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  • The two-day wave in the Antarctic and Arctic mesosphere and lower thermosphere

    There have been comparatively few studies reported of the 2-day planetary wave in the middle atmosphere at polar latitudes. Here we report on a study made using high-latitude meteor radars at Rothera in the Antarctic (68&deg; S, 68&deg; W) and Esrange in Arctic Sweden (68&deg; N, 21&deg; E). Observations from 2005–2008 are used for Rothera and from 1999–2008 for Esrange. Measurements were made of horizontal winds at heights of 80–100 km. The radar data revealed distinct summertime and wintertime 2-day waves. The Antarctic summertime wave occurs with significant amplitudes in January – February at heights between about 88–100 km. Horizontal wind monthly variances associated with the wave exceed 160 m<sup>2</sup> s<sup>&minus;2</sup> and the zonal component has larger amplitudes than the meridional. In contrast, the Arctic summertime wave occurs for a longer duration, June–August and has meridional amplitudes larger than the zonal amplitudes. The Arctic summertime wave is weaker than that in the Antarctic and maximum monthly variances are typically 60 m<sup>2</sup> s<sup>&minus;2</sup>. In both hemispheres the summertime wave reaches largest amplitudes in the strongly sheared eastward zonal flow above the zero-wind line and is largely absent in the westward flow below. The observed differences in the summertime wave are probably due to the differences in the background zonal winds in the two hemispheres. The Antarctic and Arctic wintertime 2-day waves have very similar behaviour. The Antarctic wave has significant amplitudes in May–August and the Arctic wave in November–February. Both are evident across the full height range observed.
  • The simulation of the Antarctic ozone hole by chemistry-climate models

    While chemistry-climate models are able to reproduce many characteristics of the global total column ozone field and its long-term evolution, they have fared less well in simulating the commonly used diagnostic of the area of the Antarctic ozone hole i.e. the area within the 220 Dobson Unit (DU) contour. Two possible reasons for this are: (1) the underlying Global Climate Model (GCM) does not correctly simulate the size of the polar vortex, and (2) the stratospheric chemistry scheme incorporated into the GCM, and/or the model dynamics, results in systematic biases in the total column ozone fields such that the 220 DU contour is no longer appropriate for delineating the edge of the ozone hole. Both causes are examined here with a view to developing ozone hole area diagnostics that better suit measurement-model inter-comparisons. The interplay between the shape of the meridional mixing barrier at the edge of the vortex and the meridional gradients in total column ozone across the vortex edge is investigated in measurements and in 5 chemistry-climate models (CCMs). Analysis of the simulation of the polar vortex in the CCMs shows that the first of the two possible causes does play a role in some models. This in turn affects the ability of the models to simulate the large observed meridional gradients in total column ozone. The second of the two causes also strongly affects the ability of the CCMs to track the observed size of the ozone hole. It is shown that by applying a common algorithm to the CCMs for selecting a delineating threshold unique to each model, a more appropriate diagnostic of ozone hole area can be generated that shows better agreement with that derived from observations.
  • Impact of tropospheric nitrogen dioxide on the regional radiation budget

    Following the launch of several satellite ultraviolet and visible spectrometers including the Ozone Monitoring Instrument (OMI), much has been learned about the global distribution of nitrogen dioxide (NO<sub>2</sub>). NO<sub>2</sub>, which is mostly anthropogenic in origin, absorbs solar radiation at ultraviolet and visible wavelengths. We parameterized NO<sub>2</sub> absorption for fast radiative transfer calculations. Using this parameterization with cloud, surface, and NO<sub>2</sub> information from different sensors in the NASA A-train constellation of satellites and NO<sub>2</sub> profiles from the Global Modeling Initiative (GMI), we compute the global distribution of net atmospheric heating (NAH) due to tropospheric NO<sub>2</sub> for January and July 2005. The globally-averaged NAH values due to tropospheric NO<sub>2</sub> are very low: they are about 0.05 W/m<sup>2</sup>. While the impact of NO<sub>2</sub> on the global radiative forcing is small, locally it can produce instantaneous net atmospheric heating of 2–4 W/m<sup>2</sup> in heavily polluted areas. We assess the impact of clouds and find that they reduce the globally-averaged NAH values by 5–6% only. However, because most of NO<sub>2</sub> is contained in the boundary layer in polluted regions, the cloud shielding effect can significantly reduce the net atmospheric heating due to tropospheric NO<sub>2</sub> (up to 50%). We examine the effect of diurnal variations in NO<sub>2</sub> emissions and chemistry on net atmospheric heating and find only a small impact of these on the daily-averaged heating (11–14% at the most). We also examine the sensitivity of NO<sub>2</sub> absorption to various geophysical conditions. Effects of the vertical distributions of cloud optical depth and NO<sub>2</sub> on net atmospheric heating and downwelling radiance are simulated in detail for various scenarios including vertically-inhomogeneous convective clouds observed by CloudSat. The maximum effect of NO<sub>2</sub> on downwelling radiance occurs when the NO<sub>2</sub> is located in the middle part of the cloud where the optical extinction peaks.
  • Observations of high rates of NO2-HONO conversion in the nocturnal atmospheric boundary layer in Kathmandu, Nepal

    Nitrous acid (HONO) plays a significant role in the atmosphere, especially in the polluted troposphere. Its photolysis after sunrise is an important source of hydroxyl free radicals (OH). Measurements of nitrous acid and other pollutants were carried out in the Kathmandu urban atmosphere during January–February 2003, contributing to the sparse knowledge of nitrous acid in South Asia. The results showed average nocturnal levels of HONO (1.7&plusmn;0.8 ppbv), NO<sub>2</sub> (17.9&plusmn;10.2 ppbv), and PM<sub>10</sub> (0.18&plusmn;0.11 mg m<sup>&minus;3</sup>) in urban air in Kathmandu. Surprisingly high ratios of chemically formed secondary [HONO] to [NO<sub>2</sub>] (up to 30%) were found, which indicates unexpectedly efficient chemical conversion of NO<sub>2</sub> to HONO in Kathmandu. The ratios of [HONO]/[NO<sub>2</sub>] at night were found to be much higher than previously reported values from measurements in urban air in Europe, North America and Asia. The influences of aerosol surface, ground reactive surface, and relative humidity on NO<sub>2</sub>-HONO chemical conversion were discussed. The high humidity, strong and low inversion layer at night, and high aerosol pollution burden in Kathmandu may explain the particularly efficient conversion of NO<sub>2</sub> to HONO.
  • IASI temperature and water vapor retrievals – error assessment and validation

    The METOP-A satellite Infrared Atmospheric Sounding Interferometer (IASI) Level 2 products comprise retrievals of vertical profiles of temperature and water vapor. The error covariance matrices and biases of the most recent version (4.3.1) of the L2 data were assessed, and the assessment was validated using radiosonde data for reference. The radiosonde data set includes dedicated and synoptic time launches at the Lindenberg station in Germany. For optimal validation, the linear statistical Validation Assessment Model (VAM) was used. The VAM uses radiosonde profiles as input and provides optimal estimate of the nominal IASI retrieval by utilizing IASI averaging kernels and statistical characteristics of the ensembles of the reference radiosondes. For temperatures above 900 mb and water retrievals above 700 mb, level expected and assessed errors are in good agreement. Below those levels, noticeable excess in assessed error is observed, possibly due to inaccurate surface parameters and undetected clouds/haze.
  • A model study of the January 2006 low total ozone episode over Western Europe and comparison with ozone sonde data

    Total column and stratospheric ozone levels at mid-latitudes often reveal strong fluctuations on time scales of days caused by dynamic processes. In some cases the total ozone column is distinctly reduced below climatological values. Here, a very low total ozone episode around 19 January 2006 over Western Europe is investigated when the observed total ozone column over Uccle (BE), measured by a Brewer spectrophotometer, reached a daily minimum of 200 DU, the lowest recorded value at this station. In order to investigate the mechanisms leading to the ozone minimum, the present study used data from (i) six ozone sounding stations in Western and Middle Europe, (ii) ECMWF meteorological fields, (iii) a simulation of the CLaMS model for January 2006, (iv) a multi-year run of the chemistry transport model KASIMA, and (v) a six-year run of the climate chemistry model ECHAM5/MESSy1. The ozone decrease at different heights was quantified and it was determined to what extent different transport mechanisms, and instantaneous, in-situ chemical ozone depletion contributed to the event. All three models reproduced the evolution and formation of the event. The ozone column decrease between &Theta;=300 and 750 K was strongest at Uccle (BE) and De Bilt (NL) with 108 and 103 DU, respectively, and somewhat lower at Hohenpeissenberg (DE), Payerne (CH), Prague (CZ) and Lerwick (UK) with 85, 84, 83 and 74 DU, respectively. This analysis demonstrated that mainly the displacement of the ozone depleted polar vortex contributed to the ozone column decrease. Advection of ozone-poor low-latitude air masses was important in the UTLS region. The vertical displacement of isentropes connected with divergence of air out of the column was found to be of minor importance compared to the horizontal transport processes. Severe low total ozone episodes seem to occur when the mentioned mechanisms are superimposed. Instantaneous, in-situ chemical ozone depletion accounted for only 2&plusmn;1% of the overall total ozone decrease at the sounding stations.
  • Distribution and sources of bioaccumulative air pollutants at Mezquital Valley, Mexico, as reflected by the atmospheric plant Tillandsia recurvata L.

    Mezquital Valley (MV), a Mexican wastewater-based agricultural and industrial region, is a "hot spot" of regulated air pollutants emissions, but the concurrent unregulated ones, like hazardous metals and polycyclic aromatic hydrocarbons (PAH), remain undocumented. A biomonitoring survey with the epiphytic <i>Tillandsia recurvata</i> was conducted there to detect spatial patterns and potential sources of 20 airborne elements and 15 PAH. The natural &delta;<sup>13</sup>C and &delta;<sup>15</sup>N ratios of this plant helped in source identification. The regional mean concentration of most elements was two (Cr) to over 40 times (Ni, Pb, V) higher than reported for <i>Tillandsia</i> in other countries. Eleven elements, pyrene and chrysene had 18–214% higher mean concentration at the industrial south than at the agricultural north of MV. The total quantified PAH (mean, 572 ng g<sup>&minus;1</sup>; range, 143–2568) were composed by medium (65%, phenanthrene to chrysene), low (28%, naphthalene to fluorene) and high molecular weight compounds (7%, Benzo(<i>b</i>)fluoranthene to indeno(1,2,3-<i>cd</i>)pyrene). The &delta;<sup>13</sup>C (mean, &minus;14.6&permil;; range, &minus;15.7&permil; to &minus;13.7&permil;) was consistently lower than &minus;15&permil; near the major petroleum combustion sources. The &delta;<sup>15</sup>N (mean, &minus;3.0&permil;; range, &minus;9.9&permil; to 3.3&permil;) varied from positive at agriculture/industrial areas to negative at rural sites. Factor analysis provided a five-factor solution for 74% of the data variance: 1) crustal rocks, 39.5% (Al, Ba, Cu, Fe, Sr, Ti); 2) soils, 11.3%, contrasting contributions from natural (Mg, Mn, Zn) and saline agriculture soils (Na); 3) cement production and fossil fuel combustion, 9.8% (Ca, Ni, V, chrysene, pyrene); 4) probable agricultural biomass burning, 8.1% (K and benzo(<i>g,h,i</i>)perylene), and 5) agriculture with wastewater, 5.2% (&delta;<sup>15</sup>N and P). These results indicated high deposition of bioaccumulative air pollutants at MV, especially at the industrial area. Since <i>T. recurvata</i> reflected the regional differences in exposition, it is recommended as a biomonitor for comparisons within and among countries where it is distributed: southern USA to Argentina.
  • Analysing spatio-temporal patterns of the global NO2-distribution retrieved from GOME satellite observations using a generalized additive model

    With the increasing availability of observational data from different sources at a global level, joint analysis of these data is becoming especially attractive. For such an analysis – oftentimes with little prior knowledge about local and global interactions between the different observational variables at hand – an exploratory, data-driven analysis of the data may be of particular relevance. <br><br> In the present work we used generalized additive models (GAM) in an exemplary study of spatio-temporal patterns in the tropospheric NO<sub>2</sub>-distribution derived from GOME satellite observations (1996 to 2001) at global scale. We focused on identifying correlations between NO<sub>2</sub> and local wind fields, a quantity which is of particular interest in the analysis of spatio-temporal interactions. Formulating general functional, parametric relationships between the observed NO<sub>2</sub> distribution and local wind fields, however, is difficult – if not impossible. So, rather than following a model-based analysis testing the data for predefined hypotheses (assuming, for example, sinusoidal seasonal trends), we used a GAM with non-parametric model terms to learn this functional relationship between NO<sub>2</sub> and wind directly from the data. <br><br> The NO<sub>2</sub> observations showed to be affected by wind-dominated processes over large areas. We estimated the extent of areas affected by specific NO<sub>2</sub> emission sources, and were able to highlight likely atmospheric transport "pathways". General temporal trends which were also part of our model – weekly, seasonal and linear changes – showed to be in good agreement with previous studies and alternative ways of analysing the time series. Overall, using a non-parametric model provided favorable means for a rapid inspection of this large spatio-temporal NO<sub>2</sub> data set, with less bias than parametric approaches, and allowing to visualize dynamical processes of the NO<sub>2</sub> distribution at a global scale.
  • Technical Note: Determination of aerosol optical properties by a calibrated sky imager

    The calibrated ground-based sky imager developed in the Marine Physical Laboratory, the Whole Sky Imager (WSI), has been tested with data from the Atmospheric Radiation Measurement Program (ARM) at the Southern Great Plain site (SGP) to determine optical properties of the atmospheric aerosol. Different neural network-based models calculate the aerosol optical depth (AOD) for three wavelengths using the radiance extracted from the principal plane of sky images from the WSI as input parameters. The models use data from a CIMEL CE318 photometer for training and validation and the wavelengths used correspond to the closest wavelengths in both instruments. The spectral dependency of the AOD, characterized by the Ångström exponent α in the interval 440–870 nm, is also derived using the standard AERONET procedure and also with a neural network-based model using the values obtained with a CIMEL CE318. The deviations between the WSI derived AOD and the AOD retrieved by AERONET are within the nominal uncertainty assigned to the AERONET AOD calculation (&plusmn;0.01), in 80% of the cases. The explanation of data variance by the model is over 92% in all cases. In the case of α, the deviation is within the uncertainty assigned to the AERONET α (&plusmn;0.1) in 50% of the cases for the standard method and 84% for the neural network-based model. The explanation of data variance by the model is 63% for the standard method and 77% for the neural network-based model.
  • Comparison of a global-climate model simulation to a cloud-system resolving model simulation for long-term thin stratocumulus clouds

    A case of thin, warm marine-boundary-layer (MBL) clouds is simulated by a cloud-system resolving model (CSRM) and is compared to the same case of clouds simulated by a general circulation model (GCM). In this study, the simulation by the CSRM adopts higher resolutions which are generally used in large-eddy simulations (LES) and more advanced microphysics as compared to those by the GCM, enabling the CSRM-simulation to act as a benchmark to assess the simulation by the GCM. Explicitly simulated interactions among the surface latent heat (LH) fluxes, buoyancy fluxes, and cloud-top entrainment lead to the deepening-warming decoupling and thereby the transition from stratiform clouds to cumulus clouds in the CSRM. However, in the simulation by the GCM, these interactions are not resolved and thus the transition to cumulus clouds is not simulated. This leads to substantial differences in liquid water content (LWC) and radiation between simulations by the CSRM and the GCM. When stratocumulus clouds are dominant prior to the transition to cumulus clouds, interactions between supersaturation and cloud droplet number concentration (CDNC) (controlling condensation) and those between rain evaporation and cloud-base instability (controlling cloud dynamics and thereby condensation) determine LWC and thus the radiation budget in the simulation by the CSRM. These interactions result in smaller condensation and thus smaller LWC and reflected solar radiation by clouds in the simulation by the CSRM than in the simulation by the GCM where these interactions are not resolved. The resolved interactions (associated with condensation and the transition to cumulus clouds) lead to better agreement between the CSRM-simulation and observation than that between the GCM-simulation and observation.
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