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The Infrared Atmospheric Sounding Interferometer (IASI) is an ultra-spectral satellite sensor with 8461 spectral channels. IASI spectra contain high information content on atmospheric, cloud, and surface properties. The instrument presents a challenge for using thousands of spectral channels in a physical retrieval system or in a Numerical Weather Prediction (NWP) data assimilation system. In this paper we describe a method of simultaneously retrieving atmospheric temperature, moisture, and cloud properties using all available IASI channels without sacrificing computational speed. The essence of the method is to convert the IASI channel radiance spectra into super-channels by an Empirical Orthogonal Function (EOF) transformation. Studies show that about 100 super-channels are adequate to capture the information content of the radiance spectra. A Principal Component-based Radiative Transfer Model (PCRTM) is used to calculate both the super-channel magnitudes and derivatives with respect to atmospheric profiles and other properties. A physical retrieval algorithm then performs an inversion of atmospheric, cloud, and surface properties in the super channel domain directly therefore both reducing the computational need and preserving the information content of the IASI measurements. While no large-scale validation has been performed on any retrieval methodology presented in this paper, comparisons of the retrieved atmospheric profiles, sea surface temperatures, and surface emissivities with co-located ground- and aircraft-based measurements over four days in Spring 2007 over the South-Central United States indicate excellent agreement.
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The hydroxyl radical (OH) is an important oxidant in the troposphere due to its high reactivity and relative abundance. Measuring the concentration of OH in situ, however, is technically challenging. Here we present a simple method of estimating an OH-equivalent oxidant concentration ("effective OH") in the marine boundary layer (MBL) from the mass balance of dimethylsulfide (DMS). We use shipboard eddy covariance measurements of the sea-to-air DMS flux from the Vamos Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) in October and November of 2008. The persistent stratocumulus cloud-cover off the west coast of South America and the associated strong inversion between MBL and the free troposphere (FT) greatly simplify the dynamics in this region and make our budget estimate possible. From the observed diurnal cycle in DMS concentration, the nighttime entrainment velocity at the inversion is estimated to be 4 mm s<sup>−1</sup>. We calculate 1.4(±0.2)×10<sup>6</sup> OH molecules cm<sup>−3</sup> from the DMS budget, which represents a monthly effective concentration and is well within the range of previous estimates. Furthermore, when linearly proportioned according to the intensity of solar flux, the resultant diel OH profile, together with DMS surface and entrainment fluxes, enables us to accurately replicate the observed diurnal cycle in DMS (correlation coefficient over 0.9). The nitrate radical (NO<sub>3</sub>) is found to have little contribution to DMS oxidation during VOCALS-REx. An upper limit estimate of 1 pptv of bromine oxide radical (BrO) would account for 30% of DMS oxidation and lower the OH concentration to 1.0)×10<sup>6</sup> OH molecules cm<sup>−3</sup>. Our effective OH estimate includes the oxidation of DMS by such radicals.
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A method is presented for the evaluation of the exhaust emissions of marine traffic, based on the messages provided by the Automatic Identification System (AIS), which enable the identification and location determination of ships. The use of the AIS data facilitates the positioning of ship emissions with a high spatial resolution, which is limited only by the inaccuracies of the Global Positioning System (typically a few metres) that is used in vessel navigation. The emissions are computed based on the relationship of the instantaneous speed to the design speed, and the detailed technical information of the engines of the ships. The modelling of emissions is also based on a few basic principles of ship design, including the modelling of the propelling power of each vessel in terms of its speed. We have investigated the effect of waves on the consumption of fuel, and on the emissions to the atmosphere. The predictions of fuel consumption were compared with the actual values obtained from the shipowners. For a Roll on – Roll off cargo/passenger ship (RoPax), the predicted and reported values of annual fuel consumption agreed within an accuracy of 6%. According to the data analysis and model computations, the emissions of NO<sub>x</sub>, SO<sub>x</sub> and CO<sub>2</sub> originating from ships in the Baltic Sea during the full calendar year of 2007 were in total 400 kt, 138 kt and 19 Mt, respectively. A breakdown of emissions by flag state, the type of ship and the year of construction is also presented. The modelling system can be used as a decision support tool in the case of issues concerning, e.g., the health effects caused by shipping emissions or the construction of emission-based fairway dues systems or emissions trading. The computation of emissions can be automated, which will save resources in constructing emission inventories. Both the methodologies and the emission computation program can be applied in any sea region in the world, provided that the AIS data from that specific region are available.
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Recently, downscaling global atmospheric model outputs (GCTM) for the USEPA Community Multiscale Air Quality (CMAQ) Initial (IC) and Boundary Conditions (BC) have become practical because of the rapid growth of computational technologies that allow global simulations to be completed within a reasonable time. The traditional method of generating IC/BC by profile data has lost its advocates due to the weakness of the limited horizontal and vertical variations found on the gridded boundary layers. Theoretically, high quality GCTM IC/BC should yield a better result in CMAQ. Unfortunately, several researchers have found that the outputs from GCTM IC/BC are not necessarily better than profile IC/BC due to the excessive transport of O<sub>3</sub> aloft in GCTM IC/BC. In this paper, we intend to investigate the effects of using profile IC/BC and global atmospheric model data. In addition, we are suggesting a novel approach to resolve the existing issue in downscaling. <br><br> In the study, we utilized the GEOS-Chem model outputs to generate time-varied and layer-varied IC/BC for year 2002 with the implementation of tropopause determining algorithm in the downscaling process (i.e., based on chemical (O<sub>3</sub>) tropopause definition). The comparison between the implemented tropopause approach and the profile IC/BC approach is performed to demonstrate improvement of considering tropopause. It is observed that without using tropopause information in the downscaling process, unrealistic O<sub>3</sub> concentrations are created at the upper layers of IC/BC. This phenomenon has caused over-prediction of surface O<sub>3</sub> in CMAQ. In addition, the amount of over-prediction is greatly affected by temperature and latitudinal location of the study domain. With the implementation of the algorithm, we have successfully resolved the incompatibility issues in the vertical layer structure between global and regional chemistry models to yield better surface O<sub>3</sub> predictions than profile IC/BC for both summer and winter conditions. At the same time, it improved the vertical O<sub>3</sub> distribution of CMAQ outputs. It is strongly recommended that the tropopause information should be incorporated into any two-way coupled global and regional models, where the tropospheric regional model is used, to solve the vertical incompatibility that exists between global and regional models.
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Formaldehyde was measured in the area of Milano, Italy, during the 2002 and 2003 FORMAT campaigns at three ground field sites and from an ultralight aircraft. The horizontal distributions show a strong impact of local emissions at a site in the centre of Milano and more photochemically driven diurnal patterns in the remote locations north and south of the city. The mixing ratios in the agricultural areas upwind of Milano were comparable to those downwind indicating the importance of biogenic emissions and anthropogenic agricultural activities. The vertical distributions were dominated by transport processes with advection of CH<sub>2</sub>O above the planetary boundary layer by cloud venting. Comparison to previously published model calculations, based on part of the data set, show discrepancies both, in the diurnal patterns and in the regional distribution which allude to uncertainties in emission inventories.
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This report describes the quality of the Nimbus 7 Limb Infrared Monitor of the Stratosphere (LIMS) water vapor (H<sub>2</sub>O) profiles of 1978/79 that were processed with a Version 6 (V6) algorithm and archived in 2002. The V6 profiles incorporate a better knowledge of the instrument attitude for the LIMS measurements along its orbits, leading to improvements for its temperature profiles and for the registration of its water vapor radiances with pressure. As a result, the LIMS V6 zonal-mean distributions of H<sub>2</sub>O exhibit better hemispheric symmetry than was the case from the original Version 5 (V5) dataset that was archived in 1982. Estimates of the precision and accuracy of the V6 H<sub>2</sub>O profiles are developed and provided. Individual profiles have a precision of order 5% and an estimated accuracy of about 19% at 3 hPa, 14% at 10 hPa, and 26% at 50 hPa. Profile segments within about 2 km of the tropopause are often affected by emissions from clouds that appear in the finite field-of-view of the detector for the LIMS H<sub>2</sub>O channel. Zonally-averaged distributions of the LIMS V6 H<sub>2</sub>O are compared with those from the more recent Microwave Limb Sounder (MLS) satellite experiment for November, February, and May of 2004/05. The patterns and values of their respective distributions are similar in many respects. Effects of a strengthened Brewer-Dobson circulation are indicated in the MLS distributions of the recent decade versus those of LIMS from 1978/79. A tropical tape recorder signal is present in the 7-month time series of LIMS V6 H<sub>2</sub>O with lowest values in February 1979, and the estimated, annually-averaged "entry-level" H<sub>2</sub>O is 3.5 to 3.8 ppmv. It is judged that this historic LIMS water vapor dataset is of good quality for studies of the near global-scale chemistry and transport for pressure levels from 3 hPa to about 70 to 100 hPa.
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Stellar light passing through the Earth atmosphere is affected by refractive effects, which should be taken into account in retrievals from stellar occultation measurements. Scintillation caused by air density irregularities is a nuisance for retrievals of atmospheric composition. In this paper, we consider the influence of scintillation on stellar occultation measurements and on the quality of ozone retrievals from these measurements, based on experience of the GOMOS (Global Ozone Monitoring by Occultation of Stars) instrument on board the Envisat satellite. <br><br> In GOMOS retrievals, the scintillation effect is corrected using scintillation measurements by the fast photometer. We present quantitative estimates of the current scintillation correction quality and of the impact of scintillation on ozone retrievals by GOMOS. The analysis has shown that the present scintillation correction efficiently removes the distortion of transmission spectra caused by scintillations, which are generated by anisotropic irregularities of air density. The impact of errors of dilution and anisotropic scintillation correction on the quality of ozone retrievals is negligible. However, the current scintillation correction is not able to remove the wavelength-dependent distortion of transmission spectra caused by isotropic scintillations, which can be present in off-orbital-plane occultations. This distortion may result in ozone retrieval errors of 0.5–1.5% at altitudes 20–40 km. This contribution constitutes a significant percentage of the total error for bright stars. The advanced inversion methods that can minimize the influence of scintillation correction error are also discussed.
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Bacteria are ubiquitous in the atmosphere, with concentrations of bacterial cells typically exceeding 1×10<sup>4</sup> m<sup>−3</sup> over land. Numerous studies have suggested that the presence of bacteria in the atmosphere may impact cloud development, atmospheric chemistry, and microbial biogeography. A sound knowledge of bacterial concentrations and distributions in the atmosphere is needed to evaluate these claims. This review focusses on published measurements of total and culturable bacteria concentrations in the atmospheric aerosol. We discuss emission mechanisms and the impacts of meteorological conditions and measurement techniques on measured bacteria concentrations. Based on the literature reviewed, we suggest representative values and ranges for the mean concentration in the near-surface air of nine natural ecosystems and three human-influenced land types. We discuss the gaps in current knowledge of bacterial concentrations in air, including the lack of reliable, long-term measurements of the total microbial concentrations in many regions and the scarcity of emission flux measurements.
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Bacteria are constantly being transported through the atmosphere, which may have implications for human health, agriculture, cloud formation, and the dispersal of bacterial species. We simulate the global transport of bacteria, represented as 1 μm and 3 μm diameter spherical solid particle tracers in a general circulation model. We investigate factors influencing residence time and distribution of the particles, including emission region, cloud condensation nucleus activity and removal by ice-phase precipitation. The global distribution depends strongly on the assumptions made about uptake into cloud droplets and ice. The transport is also affected, to a lesser extent, by the emission region, particulate diameter, and season. We find that the seasonal variation in atmospheric residence time is insufficient to explain by itself the observed seasonal variation in concentrations of particulate airborne culturable bacteria, indicating that this variability is mainly driven by seasonal variations in culturability and/or emission strength. We examine the potential for exchange of bacteria between ecosystems and obtain rough estimates of the flux from each ecosystem by using a maximum likelihood estimation technique, together with a new compilation of available observations described in a companion paper. Globally, we estimate the total emissions of bacteria-containing particles to the atmosphere to be 7.6×10<sup>23</sup>–3.5×10<sup>24</sup> a<sup>−1</sup>, originating mainly from grasslands, shrubs and crops. We estimate the mass of emitted bacteria- to be 40–1800 Gg a<sup>−1</sup>, depending on the mass fraction of bacterial cells in the particles. In order to improve understanding of this topic, more measurements of the bacterial content of the air and of the rate of surface-atmosphere exchange of bacteria will be necessary. Future observations in wetlands, hot deserts, tundra, remote glacial and coastal regions and over oceans will be of particular interest.
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We present airborne measurements of carbon dioxide (CO<sub>2</sub>), carbon monoxide (CO), ozone (O<sub>3</sub>), equivalent black carbon (EBC) and ultra fine particles over North-Eastern Siberia in July 2008 performed during the YAK-AEROSIB/POLARCAT experiment. During a "golden day" (11 July 2008) a number of biomass burning plumes were encountered with CO mixing ratio enhancements of up to 500 ppb relative to a background of 90 ppb. Number concentrations of aerosols in the size range 3.5–200 nm peaked at 4000 cm<sup>−3</sup> and the EBC content reached 1.4 μg m<sup>−3</sup>. These high concentrations were caused by forest fires in the vicinity of the landing airport in Yakutsk where measurements in fresh smoke could be made during the descent. We estimate a combustion efficiency of 90 ± 3% based on CO and CO<sub>2</sub> measurements and a CO emission factor of 65.5 ± 10.8 g CO per kilogram of dry matter burned. This suggests a potential increase in the average northern hemispheric CO mixing ratio of 3.0–7.2 ppb per million hectares of Siberian forest burned. For BC, we estimate an emission factor of 0.52 ± 0.07 g BC kg<sup>−1</sup>, comparable to values reported in the literature. The emission ratio of ultra-fine particles (3.5–200 nm) was 26 cm<sup>−3</sup> (ppb CO)<sup>−1</sup>, consistent with other airborne studies. <br><br> The transport of identified biomass burning plumes was investigated using the FLEXPART Lagrangian model. Based on sampling of wildfire plumes from the same source but with different atmospheric ages derived from FLEXPART, we estimate that the e-folding lifetimes of EBC and ultra fine particles (between 3.5 and 200 nm in size) against removal and growth processes are 5.1 and 5.5 days respectively, supporting lifetime estimates used in various modelling studies.