impact on methane, ozone and stratospheric water vapor. Studies performed by several groups show that the transport sectors have the potential for significant impacts on climate-chemistry interactions. There are large uncertainties connected to ozone and methane changes from the transport sector, and to methane release and climate impact during permafrost thawing.
Atmosphere2014, 5(3), 484-517; doi:10.3390/atmos5030484 - published online 24 July 2014 Show/Hide Abstract
Abstract: This paper examines different distribution functions used in a three-moment parameterization scheme with regard to their influence on the implementation and the results of the parameterization scheme. In parameterizations with moment methods, the prognostic variables are interpreted as statistical moments of a drop size distribution, for which a functional form has to be assumed. In cloud microphysics, parameterizations are frequently based on gamma- and log-normal distributions, while for particle-laden flows in engineering, the beta-distribution is sometimes used. In this study, the three-moment schemes with beta-, gamma- and log-normal distributions are tested in a 1D framework for drop sedimentation, and their results are compared with those of a spectral reference model. The gamma-distribution performs best. The results of the parameterization with the beta- and the log-normal distribution have less similarity to the reference solution, particularly with regard to number density and rain rate. Theoretical considerations reveal that (depending on the type of the distribution function) only selected combinations of moments can be predicted together. Among these is the important combination of “number density, liquid water content, radar reflectivity” for all three distributions. Advection or source/sink terms can only be calculated under certain conditions on the moment values (positivity of the Hankel–Hadamard determinant). These are derived from mathematical theory (“moment problem”) and are more restrictive for three-moment than for two-moment schemes.
Atmosphere2014, 5(3), 473-483; doi:10.3390/atmos5030473 - published online 17 July 2014 Show/Hide Abstract
Abstract: CFC-113a (CF3CCl3), CFC-112 (CFCl2CFCl2) and HCFC-133a (CF3CH2Cl) are three newly detected molecules in the atmosphere that are almost certainly emitted as a result of human activity. It is important to characterise the possible contribution of these gases to radiative forcing of climate change and also to provide information on the CO2-equivalence of their emissions. We report new laboratory measurements of absorption cross-sections of these three compounds at a resolution of 0.01 cm−1 for two temperatures 250 K and 295 K in the spectral range of 600–1730 cm−1. These spectra are then used to calculate the radiative efficiencies and global warming potentials (GWP). The radiative efficiencies are found to be between 0.15 and 0.3 W∙m−2∙ppbv−1. The GWP for a 100 year time horizon, relative to carbon dioxide, ranges from 340 for the relatively short-lived HCFC-133a to 3840 for the longer-lived CFC-112. At current (2012) concentrations, these gases make a trivial contribution to total radiative forcing; however, the concentrations of CFC-113a and HCFC-133a are continuing to increase. The 2012 CO2-equivalent emissions, using the GWP (100), are estimated to be about 4% of the current global CO2-equivalent emissions of HFC-134a.
Atmosphere2014, 5(2), 454-472; doi:10.3390/atmos5020454 - published online 18 June 2014 Show/Hide Abstract
Abstract: The aim of our study is to estimate the parameters M (water content), R (rain rate) and Z (radar reflectivity) with raindrop size distribution by using the neural network method. Our investigations have been conducted in five African localities: Abidjan (Côte d’Ivoire), Boyele (Congo-Brazzaville), Debuncha (Cameroon), Dakar (Senegal) and Niamey (Niger). For the first time, we have predicted the values of the various parameters in each locality after using neural models (LANN) which have been developed with locally obtained disdrometer data. We have shown that each LANN can be used under other latitudes to get satisfactory results. Secondly, we have also constructed a model, using as train-data, a combination of data issued from all five localities. With this last model called PANN, we could obtain satisfactory estimates forall localities. Lastly, we have distinguished between stratiform and convective rain while building the neural networks. In fact, using simulation data from stratiform rain situations, we have obtained smaller root mean square errors (RMSE) between neural values and disdrometer values than using data issued from convective situations.
Atmosphere2014, 5(2), 435-453; doi:10.3390/atmos5020435 - published online 16 June 2014 Show/Hide Abstract
Abstract: Samples of PM10 and PM2.5 were collected discontinuously between 2003 and 2010 at fifteen monitoring sites (urban, background, industrial) in the south-eastern part of Italy using a mobile laboratory. In total, 483 PM10 and 154 PM2.5 samples were collected and chemically analyzed for the determination of metal content. Data were used to investigate concentration differences among the typologies of sites, the seasonal patterns, and the influence of advection of Saharan dust (SD). PM10 and PM2.5 average concentrations increase from background to industrial and urban sites but the ratio PM2.5/PM10 is significantly lower (0.61 ± 0.10) in background sites. The average metals concentrations in PM10 and in PM2.5 do not show a clear dependence on site typology apart an increase in crustal elements in background sites and an increase in the enrichment factors of Ni and of Cr in PM10 in industrial sites. Urban sites show a statistically significant increase of PM10 average concentration during the cold seasons (autumn and winter), likely associated with the anthropogenic urban emissions, instead, the background sites show a decrease in concentrations during the cold seasons. This could be due to more frequent cases of SD observed in spring and summer periods that mainly influence background sites. The seasonal difference on the average concentration for industrial sites is not statistically significant. The SD cases influence both PM10 and PM2.5 concentrations but their effect is significantly larger on PM10. Over the studied area, the effect is relatively limited on long-term average PM10 (estimated increase of 3.2%) and PM2.5 (estimated increase of 1.5%) concentrations but it is significant on daily concentrations. It is estimated an increase of 22% of the probability to overcome the air quality standard daily threshold for PM10.
Atmosphere2014, 5(2), 420-434; doi:10.3390/atmos5020420 - published online 4 June 2014 Show/Hide Abstract
Abstract: The first observations of the feedstocks, CFC-216ba (1,2-dichlorohexafluoropropane) and CFC-216ca (1,3-dichlorohexafluoropropane), as well as the CFC substitute HCFC-225ca (3,3-dichloro-1,1,1,2,2-pentafluoropropane), are reported in air samples collected between 1978 and 2012 at Cape Grim, Tasmania. Present day (2012) mixing ratios are 37.8 ± 0.08 ppq (parts per quadrillion; 1015) and 20.2 ± 0.3 ppq for CFC-216ba and CFC-216ca, respectively. The abundance of CFC-216ba has been approximately constant for the past 20 years, whilst that of CFC-216ca is increasing, at a current rate of 0.2 ppq/year. Upper tropospheric air samples collected in 2013 suggest a further continuation of this trend. Inferred annual emissions peaked 421 at 0.18 Gg/year (CFC-216ba) and 0.05 Gg/year (CFC-216ca) in the mid-1980s and then decreased sharply as expected from the Montreal Protocol phase-out schedule for CFCs. The atmospheric trend of CFC-216ca and CFC-216ba translates into continuing emissions of around 0.01 Gg/year in 2011, indicating that significant banks still exist or that they are still being used. HCFC-225ca was not detected in air samples collected before 1992. The highest mixing ratio of 52 ± 1 ppq was observed in 2001. Increasing annual emissions were found in the 1990s (i.e., when HCFC-225ca was being introduced as a replacement for CFCs). Emissions peaked around 1999 at about 1.51 Gg/year. In accordance with the Montreal Protocol, restrictions on HCFC consumption and the short lifetime of HCFC-225ca, mixing ratios declined after 2001 to 23.3 ± 0.7 ppq by 2012.