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.     

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).     

Variations of the total content of carbon monoxide over Moscow megapolis

The results of the carbon monoxide total content measurements over Moscow and Zvenigorod for 2005–2008 are compared with the same data sets for Moscow 1986–2005 and Beijing, 1992–2007. Two identical medium resolution diffraction spectrometers (resolution 0.2 cm^?1) with solar tracking system were used. The CO total content measured simultaneously over the city and over Zvenigorod Scientific Station (ZSS) of the Obukhov Institute of Atmospheric Physics, Russian Academy of Sciences (60 km west from Moscow). This method allows to isolate an urban part of CO content. The acoustic locator SODAR LATAN-3 measurements permitted us to study the influence of the carbon monoxide ventilation conditions upon level of pollution. Correlation coefficients between the urban part of CO content and average wind speed for cold and warm seasons were obtained. The data sets analysis showed a preeminent effect of the wind within boundary layer (up to 300 m) over the CO ventilation. The urban part of the CO content hasn’t increased in spite of more than quintuple increase of the motor-vehicles number in Moscow. An increase of the rural CO total column for the 1970–1985 has transformed into its virtually stable amount in between of 1986 to 2000, changed then to a decrease for 2001–2008. We noted the 2008 as “the year of the CO total column minimum” over the past decade. The effect of urban CO sources influence on the CO total column in rural area is small, i.e. on a level of 3% of the total number of measurements. The number of extremal daily values for Moscow is estimated as 5%, and 20% for Beijing.     

Effects of the equatorial quasi-biennial oscillation in the total ozone content over Russia

On the basis of ground-based measurements of total ozone content (TOC) over Russia and a number of neighboring states during 1973–2002, the amplitudes and phases of TOC variations caused by the quasi-biennial oscillation (QBO) of wind in the equatorial stratosphere are estimated for different regions and for the whole area. The seasonal dependence of the QBO effect in the TOC is analyzed. It is shown that the magnitude and even the sign of the effect depend on the relation between the equatorial QBO phase and the season. The regional empirical models of seasonally dependent QBO effects are constructed. It is found that the seasonal dependence of regional effects accounts for 4% (in the north of the area) to 20% (in the south) of the interannual variability of the TOC. The relation between the QBO effect and the 11-year cycle of solar activity is analyzed. Significant differences are revealed in the effects under the conditions of maximum and minimum solar activity. The QBO effects obtained from observations at Russian stations, satellite measurements with a TOMS instrument, and spectrometric observations of the TOC at western European stations are compared, and their satisfactory agreement is shown. An analysis of the results suggests that the QBO effects in the TOC over Russia are caused by several interacting factors and apparently reflect their regional properties.     

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.     

Carbon dioxide and carbon monoxide photoproduction quantum yields in the Delaware Estuary

Photochemical mineralization of dissolved organic matter (DOM) plays an important role in the cycling of carbon in estuarine systems. A key to modeling this process is knowledge of apparent quantum yields (AQYs) for the photochemical products. Here we determined spectral AQYs for carbon dioxide (CO₂) and carbon monoxide (CO), the main products of DOM photomineralization, along the main axis of the Delaware Estuary. Apparent quantum yields for CO₂ photoproduction were determined shipboard using a multi-spectral irradiation system. Carbon monoxide AQYs were determined in stored samples by employing a narrow band spectral irradiation system. A single AQY spectrum described carbon dioxide photochemical production within the estuary whereas CO AQY spectra varied with salinity, suggesting different precursors and mechanisms for the production of these two species. CO₂ AQYs were used along with shipboard measurements of DOM absorbance and solar irradiance to calculate photoproduction rates. Calculated CO₂ photoproduction rates agreed with directly measured rates (2 to 4 μM CO₂ d^? 1) within experimental error, supporting the further development and use of AQYs to calculate regional-scale photochemical fluxes.     

Monitoring the carbon dioxide mixing ratio in the troposphere and the methane total column over Siberia according to the data of the AIRS and IASI IR sounders

The development of the AIRS (EOS/Aqua) and IASI (MetOp) satellite hyperspectral IR sounders opens new opportunities for determining the average tropospheric carbon dioxide concentration (X_CO2 X_{CO_2 } ) and total methane content (Q_CH4 Q_{CH_4 } ) in the atmosphere from large distances, which is important in climatic studies and since the ground network for CO₂ and CH₄ observations is scarce. The improved scheme for X_CO2 X_{CO_2 } retrieval from the AIRS data, which was used to construct the X_CO2 X_{CO_2 } spatial distribution based on the AIRS data for July 2003 and 2010 covering Siberia, is presented. A similar methodology was also used to retrieve instantaneous X_CO2 X_{CO_2 } values from the cloud-cleared IASI data for July 7, 2008 and the YAK-AEROSIB experimental region. A comparison of the satellite data with quasi-synchronous aircraft observations gives an error of about 2.2 million⁻¹. The iterative physical algorithm was developed in order to retrieve Q_CH4 Q_{CH_4 } . The efficiency of the proposed algorithm was estimated during the experiments with actual IASI data covering the Siberian region during several days in July 2008. The Q_CH4 Q_{CH_4 } estimates were validated by comparing them with the spatially superimposed and quasi-synchronous Q_CH4 Q_{CH_4 } , estimates based on the AIRS data. The standard deviations of both types of estimates are not more than 3%.     

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.     

Diurnal cycling of carbon monoxide (CO) in the upper ocean near Bermuda

A coupled photochemical–physical model for the upper ocean carbon monoxide concentration is presented. The coupled model uses a spectral optical model and a number of different mixing parameterizations. It is run using the meteorological forcing conditions measured during a 9-day investigation near Bermuda in the Sargasso Sea in March 1993 in the declining phase of the spring bloom. The baseline runs of the model are successful in simulating measurements made during the campaign, and form the basis of an optimization routine to find better estimates of the production and destruction constants of the photochemical tracer. The optimized values derived in this inverse procedure depend on the mixing parameterization and the assumed dark production rate of carbon monoxide.     

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.     

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.     

胶州湾海水中一氧化碳光致生成影响因素的研究

海水中的一氧化碳(CO)主要由溶解有色有机物(CDOM)光降解产生,且CO的光致生成量受到环境因素的影响。采集了胶州湾及其河口表层水样,通过实验室模拟实验开展了不同的环境条件(辐射强度、光照时间、温度、pH和盐度)以及水体中CDOM的来源对CO光致生成的影响研究。结果表明胶州湾海水中CO的光致生成速率随辐射强度的增强、水温的升高和水体pH的增大而增大;随着光照时间的延长、水体盐度的增大而逐渐减小;不同来源的CDOM对水体中CO的光致生成速率产生了不同的影响。     

胶州湾海水中一氧化碳光致生成影响因素的研究

海水中的一氧化碳(CO)主要由溶解有色有机物(CDOM)光降解产生,且CO的光致生成量受到环境因素的影响。采集了胶州湾及其河口表层水样,通过实验室模拟实验开展了不同的环境条件(辐射强度、光照时间、温度、pH和盐度)以及水体中CDOM的来源对CO光致生成的影响研究。结果表明胶州湾海水中CO的光致生成速率随辐射强度的增强、水温的升高和水体pH的增大而增大;随着光照时间的延长、水体盐度的增大而逐渐减小;不同来源的CDOM对水体中CO的光致生成速率产生了不同的影响。     

Aerosol optical thickness and the total carbon monoxide content over the European Russia territory in the 2010 summer period of mass fires: Interrelation between the variation in pollutants and meteorological parameters

The spatial and temporal variabilities of the aerosol optical thickness (AOT) and the total carbon monoxide content (CO) in the period of development and weakening of mass forest and peatbog fires in the European Russia territory (ERT) in the summer of 2010 are investigated from data of the AOT and CO satellite observations. The intensities of aerosol and CO emissions in the period of mass fires and the ratio of the emission factors of aerosol particles and CO are estimated on the basis of calculations of the smoke and CO masses over the ERT. The interrelation between variations in the levels of the regional pollution by combustion products and the variability of meteorological parameters is investigated. Various aspects of the manifestation of radiation effects of aerosols are discussed. The synchronization of weekly signals of the AOT, CO, and meteorological parameters in the period of mass fires is noted.     

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.     

夏季东海一氧化碳的浓度分布、海-气通量和微生物消耗研究

研究了夏季东海海水中和大气中一氧化碳(CO)的浓度分布、海-气通量和表层海水中CO的微生物消耗。夏季东海大气中CO的体积分数范围为63×10-9~120×10-9,平均值为87×10-9(SD=18×10-9,n=37),呈现出近岸高,远海低和北高南低的特点。夏季东海表层海水中CO的浓度范围为0.24~5.51nmol/L,平均值为1.48nmol/L(SD=1.46,n=37),CO的浓度受太阳辐射影响明显;CO在垂直分布上表现出浓度随深度增加迅速减小的特征,浓度最大值出现在表层。调查期间表层海水中CO相比大气处于过饱和状态,过饱和系数变化范围为3.65~113.55,平均值为23.63(SD=24.56,n=37),这表明调查海域是大气中CO的源。CO的海-气通量变化范围为0.25~78.50μmol/(m2·d),平均值为9.97μmol/(m2·d)(SD=14.92,n=37)。在CO的微生物消耗培养实验中,CO的浓度随时间增长呈指数降低,消耗过程表现出一级反应的特点,速率常数KCO范围为0.043~0.32/h,平均值为0.18/h(SD=0.088,n=9),KCO与盐度之间存在负相关关系。     

Spectral characteristics of quasi-biennial oscillations of the equatorial stratospheric wind and the problem of synchronization

Spectral characteristics of the quasi-biennial oscillations (QBO) of the zonal velocity in the equatorial stratosphere are investigated in this work on the basis of data from the NCEP/NCAR and ERA40 reanalyses and numerical experiments with the atmospheric general circulation (GCM) model developed at the Institute of Numerical Mathematics, Russian Academy of Sciences (INM RAS). The problem of synchronizing QBO and semiannual oscillations (SAO) of the zonal velocity in the mesosphere is considered. It is shown that the process of synchronization to multiples of SAO periods is identifiable in the transition region between QBO and SAO. For all heights where QBO exist, their synchronization with SAO is expressed in the calculation of the period in terms of differences between the westerly maxima. The INM RAS GCM model is shown to satisfactorily reproduce the main spectral characteristics of QBO and SAO, as well as specific features of the variability of the QBO period obtained from reanalysis data. The possibility of synchronization with SAO or the annual cycle in the upper layers is shown on the basis of an investigation of QBO models with a small number of parameters, both for the absorption mechanism of planetary waves by the mean flow and for the breaking of short gravity waves. The QBO formation from different wave types, together with SAO and the annual cycle, can be considered a unified system of oscillations in the circulation of the equatorial upper atmosphere.     

Time variability of the total methane content in the atmosphere over the vicinity of St. Petersburg

The results of measuring the methane content in the entire atmospheric thickness over the St. Petersburg region are given for 1991–2007. It is shown that, within this period, the mean annual cycle of the total methane content is characterized by its maximum values in December–January and its minimum values in June–August when the annual-cycle amplitude amounts to ∼3.6%. In this case, the annual variations in the total methane content may differ significantly from the mean annual cycle obtained in some years. A statistically significant linear trend of the total CH₄ content has not been revealed for 1991–2007. The obtained values of the linear-trend index have opposite signs in the winter and summer months (positive for January 0.6 ± 0.2%/year and February 0.4 ± 0.2%/year and negative for July 0.3 ± 0.2%/year and August 0.2 ± 0.1%/year). This fact suggests the tendency for an increase in the amplitude of the annual cycle of the total CH₄ content. The results of a spectral analysis of a series of data on the total CH₄ content show that, for 1991–2007, the following harmonics are pronounced with a confidence of 95%: 12 months (annual harmonic), 32 months (quasi-biennial oscillations), and 55 months (4.5 years), which are also pronounced in the series of meteorological parameters and total ozone content.