Abstract. Global climate change is one of the most important scientific, societal and economic contemporary challenges. Fundamental understanding of the major processes driving climate change is the key problem which is to be solved not only on a global but also on a regional scale. The accuracy of regional climate modelling depends on a number of factors. One of these factors is the adequate and comprehensive information on the anthropogenic impact which is highest in industrial regions and areas with dense population – modern megacities. Megacities are not only “heat islands”, but also significant sources of emissions of various substances into the atmosphere, including greenhouse and reactive gases. In 2019, the mobile experiment EMME (Emission Monitoring Mobile Experiment) was conducted within the St. Petersburg agglomeration (Russia) aiming to estimate the emission intensity of greenhouse (CO2, CH4) and reactive (CO, NOx) gases for St. Petersburg, which is the largest northern megacity. St. Petersburg State University (Russia), Karlsruhe Institute of Technology (Germany) and the University of Bremen (Germany) jointly ran this experiment. The core instruments of the campaign were two portable Bruker EM27/SUN Fourier transform infrared (FTIR) spectrometers which were used for ground-based remote sensing measurements of the total column amount of CO2, CH4 and CO at upwind and downwind locations on opposite sides of the city. The NO2 tropospheric column amount was observed along a circular highway around the city by continuous mobile measurements of scattered solar visible radiation with an OceanOptics HR4000 spectrometer using the differential optical absorption spectroscopy (DOAS) technique. Simultaneously, air samples were collected in air bags for subsequent laboratory analysis. The air samples were taken at the locations of FTIR observations at the ground level and also at altitudes of about 100 m when air bags were lifted by a kite (in case of suitable landscape and favourable wind conditions). The entire campaign consisted of 11 mostly cloudless days of measurements in March–April 2019. Planning of measurements for each day included the determination of optimal location for FTIR spectrometers based on weather forecasts, combined with the numerical modelling of the pollution transport in the megacity area. The real-time corrections of the FTIR operation sites were performed depending on the actual evolution of the megacity NOx plume as detected by the mobile DOAS observations. The estimates of the St. Petersburg emission intensities for the considered greenhouse and reactive gases were obtained by coupling a box model and the results of the EMME observational campaign using the mass balance approach. The CO2 emission flux for St. Petersburg as an area source was estimated to be 89 ± 28 ktkm-2yr-1, which is 2 times higher than the corresponding value in the EDGAR database. The experiment revealed the CH4 emission flux of 135 ± 68 tkm-2yr-1, which is about 1 order of magnitude greater than the value reported by the official inventories of St. Petersburg emissions (∼ 25 tkm-2yr-1 for 2017). At the same time, for the urban territory of St. Petersburg, both the EMME experiment and the official inventories for 2017 give similar results for the CO anthropogenic flux (251 ± 104 tkm-2yr-1 vs. 410 tkm-2yr-1) and for the NOx anthropogenic flux (66 ± 28 tkm-2yr-1 vs. 69 tkm-2yr-1).
[1] We describe a new inversion algorithm developed for the retrieval of atmospheric constituents from Stratospheric Aerosol and Gas Experiment III (SAGE III) solar occultation measurements. The methodology differs from the operational (NASA) algorithm in several important ways. Our algorithm takes account of the finite altitude and spectral resolution of the measurements by integrating over the viewing window spectrally and spatially. We solve the problem nonlinearly by using optimal estimation theory, and we use an aerosol parameterization scheme based on eigenvectors derived from existing empirical and modeled information about their microphysical properties. The first four of these eigenvectors are employed in the retrieval algorithm to describe the spectral variation of the aerosol extinction. We retrieve ozone and nitrogen dioxide number densities and aerosol extinction from transmission measurements at 41 channels from 0.29 to 1.55 mm. In this paper we describe the results of the gas retrievals. Numerical simulations test the accuracy of the scheme, and subsequent retrievals from SAGE III transmission data for the period between May and October 2002 produce profiles of O 3 and NO 2 . Comparisons of the O 3 and NO 2 profiles with those obtained using the SAGE III operational algorithm and with those from independent measurements made by satellites, ozonesondes, and lidar indicate agreement in ozone measurements in the middle and upper stratosphere significantly closer than the natural variability and agreement in the lower stratosphere and upper troposphere approximately equal to the natural variability.
Abstract. The anthropogenic impact is a major factor of climate change, which is highest in industrial regions and modern megacities. Megacities are a significant source of emissions of various substances into the atmosphere, including CO2 which is the most important anthropogenic greenhouse gas. In 2019 and 2020, the mobile experiment EMME (Emission Monitoring Mobile Experiment) was carried out on the territory of St Petersburg which is the second-largest industrial city in Russia with a population of more than 5 million people. In 2020, several measurement data sets were obtained during the lockdown period caused by the COVID-19 (COronaVIrus Disease of 2019) pandemic. One of the goals of EMME was to evaluate the CO2 emission from the St Petersburg agglomeration. Previously, the CO2 area flux has been obtained from the data of the EMME-2019 experiment using the mass balance approach. The value of the CO2 area flux for St Petersburg has been estimated as being 89±28 kt km−2 yr−1, which is 3 times higher than the corresponding value reported in the official municipal inventory. The present study is focused on the derivation of the integral CO2 emission from St Petersburg by coupling the results of the EMME observational campaigns of 2019 and 2020 and the HYSPLIT (HYbrid Single-Particle Lagrangian Integrated Trajectories) model. The ODIAC (Open-Data Inventory for Anthropogenic CO2) database is used as the source of the a priori information on the CO2 emissions for the territory of St Petersburg. The most important finding of the present study, based on the analysis of two observational campaigns, is a significantly higher CO2 emission from the megacity of St Petersburg compared to the data of municipal inventory, i.e. ∼75800±5400 kt yr−1 for 2019 and ∼68400±7100 kt yr−1 for 2020 versus ∼30 000 kt yr−1 reported by official inventory. The comparison of the CO2 emissions obtained during the COVID-19 lockdown period in 2020 to the results obtained during the same period of 2019 demonstrated the decrease in emissions of 10 % or 7400 kt yr−1.
Abstract. Monitoring atmospheric anthropogenic halocarbons plays an important role in tracking their atmospheric concentrations in accordance with international agreements on emissions of ozone-depleting substances and, thus, in estimating the ozone layer recovery. Within the Network for the Detection of Atmospheric Composition Change (NDACC), regular Fourier transform infrared (FTIR) measurements can provide information on the abundancies of halocarbons on a global scale. We improved retrieval strategies for deriving the CFC-11 (CCl3F), CFC-12 (CCl2F2), and HCFC-22 (CHClF2) atmospheric columns from IR solar radiation spectra measured by the Bruker IFS125HR spectrometer at the St. Petersburg site (Russia). We used the Tikhonov–Phillips regularization approach for solving the inverse problem with optimized values of regularization parameters. We tested the strategies developed by comparison of the FTIR measurements with independent data. The analysis of the time series of column-averaged dry air mole fractions (Xgas) measured in 2009–2019 gives mean values of 225 pptv (parts per trillion by volume; CFC-11), 493 pptv (CFC-12), and 238 pptv (HCFC-22). Trend values total −0.40 % yr−1 (CFC-11), −0.49 % yr−1 (CFC-12), and 2.12 % yr−1 (HCFC-22). We compared the means, trends, and seasonal variability in XCFC-11, XCFC-12, and XHCFC-22 to that of (1) near-ground volume mixing ratios (VMRs), measured at the observational site Mace Head, Ireland (GVMR), (2) the mean in the 8–12 km layer VMRs, measured by ACE-FTS and averaged over 55–65∘ N latitudes (SVMR), and (3) Xgas values of the Whole Atmosphere Community Climate Model (WACCM) for the St. Petersburg site (WXgas). In general, the comparison of Xgas with the independent data showed a good agreement of their means within the systematic errors of the measurements considered. The trends observed over the St. Petersburg site demonstrate the smaller decrease rates for XCFC-11 and XCFC-12 than that of the independent data and the same increase rate for XHCFC-22. As a whole, Xgas, SVMR, and WXgas showed qualitatively similar seasonal variations, while the GVMR variability is significantly less, and only the WXHCFC-22 variations are essentially smaller than that of XHCFC-22 and SVMRHCFC-22.
We compared two datasets of the total content of atmospheric water vapor received near St. Petersburg in 2009-2012 from ground based Fourier transform spectroscopy measurements at the Peter hof station and from radio sounding at Voyeykovo station. Despite a good correlation of daily measurements in Peterhof and Voyeykovo, the standard mismatch is significant, 20% or more, for most subsets taken for the comparison. The high mismatch is mainly due to the natural spatial variability of the total content of water vapor, accounting for the 50 km distance between Peterhof and Voyeykovo. This variability needs to be con sidered when validating the satellite measurements of water vapor content by ground based measurements.
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