Determination of carbon monoxide pollution of the atmosphere over Moscow with a spectroscopic method

The results of measurements of the total content of carbon monoxide in an atmospheric column over Moscow and the Zvenigorod Scientific Station (ZSS) are given for the period 1993–2005. The simultaneous measurements of the regional background contents of carbon monoxide over a rural area (ZSS) and over Moscow made it possible to isolate an urban portion of the CO content. The total content of CO over the city varies significantly from day to day from values close to the background value to values that are 2.5–3 times greater than the background value. The number of days with such a CO content is 5% of the total number of measurement days. Such a CO content is most often observed during the cold seasons. During the warm seasons, in most of the cases, slight excesses of the CO background value are observed in the urban atmosphere. Variations in the CO content are determined mainly by wind-velocity variations and temperature inversions. In 2002, the high CO concentrations were due to forest and peatbog fires. On some days, over the ZSS, the concentrations of CO were high as never before. Over this period (12 years), the CO content in the surface air layer over the city did not increase.     

Total content of carbon monoxide in the atmosphere over Russian regions according to satellite data

Carbon monoxide (CO) total columns over European Russia (ER) and western Siberia (WS) have been analyzed using MOPITT (V5, TIR/NIR, L3) IR-radiometer data obtained in 2000–2014. High CO contents are revealed over large urban and industrial agglomerations and over regions of oil-and-gas production. A stable local CO maximum is observed over the Moscow agglomeration. Statistical characteristics of CO total columns observed in the atmosphere over ER and WS in 2000–2014 are presented. An analysis of long-term changes in CO content reveals nonlinear changes in the CO total column over northern Eurasia in 2000–2014. Results of a comparative analysis of annual variations in atmospheric CO contents over ER and WS are given. Based on Fourier analysis, empirical models of annual variations in total CO contents over ER and WS are proposed. Relations between regional CO contents and fire characteristics and between spatial CO distributions and features of large-scale atmospheric dynamics under conditions of weather and climate anomalies in the summers of 2010 in ER and 2012 in WS are analyzed. Data on total CO contents measured with a MOPITT satellite radiometer and a ground-based spectrometer operating at the Zvenigorod Scientific Station of the Obukhov Institute of Atmospheric Physics are compared.     

Investigation of the 2010 July–August fires impact on carbon monoxide atmospheric pollution in Moscow and its outskirts, estimating of emissions

We investigate the air pollution in the central European part of Russia during the 2010 summer fires. The results of ground-based (Institute of Atmospheric Physics (IAP), Moscow State University (MSU), and Zvenigorod Scientific Station (ZSS)) and satellite (MOPITT, AIRS, of Terra and Aqua satellites) measurements of the total content and concentration of carbon monoxide (CO), as well as MODIS data on the spatial and temporal distribution of forest and peat fires obtained from Terra and Aqua satellites, are presented. A comparison between similar situations in 2010 and 2002 revealed the causes of higher pollution levels in 2010. The use of trajectory analysis, detailed space imagery, and model calculations made it possible to reveal the location of peat fires and their contribution to the air pollution over the Moscow megalopolis. Fireemission estimates were obtained using two independent methods.     

Carbon monoxide emissions in summer 2010 in the central part of the Russian Plain and estimation of their uncertainties with the use of different land-cover maps

This study is devoted to estimation of carbon monoxide (CO) emissions during the wildfires of the anomalously hot 2010 summer in the central part of the Russian Plain. CO emissions from the forest wildfires have been estimated with use of the Active Fires (AF) (MODIS MCD14ML) and Burned Areas (BA) (MODIS MCD45) methods for AVHRR/UDM, Global Land Cover 2000 (GLC 2000), GlobCover, and MCD12Q1 vegetation maps. A comparison of the vegetation maps and investigation of forest structure dynamics for the period from 2005 to 2009 have been carried out. It is shown that the major uncertainties during the estimation of CO in decreasing order are the following: distinctions in emission-calculation methods, differences in the vegetation maps used, differences in satellite data from Terra and Aqua, and the insufficient registration of forest structure dynamics. For additional comparison of estimations obtained by an independent method with the use of orbital (MOPITT, AIRS, and IASI) and ground-based (Moscow and Zvenigorod) spectroscopic measurements of CO content were presented.     

Analysis of the weekly cycle in the atmosphere near Moscow

Using the spectral method and the method of grouping by days of week, we analyzed the weekly cycles by standard air sounding data obtained at the Dolgoprudny station near Moscow and by the results of measurements of NO₂ content in the stratosphere and the atmospheric boundary layer at the Zvenigorod Research Station of the Obukhov Institute of Atmospheric Physics, Russian Academy of Sciences, in 1990–2010. We revealed weekly cycles of the NO₂ content in the vertical column of the stratosphere, temperature, geopotential, meridional wind velocity in the troposphere and lower stratosphere, and the tropopause height in the warm half of the year (mid-April to mid-October). The weekly variations in temperature in the troposphere are positive in the first half of the week and negative in the second half, and the variations in temperature in the tropopause layer and in the lower stratosphere are opposite in sign to the tropospheric variations. The weekly cycle of the tropopause height is approximately in phase with the cycle of tropospheric temperature, and the weekly cycle of the NO₂ content in the stratospheric column is opposite in phase to the cycle of the tropopause height. Weekly variations were also observed in the total ozone content over Moscow. This finding was confirmed by calculations based on regression relationships between the vertical distribution of ozone and tropopause height. Conceptual mechanisms of weekly cycles were proposed.     

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.     

Time variations of the total CO content in the atmosphere near St. Petersburg

We analyzed measurements of the total carbon monoxide (CO) content in the atmosphere in the region of St. Petersburg (59.88°N, 29.83° E; 20 m above sea level) in the period from 1995 to 2009. The average annual behavior for the entire measurement period has a maximum in February–March and a minimum in July with an amplitude of ～20%. In the absence of strong forest fires in the European part of the Russian Federation and Siberia, the annual minimum of the total CO content is usually recorded in August–September. In winter 1995–2009 (November–January), there was a decrease in the total CO content with a gradual shift in the maximum of the annual behavior from January (1995–1999) to February (2000–2004) and March (2005–2009). The total CO content in January–February 2009 was ～20% lower than the multiyear average level. Estimates of the linear trend for the maximum, minimum, and average values for the period of 1996–2009 showed an absence of statistically significant long-term changes in the total CO content. A spectral analysis of data showed that the spectral components with periods of 12, 14, 17, 24, and 46 months are extracted with 80% confidence. It is shown that the irregular component of the time series of the total CO content (calculated for the period from May to September) agrees well with data on the areas of the forest fires and on the volume of the burnt forest and that 1999, 2001, 2005, 2007, and 2009 can be considered “background” years with the least numbers of forest fires.     

Analysis of the quasi-biennial variability of carbon monoxide total column

On the basis of satellite observations of column carbon monoxide (CO) and total ozone (TO), an analysis has been performed of the connection of the interannual variability of CO with the quasi-biennial oscillation (QBO) of the equatorial stratospheric wind and the QBO of total ozone. It is found that the CO total colomn over most of the globe in the westerly phase of the QBO is greater than that in the easterly phase. The global distribution of the CO QBO amplitudes exhibits a local maximum over Indonesia, where the peak-to-peak amplitude of the CO QBO signal averages 15% of the local annual mean CO in this region. Analysis shows that the QBOs of CO are well synchronized with the QBO of wind at 50 hPa. At the same time, a joint analysis of the characteristics of the CO QBO and TO QBO demonstrates no direct photochemical coupling between of the quasi-biennial variations of TO and CO.     

Variations in the total column amounts of carbon monoxide and methane in the Antarctic atmosphere

The results of measuring the total contents of carbon monoxide and methane via the method of solar-absorption spectroscopy are presented. The measurements were performed at the Molodezhnaya Station in 1977–1978, at the Mirny Observatory from 1982 to 1992, and at the Novolazarevskaya Station from 2003 to 2006. The character of seasonal variations in the contents of these gases in the Antarctic atmosphere is described and compared to the intra-annual variation of their surface concentrations measured at the Syowa Station (Japan). Synchronous intra-annual variations in the contents of carbon monoxide in the atmospheric column and in its surface concentrations are observed, while the spring maximum content of methane is observed three months after the maximum of its surface concentration. Synchronous seasonal variations in the total content of methane and ozone are observed, which makes it possible to suggest that the Antarctic circumpolar vortex has a significant influence on the characteristics of the vertical distribution of methane during Antarctic spring. Quantitative estimates of the parameters of multiyear variations in the contents of CO and CH₄ are given. The content of methane was increasing (although with different rates) during the entire observation period 1977–2006. The content of CO was observed to increase until 1992 and to decrease during 2003–2006.     

Chemical composition and microphysical characteristics of atmospheric aerosol over moscow and its vicinity in June 2009 and during the fire peak of 2010

The microphysical characteristics of aerosol were measured in the atmospheric surface layer simultaneously over the center of Moscow and its vicinity (Zvenigorod Scientific Station, Obukhov Institute of Atmospheric Physics, Russian Academy of Sciences) from June 15 to June 30, 2009, in order to compare the mass concentrations, particle-size distribution functions, and elemental compositions of aerosol over the megapolis and the background zone. During the fire peak of 2010, on August 8, aerosol samples were taken in the center of Moscow and their chemical composition was determined. Comparing results obtained from the simultaneous measurements of the concentrations of aerosol and its elemental composition made it possible to determine their interdiurnal variability, which suggests that the features of time variations are of a regional character and they are determined mainly by the dynamics of the synoptical processes of air-mass exchange. The chemical composition of obtained samples was determined using the method of atomic absorption spectrometry. The measurement results obtained in June 2009 revealed an increase in the content of anthropogenic elements in the atmosphere over Moscow when compared to their content in the atmosphere over the background zone. In Moscow, during the summer fires of 2010, the concentration of sulfur exceeded its concentration in June 2009 by an order of magnitude, and the concentrations of Na, Mg, Al, Si, K, Ca, and Fe increased several times. The mean mass concentration of aerosol amounted to 917 μg/m³ in August 2010 and 50–70 μg/m³ in June 2009.     

The effect of meteorology on air pollution in Moscow during the summer episodes of 2010

Relations between short-term variations in the concentrations of aerosol (PM₁₀) and carbon monoxide (CO) and meteorological characteristics are considered for the episodes of severe atmospheric pollution in the region of Moscow in the summer of 2010. The assumption is made and substantiated that the observed (in late June) severe aerosol pollution of the atmosphere over Moscow was caused by air masses arrived from soil-drought regions of southern Russia. In August, during the episodes of advection of forest-fire products, the maximum surface concentrations of pollutants were observed in Moscow mainly at 11:00–12:00 under a convective burst into the atmospheric boundary layer and at night in the presence of local wind-velocity maxima or low-level jet streams within the inversion layer. On the basis of results from an analysis of these air-pollution episodes before and after fires, it is concluded that the shearing instability of wind velocity favors the surface-air purification under ordinary conditions and an increase in the surface concentrations of pollutants during their advection (long-range transport, natural-fire plumes, etc.). It is shown that the pollution of the air basin over the megapolis with biomass-combustion products in 2010 led to an increase in the thermal stability of the atmospheric surface layer and in the duration of radiation inversions, as well as to an attenuation of the processes of purification in the urban heat island.     

Variability of trace gases in the atmospheric surface layer from observations in the city of Moscow

The results of continuous minute measurements of the surface concentrations of ozone, nitric oxide, nitrogen dioxide, carbon monoxide, and sulfur dioxide during the 2002–2004 period at the environmental station of the Oboukhov Institute of Atmospheric Physics, Russian Academy of Sciences (IAP), and the Faculty of Geography, Moscow State University (MSU), are discussed. It is shown that the conditions of Moscow’s southwestern region remote from large local pollution sources reflect the general regularities of the variability of trace gases in an urban atmosphere. This is manifested in the mean annual value of the ratio NO/NO₂ (a little less than 1), decreased daylight values of O₃, increased values of the rest of the trace gases as compared to the background region, and the presence of a secondary nocturnal maximum in the diurnal cycle of O₃. The features of the annual and diurnal cycles of the concentrations of the substances under analysis are discussed. In the diurnal cycle of the primary products of combustion (NO and CO), an excess of the morning maximum (over the evening one) is observed during both warm and transition periods and higher values of the night maximum (as compared to the daylight one) are noted for summer. The temperature stratification properties determined from the MSU long-term acoustic sounding data serve as a possible cause for both of the effects revealed. The annual cycle of the concentration of surface ozone is characterized by the highest values for spring and summer. The annual cycles of NO, NO₂, CO, and SO₂ do not demonstrate any obvious seasonal regularities. A significant seasonal variation of the ratio NO/NO₂, which is associated with the oxidizing properties of the urban atmosphere, is revealed. The record high concentrations of trace gases in the atmosphere over Moscow are given, and the meteorological conditions for their accumulation are discussed.     

Methane, carbon monoxide, and carbon dioxide concentrations measured in the atmospheric surface layer over continental Russia in the TROICA experiments

The principal statistical regularities typical of the behaviors of the CH₄, CO, and CO₂ concentrations in the atmospheric surface layer over the continental Russian territory are revealed from the measurements performed in 1997–2004 along the Trans-Siberian Railroad from Moscow to Khabarovsk with a mobile laboratory. The data obtained under the conditions of the atmosphere free of anthropogenic pollutants are analyzed. For near-background conditions, the typical continental methane, carbon monoxide, and carbon dioxide concentrations and characteristic features of their large-scale spatial distributions and daily variations, including those caused by surface inversions, are determined. Variations in the concentrations of these trace gases over industrial regions are analyzed. Our results are compared to the data obtained at background stations of the world network of atmospheric monitoring and to the data of a numerical simulation.     

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).     

Retrieval of spatial field of atmospheric aerosol concentration according to data from local measurements: A modification of the method of back trajectory statistics

The well-known method of the back trajectory statistics (BTS) is used to develop a new approach to estimating atmospheric pollution fields according to local measurements. On the basis of instrumental measurements at one or a few monitoring points and information on atmospheric dynamics (in this work, back trajectories of the motion of air particles), the BTS method makes it possible to estimate the spatial structure of fields of a measured quantity. Results from solving a simplified demonstration of estimating the spatial distribution of the volume concentration of a fine aerosol fraction are presented; these results were obtained on the basis of an analysis of photometric measurements in the period of 2004–2010 at six AERO-NET monitoring sites on the territory of Russia: Zvenigorod, Moscow, Yekaterinburg, Tomsk, Yakutsk, and Ussuriisk.     

Measurements of the atmospheric turbulence in the coastal zone of the sea during weak wind from a mountainous coast

Results of measurements of the atmospheric turbulence in the layer between 1.5 and 21 m above sea level and the drag coefficient of the sea surface as the wind blows from a 4-km-long mountainous slope with a mean inclination of 11° are presented. The measurements of wind-speed profiles and its fluctuations at several levels, waves, and the main meteorological parameters were carried out in autumn 2005 and 2008 from a stationary platform located in the Black Sea at a distance of approximately 1 km from the southern coast of Crimea. It is shown that during weak synoptic wind a low-level wind jet develops at night over the sea with a maximum velocity up to 5–6 m/s at a level of approximately 6 m over the sea induced by the katabatic wind over the coastal slope. According to the approximate estimates, the horizontal scale of the low-level jet can reach a few tens of kilometers. This flow is characterized by the dissipation rate of the turbulence energy independent of height and low-frequency velocity fluctuations related to the gravity waves and advection of turbulence from the coast. It is shown that the lower part of the boundary layer (up to a height of 3 m) is adjusted to the sea-surface roughness. The dependencies of the drag coefficient on the wind speed or wave age are steadier than in the data for the open sea. However, the age of the waves is not a universal parameter at long and short fetches.     

Weekly variability of surface CO concentrations in Moscow

Based on observations of carbon monoxide (CO) concentrations at three Mosekomonitoring stations, we have analyzed the weekly cycle of CO in the surface air of Moscow in 2004–2007. At all stations the minimum long-term mean daily CO values are observed on Sunday. The weekly cycle of CO more clearly manifests itself at the center of Moscow and becomes less clear closer to the outskirts. We have analyzed the reproducibility of the weekly cycle of CO from one year to another, the seasonal dependence, its specific features at different times of day, and the changes in the diurnal cycle of CO during the week. The factors responsible for specific features of the evolution of surface CO concentrations at different observation stations have been analyzed. The empirical probability density functions of CO concentrations on weekdays and at week- end are presented. The regularity of the occurrence of the weekend effect in CO has been investigated and the possible reasons for breaks in weekly cycles have been analyzed. The Kruskal-Wallis test was used to study the statistical significance of intraweek differences in surface CO contents.     

Radiative and Thermal Impacts of Smoke Aerosol Longwave Absorption during Fires in the Moscow Region in Summer 2010

The aerosol longwave radiative forcing of the atmosphere and heating rate of the near-surface aerosol layer are estimated for the extreme smoke conditions in the Moscow region in summer 2010. Thermal radiation fluxes in the atmosphere are determined using the integral transmission function and semiempirical aerosol model developed on the basis of standard aerosol models and measurements at the Zvenigorod Scientific Station, Obukhov Institute of Atmospheric Physics, Russian Academy of Sciences. The aerosol radiative forcing reached 33 W/m² at the lower atmospheric boundary and ranged between–1.0 and 1.0 W/m² at the upper atmospheric boundary. The heating rate of the 10-m atmospheric layer near surface was up to 0.2 K/h during the maximum smoke conditions on August 7–9. The sensitivity of the aerosol longwave radiative forcing to the changes in the aerosol absorption coefficient and aerosol optical thickness are estimated.     

Variations in gaseous pollutants in the air basin of Moscow

Variations in the concentrations of gaseous pollutants in the air basin of Moscow are statistically analyzed. The basic statistical characteristics of variations in the concentrations of carbon monoxide, nitric oxide, nitrogen dioxide, ozone, formaldehyde, and a number of aromatic compounds are calculated. The main properties of intradiurnal, synoptic, seasonal, and interannual variations in the concentrations of gaseous pollutants are described. The power spectral densities of variations in the concentrations of carbon monoxide and nitrogen oxides are analyzed. The contributions made by variations in the concentration of carbon monoxide on different time scales to the total variance are calculated. The effect of the atmospheric air polluted with carbon monoxide and nitrogen oxides on the ecological situation in the city is estimated. The probabilities of an excess over the single maximum allowable concentrations are determined for carbon monoxide and nitrogen oxides. The absorption of shortwave solar radiation by nitrogen dioxide in the atmospheric boundary layer is estimated.     

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.