Megacities are immense sources of air pollutants, with large impacts on air quality and climate. However, emission inventories in many of them still are highly uncertain, particularly in developing countries. Satellite observations allow top-down estimates of emissions to be made for nitrogen oxides (NO(x) = NO + NO(2)), but require poorly quantified a priori information on the NO(x) lifetime. We present a method for the simultaneous determination of megacity NO(x) emissions and lifetimes from satellite measurements by analyzing the downwind patterns of NO(2) separately for different wind conditions. Daytime lifetimes are ~4 hours at low and mid-latitudes, but ~8 hours in wintertime for Moscow. The derived NO(x) emissions are generally in good agreement with existing emission inventories, but are higher by a factor of 3 for the Saudi Arabian capital Riyadh.
During springtime in the polar regions, unique photochemistry converts inert halide salt ions (e.g. Br⁻) into reactive halogen species (e.g. Br atoms and BrO) that deplete ozone in the boundary layer to near zero levels. Since their discovery in the late 1980s, research on ozone depletion events (ODEs) has made great advances; however many key processes remain poorly understood. In this article we review the history, chemistry, dependence on environmental conditions, and impacts of ODEs. This research has shown the central role of bromine photochemistry, but how salts are transported from the ocean and are oxidized to become reactive halogen species in the air is still not fully understood. Halogens other than bromine (chlorine and iodine) are also activated through incompletely understood mechanisms that are probably coupled to bromine chemistry. The main consequence of halogen activation is chemical destruction of ozone, which removes the primary precursor of atmospheric oxidation, and generation of reactive halogen atoms/oxides that become the primary oxidizing species. The different reactivity of halogens as compared to OH and ozone has broad impacts on atmospheric chemistry, including near complete removal and deposition of mercury, alteration of oxidation fates for organic gases, and export of bromine into the free troposphere. Recent changes in the climate of the Arctic and state of the Arctic sea ice cover are likely to have strong effects on halogen activation and ODEs; however, more research is needed to make meaningful predictions of these changes
[1] We extend the analysis of a global CH 4 data set retrieved from SCIAMACHY (Frankenberg et al., 2006) by making a detailed comparison with inverse TM5 model simulations for 2003 that are optimized versus high accuracy CH 4 surface measurements from the NOAA ESRL network. The comparison of column averaged mixing ratios over remote continental and oceanic regions shows that major features of the atmospheric CH 4 distribution are consistent between SCIAMACHY observations and model simulations. However, the analysis suggests that SCIAMACHY CH 4 retrievals may have some bias that depends on latitude and season (up to $30 ppb). Large enhancements of column averaged CH 4 mixing ratios ($50-100 ppb) are observed and modeled over India, Southeast Asia, and the tropical regions of South America, and Africa. We present a detailed comparison of observed spatial patterns and their seasonal evolution with TM5 1°Â 1°zoom simulations over these regions. Application of a new wetland inventory leads to a significant improvement in the agreement between SCIAMACHY retrievals and model simulations over the Amazon basin during the first half of the year. Furthermore, we present an initial coupled inversion that simultaneously uses the surface and satellite observations and that allows the inverse system to compensate for the potential systematic bias. The results suggest significantly greater tropical emissions compared to either the a priori estimates or the inversion based on the surface measurements only. Emissions from rice paddies in India and Southeast Asia are relatively well constrained by the SCIAMACHY data and are slightly reduced by the inversion.
Differential optical absorption spectroscopy (DOAS) allows the quantitative determination of atmospheric trace gas concentrations by recording and evaluating the characteristic absorption structures (lines or bands) of the trace gas molecules along an absorption path of known length in the open atmosphere. The DOAS technique is characterized by the following: (1) measuring the transmitted light intensity over a relatively (compared to the width of an absorption band) broad spectral interval; (2) high‐pass filtering of the spectra to obtain a differential absorption signal and eliminating broad‐band extinction processes such as Rayleigh and Mie scattering (RS and MS); and (3) quantitative determination of trace column densities by matching the observed spectral signatures to prerecorded (reference) spectra by, for instance, least‐squares methods. DOAS shares the advantages of most other spectroscopic techniques, including inherent calibration, sub‐parts per trillion (ppt) to ppt sensitivity and precision (1–10%), good specificity, wall‐less operation, and the capability for remote measurements. In particular, the concentration of very reactive species such as the free radicals OH, NO 3 , ClO, BrO, and IO are determined with DOAS. Other species of interest to atmospheric chemistry are also measurable such as SO 2 , CS 2 , O 3 , NO, NO 2 , HONO, NH 3 , CH 2 O, and most monocyclic aromatic hydrocarbons. A description of the technique is given, and the various modes of operation and light‐path configurations are explained. The emphasis of this article is on the practical aspects of instrument design, components of DOAS systems, operation of DOAS instruments, and state‐of‐the‐art techniques for the evaluation of DOAS spectra and realistic determination of detection limits. Finally some examples of DOAS applications are given.
1. Scope -is the work directly or implicitly related to atmospheric composition? 2. Novelty -does the work provide a) a general and/or broader relevance (e.g. not a pure local study), b) new results or methods, and c) does it add significantly to the knowledge of atmospheric composition and its impacts?3. Quality -does the work contain high quality a) atmospheric observations, b) process studies, c) modeling exercises or d) data analysis?Will your paper be within the scope of Atmospheric Environment?We try to be flexible with novel scientific articles on issues of atmospheric composition even, if they are not directly related to atmospheric measurements (e.g. wind tunnel studies, dynamometer studies, remote sensing retrieval, etc). However, we are still cautious of purely mathematical derivations, preliminary results or insignificant case and local studies. The authors should make sure that the articles contain substantial contributions to the science of atmospheric composition before sending them for review.
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