NO<Subscript>2</Subscript> content variations near St. Petersburg as inferred from ground-based and satellite measurements of scattered solar radiation

An automatic spectral complex developed at the Institute of Physics, St. Petersburg State University, is described. This complex is used for regular ground-based spectroscopic measurements of the total NO₂ content in the vertical column of the atmosphere during the twilight and daylight hours of the day near St. Petersburg (Petrodvorets). In 2004–2006, a number of ground-based twilight measurements of the total NO₂ content were obtained near St. Petersburg, and variations in the NO₂ content in the troposphere were estimated from the results of daytime ground-based measurements. An example of the spatial annual mean distribution of the NO₂ content (central and northern Europe, northwestern Russia) based on the data of satellite measurements over the period 2003–2005 is presented. This example demonstrates the main sources of anthropogenic pollution. An increase in the mean annual contents of tropospheric NO₂ near Moscow and St. Petersburg is preliminarily estimated for the entire period of satellite observations with the GOME instrument at about 30–40% over ten years.     

Integral emission of nitrogen oxides from the territory of St. Petersburg based on the data of mobile measurements and numerical simulation results

The results of spectroscopic measurements of tropospheric NO₂ content performed on a closed route along the circular road around the city of St. Petersburg in 2012, 2014, and 2015 are presented. A procedure for determining the integral emission of NO _x based on the data of measurements on the route enveloping the sources under study is described. An analysis of the experimental data together with the results of a numerical simulation of air pollutant dispersion (the HYSPLIT model) provided an estimate of the total volume of NO _x emitted by all sources located inside the circular road. The average emission rate of NO _x according to the sources of the megacity of St. Petersburg is 57000 t/yr, which correlates satisfactorily with the official data of a municipal inventory of the sources of air pollution (62000–63 000 t/yr).     

Stratospheric NO2 content according to data from ground-based measurements of solar IR radiation

Atmospheric NO₂ content data obtained from regular ground-based measurements of solar IR radiation in the St. Petersburg region using a spectrometer with a high spectral resolution are analyzed. The absorption spectra of the NO₂ multiplet in the vicinity of ～2915 cm^?1 allow one to obtain data on variations in the stratospheric total content of NO₂ in 2009–2011. The accuracy of these data is estimated from their comparison with data obtained from independent ground-based and satellite measurements. The parameters of the seasonal cycle of the stratospheric content of NO₂ are estimated. The body of data accumulated during these measurements in the IR region made it possible to isolate the component of a daytime photochemical increase in the stratospheric content of NO₂ and estimate its rate.     

Regional space monitoring of nitrogen dioxide in the troposphere

Satellite instruments for the routine global monitoring of NO₂ in the atmosphere—the Global Ozone Monitoring Experiment (GOME) on the ERS-2 satellite, the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) on the ENVISAT satellite, the Ozone Monitoring Instrument (OMI) on the AURA satellite, and the GOME-2 on the MetOp satellite—are briefly described. It is shown that the error of measuring the NO₂ total column amount (∼10% for the background conditions in the troposphere) substantially increases in regions subject to anthropogenic pollution. Examples of practically using multiyear satellite measurements for the regional monitoring of NO₂ in the troposphere are presented, including mapping the tropospheric NO₂ in Russia, identifying the weekly and annual cycles in tropospheric NO₂ variations for megalopolises (St. Petersburg, Moscow, Paris), and estimating the long-term linear trend in 1995–2007.     

Validating NO<Subscript>2</Subscript> measurements in the vertical atmospheric column with the OMI instrument aboard the EOS Aura satellite against ground-based measurements at the Zvenigorod Scientific Station

Data on the NO₂ content in the vertical column of the atmosphere obtained with the Ozone Monitoring Instrument (OMI) aboard the EOS Aura satellite (United States) in the period from October 2004 to October 2007 are compared with the results of ground-based measurements at the Zvenigorod Scientific Station (55.7° N, 36.8° E). The “unpolluted”; part of the total NO₂ content in the atmospheric column, which mostly represents the stratosphere, and the NO₂ contents in the vertical column of the troposphere, including the lower layer, which is subject to pollution, are included in the comparison. The correlation coefficient between the results of ground-based and satellite measurements of the “unpolluted” total NO₂ content is ∼0.9. The content values measured with the OMI instrument are smaller than the results of ground-based measurements (on average, by (0.30 ± 0.03) × 10¹⁵ cm⁻² or by (11 ± 1)%). Therms discrepancy between the satellite and ground-based data is 0.6 × 10¹⁵ cm⁻². The NO₂ content in the vertical column of the troposphere from the results of satellite measurements is, on average, (1.4 ± 0.5) × 10¹⁵ cm⁻², (or about 35%) smaller than from the results of ground-based measurements, and the rms discrepancy between them is about 200%. The correlation coefficient between these data is ∼0.4. This considerable discrepancy is evidently caused by the strong spatial (horizontal) inhomogeneity and the temporal variability of the NO₂ field during episodes of pollution, which leads to different (and often uncorrelated) estimates of the NO₂ content in the lower troposphere due to different spatial resolutions of ground-based and satellite measurements.     

Analysis of variability of the CO, NO2, and O3 contents in the troposphere near St. Petersburg

The space-time variability of the fields of CO, NO₂, and O₃ concentrations and contents in the troposphere of northwestern Russia is analyzed on the basis of experimental data and the results of numerical modeling. The influence that the St. Petersburg emission has on the concentrations and contents of CO, NO₂, and O₃ in the troposphere is estimated for March 2006. A comparison of the measurements of the total CO content and the tropospheric NO₂ content with the results of modeling showed a qualitative and, in come cases, quantitative agreement between the results of calculations and experimental data. When synoptic conditions are determined, the St. Petersburg train can be detected at a distance of more than 300 km, which can affect the atmospheric air quality in adjacent countries.     

Study of the factors determining anomalous variability of carbon dioxide total column amount over St. Petersburg

Results of spectroscopic measurements of the carbon dioxide total column amount near St. Petersburg during forest fires in the period from August to September 2002 are analyzed. The HYSPLIT model is used to calculate air-mass trajectories and CO distribution on a mesoscale in this period. The HYSPLIT model simulations and measurements of carbon dioxide total column amount yield an estimate of the specific intensity of CO emission in a Pskov forest fire on August 28–September 8, 2002, equal to 0.17–0.26 kg m². This estimate can be used for an estimation of the integral CO emission from fires in northwestern Russian forests and for model simulations of atmospheric CO concentration fields. The estimate of the CO emission from forest fires that is obtained from ground-based measurements can also be made on the basis of satellite measurements if they contain information on CO in the lower tropospheric layers (0 to 2 km).     

Seasonal variations in the total content of hydrogen fluoride in the atmosphere

The results of ground-based measurements of the total content (TC) of hydrogen fluoride in the atmosphere in Peterhof near St. Petersburg for one year (from April 2009 through April 2010) using a Bruker IFS125 Fourier spectrometer with a high spectral resolution (0.005 cm^?1) are presented. The well-known computer code SFIT2 (Zephyr-2) was used for the radiation data inversion. Random measurement errors were 1–5% and the systematic error was 5–10%. The seasonal trend of the HF TC in Peterhof is characterized by a minimum in summer and a maximum in winter through early spring and is very close to the seasonal HF TC trend obtained at the Harestua Network for the Detection of Atmospheric Composition Change (NDACC) station located at about the same latitude. A comparison of the St. Petersburg State University (SPbSU) ground-based measurements with the data of satellite HF TC measurements (with an ACE-FTS instrument) showed a good quantitative agreement of the results for the entire period of observations. According to our ground-based measurements and the satellite measurements with the ACE-FTS instrument, the mean values of the HF TC and its rms variations during the period under investigation are 1.77 × 10¹⁵ and 1.80 × 10¹⁵ cm^?2 (difference 1.5%) and 21 and 18%, respectively.     

Comparing data obtained from ground-based measurements of the total contents of O<Subscript>3</Subscript>, HNO<Subscript>3</Subscript>,HCl,and NO<Subscript>2</Subscript> and from their numerical simulation

Chemistry climate models of the gas composition of the atmosphere make it possible to simulate both space and time variations in atmospheric trace-gas components (TGCs) and predict their changes. Both verification and improvement of such models on the basis of a comparison with experimental data are of great importance. Data obtained from the 2009–2012 ground-based spectrometric measurements of the total contents (TCs) of a number of TGCs (ozone, HNO₃, HCl, and NO₂) in the atmosphere over the St. Petersburg region (Petergof station, St. Petersburg State University) have been compared to analogous EMAC model data. Both daily and monthly means of their TCs for this period have been analyzed in detail. The seasonal dependences of the TCs of the gases under study are shown to be adequately reproduced by the EMAC model. At the same time, a number of disagreements (including systematic ones) have been revealed between model and measurement data. Thus, for example, the EMAC model underestimates the TCs of NO₂, HCl, and HNO₃, when compared to measurement data, on average, by 14, 22, and 35%, respectively. However, the TC of ozone is overestimated by the EMAC model (on average, by 12%) when compared to measurement data. In order to reveal the reasons for such disagreements between simulated and measured data on the TCs of TGCs, it is necessary to continue studies on comparisons of the contents of TGCs in different atmospheric layers.     

Ground-based spectroscopic measurements of the total nitric acid content in the atmosphere

The results of the first ground-based spectroscopic measurements in Russia of the total content (TC) of nitric acid in the atmosphere near St. Petersburg over the period April 2009–October 2011 are presented. These measurements show a substantial seasonal trend of the HNO₃ TC with maximal values in the winter period and early in the spring and minimal values in the summer time. The seasonal trends and variations in the daily mean values of HNO₃ TC near St. Petersburg in the winter and spring periods agree well with observations at the Kiruna station of the international NDACC network.     

Variations in the column-average dry-air mole fractions of CO2 in the vicinity of St. Petersburg

The results obtained from ground-based spectroscopic measurements of column-average dry-air mole fractions of CO₂ in the atmosphere over the St. Petersburg region are given for the period April 2009–October 2011 (～900 measurement runs, 151 measurement days). These results show significant variations in the CO₂ mixing ratio in the atmosphere over the St. Petersburg region. The minimum value of this mixing ratio (373.1 ppm) was observed on April 27, 2011, and its maximum value (420.8 ppm) was observed on February 10, 2010. The typical seasonal behavior of the CO₂ mixing ratio with its summer minimum was observed in 2009. In July 2010 and 2011, the values of the CO₂ mixing ratio increased apparently due to high air temperatures. In 2010 an additional contribution to this increase in the CO₂ mixing ratio could have been made by strong natural fires.     

Intercomparison of satellite and ground-based ozone total column measurements

Ozone total column (OTC) measurements made in 2009–2012 near St. Petersburg by a Fourier Transform Infrared (FTIR) spectrometer (Peterhof, St. Petersburg State University (SPbSU)), an M-124 filter ozonometer, and a Dobson spectrophotometer (Voeikovo, MGO), as well as measurements made by a spectrometer ozone monitoring instrument (OMI) (onboard the AURA satellite) have been analyzed and compared. Comparisons have been performed both between ensembles of ground-based measurement data, as well as between ground-based and satellite data. It has been shown that the standard deviation for all devices is 2.5–4.5%; here, the FTIR and Dobson instruments measuring the direct sun are in better agreement with OMI than the M-124 ozonometer measuring the zenith-scattered solar radiation as well. A seasonal cycle in discrepancy with amplitude of 1.5% has been detected between two series of OTC measurements made by M-124 and OMI instruments for a total of 850 days. In fall and winter, the ground-based measurements underestimate the OTC values in comparison with satellite data; in spring and summer, the situation is reversed: ground-based data overestimate the OTC values. Also, it has been revealed that FTIR measurements systematically overestimate the OTC values in comparison with other instruments: from 1.4% (for Dobson) to 3.4% (for OMI). Taking into account the spatial and temporal discrepancy of independent ensembles of measurements and an analysis of standard deviations between ground-based and satellite measurement data, the FTIR spectrometer (SPbSU) can be recommended for OTC satellite data validation.     

Estimation of multiyear changes in nitrogen oxide emissions in megalopolises from satellite measurements

The influence that megalopolises have on the atmospheric composition on regional and global scales is the subject of intense investigations; however, data on the emissions of pollutants used for such investigations are often insufficiently reliable. In this work the possibilities for diagnosing long-term changes in nitrogen oxide emissions in megalopolises are investigated based on a combined use of data from satellite measurements and modeling of the tropospheric nitrogen dioxide content. Primary emphasis is placed on analyzing possible situations when emission changes are of a nonlinear character. The proposed methodology includes an original method for the nonlinear approximation of changes in a physical quantity from a noised time series of its measurements. Changes in NO _x emissions are investigated in 12 megalopolises of Europe and the Middle East in the period from 1996 to 2008. Statistically significant changes in NO _x emissions are detected in five megalopolises (Baghdad, Madrid, Milan, Moscow, and Paris). By using three megalopolises (Madrid, Milan, and Paris) as an example, it is shown that a nonlinear approximation of NO _x emission changes agrees better with independent ground-based measurements than an analogous linear approximation.     

Ground-based measurements of total column of hydrogen chloride in the atmosphere near St. Petersburg

We present ground-based spectroscopic measurements of the total hydrogen chloride in the atmosphere of Peterhof near St. Petersburg from April 2009 to March 2012. The well-known computer code SFIT-2 (Zephyr-2) was used to interpret the spectra of the solar IR radiation. The random and systematic errors of total column (TC) HCl measurements did not exceed 3.8 and 4.5%. The seasonal behavior of TC HCl in Peterhof is characterized by the presence of a maximum in March–April and a minimum in October–November. There are also extremely small TC HCl values in January–February. The time behavior obtained for Peterhof agrees well with data from nearest stations in the NDACC international network. The ground-based measurements of the TC HCl were compared with satellite measurements with the help of ACE-FTS and MLS instruments. The direct comparisons of coincident (within a day) and collocated (within 500 km) satellite and ground-based measurements showed a correspondence of results within their total errors.     

Spatial–Temporal CO2 Variations near St. Petersburg Based on Satellite and Ground-Based Measurements

Izvestiya, Atmospheric and Oceanic Physics - The results of studying spatial–temporal CO2 variations near St. Petersburg in 2014–2017 based on satellite measurements (OCO-2 satellite)...     

Analysis of satellite observations of the tropospheric NO<Subscript>2</Subscript> content over the Moscow region

The tropospheric NO₂ content over the Moscow region is analyzed on the basis of data of the satellite Ozone Monitoring Instrument (OMI) in the period 2004–2009. The spatial distributions of NO₂ are presented, and some of their features are interpreted. The characteristics of the seasonal and weekly cycles of NO₂ are described, as are its interannual and long-term variations. The relationship between the variabilities of the NO₂ content and the aerological parameters is investigated on different time scales. The mutual influence of regional pollution and meteorological regimes is discussed. The seasonal and weekly NO₂ cycles over Moscow are compared with those over the largest worldwide agglomerations.     

Seasonal features of quasi-biennial variations of NO<Subscript>2</Subscript> stratospheric content derived from ground-based measurements

Seasonal and latitudinal distributions of amplitudes of quasi-biennial variations in total NO₂ content (NO₂ TC), total ozone content (TOC), and stratospheric temperature are obtained. NO₂ TC data from ground-based spectrometric measurements within the Network for the Detection of Atmospheric Composition Change (NDACC), TOC data from satellite measurements, and stratospheric temperature data from ERA-Interim reanalysis are used for the analysis. The differences in the NO₂ TC diurnal cycles are identified between the westerly and easterly phases of the quasi-biennial oscillations (QBO) of equatorial stratospheric wind. The QBO effects in the NO₂ TC, TOC, and stratospheric temperature in the Northern (NH) and Southern (SH) hemispheres are most significant in the winter–spring periods, with essential differences between the NH and SH. The NO₂ TC in the Antarctic is less for the westerly phase of the QBO than that for the easterly phase, and the NO₂ TC quasi-biennial variations in the SH mid-latitudes are opposite of the variations in the Antarctic. In the NH, the winter values of the NO₂ TC are generally less during the westerly QBO phase than during the easterly phase, whereas in spring, on the contrary, the values for the westerly QBO phase exceed those for the easterly phase. Along with NO₂, the features of the quasi-biennial variations of TOC and stratospheric temperature are discussed. Possible mechanisms of the quasi-biennial variations of the analyzed parameters are considered for the different latitudinal zones.     

Comparison of the satellite and ground-based measurements of the hydrogen fluoride content in the atmosphere

Satellite and ground-based measurements of the hydrogen fluoride (HF) total content (TC) are analyzed and compared. The HF profiles measured with an FTS device on the ACE satellite are used to calculate the TC and compare it with the ground-based measurements near St. Petersburg in 2009–2011. A comparison indicated that the seasonal variations in HF TC based on two independent measurements are in good qualitative agreement. Rare (nine) cases of direct comparison between two measurement types coordinated with respect to time (during the day) and site (no farther than 500 km) gave the following characteristics: the average difference is 8% and satellite data predominate over ground data; the standard deviation of a difference is 7%. In two cases of close measurement pairs (closer than 200 km), a comparison gave differences of 1 and 7%. The statistical characteristics of differences between two measurement types are in good agreement with the independent comparison of the ACE-FTS HF TC measurements with the NDACC network data.     

Comparison of Ground-Based Measurement Results of Total Ozone near St. Petersburg

Izvestiya, Atmospheric and Oceanic Physics - This paper compares the results of ground-based measurements of the total ozone content (TOC) near St. Petersburg for the period of 2009–2020. The...     

Winter–spring anomalies in stratospheric O<Subscript>3</Subscript> and NO<Subscript>2</Subscript> contents over the Moscow region in 2010 and 2011

Using results of ground-based spectrometric measurements, we analyze the anomalies in the stratospheric contents of O₃ and NO₂ in the Moscow region related to the sudden stratospheric warming and associated distortion of the stratospheric circumpolar vortex in early February 2010 and to the latitudinal displacement of the vortex towards the European sector in late March 2011 before the final spring warming. In the former case, the O₃ concentration increased up to 85% and the stratospheric column NO₂ content increased twice; in the latter case, the O₃ concentration decreased by a quarter and the NO₂ content decreased twice in comparison with average values for the time periods preceding the onsets of the anomalies. Estimates of the statistical correlationship of the stratospheric O₃ and NO₂ contents with potential vorticity and geopotential have been obtained.