Identifying anthropogenic sources of nitrogen oxide emissions from calculations of Lagrangian trajectories and the observational data from a tall tower in Siberia during the spring-summer period of 2007

The task of identifying climatically significant regional anthropogenic emissions and estimating their contribution to the variability of nitrogen oxides observed at a monitoring station is considered on the basis of NO and NO₂ surface concentrations measured at the Zotino background observation station (60°26′ N, 89°24′ E, Krasnoyarsk Territory). The approach used is based on an estimation of the conditional probability of polluted air arriving from individual regions by using the results of calculating backward Lagrangian trajectories in the lower troposphere. It is established that the contribution of air masses supplied from industrial regions in the south of the Krasnoyarsk Territory to episodes of high concentrations of nitrogen oxides (>0.7 ppb) is larger than the contribution from cities and towns located in the south of Western Siberia. The results indicate that anthropogenic sources of pollution substantially affect the balance of minor gases in the lower troposphere on a regional scale and that this factor must be taken into account when observational data from the Zotino background station are analyzed and interpreted.     

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.     

Analysis of the influence that climatic variability has on the formation of the total-ozone-content field at extratropical latitudes of the Northern Hemisphere

Having applied the method of discriminant analysis to the TOMS data of satellite sounding of the total ozone content (TOC) in the March months of 1979–2008, the authors could make a new estimate of the TOC field variability in the Northern Hemisphere and interlongitudinal regularities of its changes under the action of climatic variability. The effects of temperature variations in the polar stratosphere, El Niño, and quasi-biennial oscillation (QBO) have proven comparable and reach 80 DU in some regions. The influence of the Arctic Oscillation (AO) reaches 40 DU. The regions of TOC variations and their location and dimensions change depending on the phases of QBO, AO, and El Niño-Southern Oscillation (ENSO). Three regions of increased TOC—over Europe, Eastern Siberia, and the Pacific Ocean—are formed in years with a warm stratosphere. A compensating TOC decrease takes place in the tropics and over Greenland. In the years of El Niño and the easterly QBO phase, the TOC increases over Europe and drops over the central Pacific, as well as to the south from 45° N. The AO controls the ozone growth over most of Eurasia at temperate latitudes and its weak drop over the Atlantic. It was impossible to obtain such quantitative estimates with the use of methods based on an independent analysis of the TOC series at individual points of the coordinate grid. Testing with the Monte Carlo method confirmed that the results obtained are significant with a probability of 95–99.9%.     

A chemiluminescent technique for the determination of nanomolar concentrations of nitrate and nitrite in seawater

A chemiluminescent analysis technique for the determination of nanomolar quantities of nitrate, nitrate plus nitrite or nitrite alone in seawater is described. The method depends on the selective reduction of these species to nitric oxide which is then determined by its chemiluminescent reaction with ozone, using a commercial nitrogen oxides analyzer. The necessary equipment is compact and sufficiently sturdy to allow shipboard use. A precision of ±2 nM is claimed with analytical rates of 10–12 samples h^?1, and modifications are discussed to allow doubling the analytical rate.     

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.     

Studying seasonal variations in carbonaceous aerosol particles in the atmosphere over central Siberia

The results of 2-year (2010–2012) measurements of the concentrations of organic carbon (OC) and elemental carbon (EC), which were taken at the Zotino Tall Tower Observatory (ZOTTO) Siberian background station (61° N, 89° E), are given. Despite the fact that this station is located far from populated areas and industrial zones, the concentrations of OC and EC in the atmosphere over boreal forests in central Siberia significantly exceed their background values. In winter and fall, high concentrations of atmospheric carbonaceous aerosol particles are caused by the long-range transport (~1000 km) of air masses that accumulate pollutants from large cities located in both southern and southwestern regions of Siberia. In spring and summer, the pollution level is also high due to regional forest fires and agricultural burning in the steppe zone of western Siberia in the Russian–Kazakh border region. Background concentrations of carbonaceous aerosol particles were observed within relatively short time intervals whose total duration was no more than 20% of the entire observation period. In summer, variations in the background concentrations of OC closely correlated with air temperature, which implies that the biogenic sources of organic-particle formation are dominating.     

Spectral-temporal structure of variations in the atmospheric total ozone in central Eurasia

The results of long-term (1980–2003) systematic measurements of the total ozone content at the Issyk Kul station (42.6° N, 77.0° E; 1650 m above sea level) are presented. The statistical characteristics and spectral structure of variations in the total ozone and the main tendencies of its temporal variability are determined. It is found that the total ozone content decreased in 1980–2003 at an average rate of (?1.29±0.08) DU/yr. The results of Fourier and wavelet analyses have shown that only oscillations with periods of 12, 27–29, and 102–105 months are rather stable and can be represented as harmonic oscillations. Oscillations with periods shorter than six months have the character of periodically arising pulsations. Among these, oscillations with periods of 27–29 and 34–37 days can be distinguished. It is noted that the spectral-temporal structure of variations in the total ozone content obtained from ground-based measurements at the Issyk Kul station is in good agreement with the corresponding structure obtained from TOMS satellite measurements.     

Simulation of the impact of thunderstorm activity on atmospheric gas composition

A chemistry-climate model of the lower and middle atmosphere has been used to estimate the sensitivity of the atmospheric gas composition to the rate of thunderstorm production of nitrogen oxides at upper tropospheric and lower stratospheric altitudes. The impact that nitrogen oxides produced by lightning have on the atmospheric gas composition is treated as a subgrid-scale process and included in the model parametrically. The natural uncertainty in the global production rate of nitrogen oxides in lightning flashes was specified within limits from 2 to 20 Tg N/year. Results of the model experiments have shown that, due to the variability of thunderstorm-produced nitrogen oxides, their concentration in the upper troposphere and lower stratosphere can vary by a factor of 2 or 3, which, given the influence of nitrogen oxides on ozone and other gases, creates the potential for a strong perturbation of the atmospheric gas composition and thermal regime. Model calculations have shown the strong sensitivity of ozone and the OH hydroxyl to the amount of lightning nitrogen oxides at different atmospheric altitudes. These calculations demonstrate the importance of nitrogen oxides of thunderstorm origin for the balance of atmospheric odd ozone and gases linked to it, such as ozone and hydroxyl radicals. Our results demonstrate that one important task is to raise the accuracy of estimates of the rate of nitrogen oxide production by lightning discharges and to use physical parametrizations that take into account the local lightning effects and feedbacks arising in this case rather than climatological data in models of the gas composition and general circulation of the atmosphere.     

Simulation of changes in global ozone and atmospheric dynamics in the 21st century with the chemistry-climate model SOCOL

The solar climate ozone links (SOCOL) three-dimensional chemistry-climate model is used to estimate changes in the ozone and atmospheric dynamics over the 21st century. With this model, four numerical time-slice experiments were conducted for 1980, 2000, 2050, and 2100 conditions. Boundary conditions for sea-surface temperatures, sea-ice parameters, and concentrations of greenhouse and ozone-depleting gases were set following the IPCC A1B scenario and the WMO A1 scenario. From the model results, a statistically significant cooling of the model stratosphere was obtained to be 4–5 K for 2000–2050 and 3–5 K for 2050–2100. The temperature of the lower atmosphere increases by 2–3 K over the 21st century. Tropospheric heating significantly enhances the activity of planetary-scale waves at the tropopause. As a result, the Eliassen-Palm flux divergence considerable increases in the middle and upper stratosphere. The intensity of zonal circulation decreases and the meridional residual circulation increases, especially in the winter-spring period of each hemisphere. These dynamic changes, along with a decrease in the concentrations of ozone-depleting gases, result in a faster growth of O₃ outside the tropics. For example, by 2050, the total ozone in the middle and high latitudes approaches its model level of 1980 and the ozone hole in Antarctica fills up. The superrecovery of the model ozone layer in the middle and high latitudes of both hemispheres occurs in 2100. The tropical ozone layer recovers far less slowly, reaching a 1980 level only by 2100.     

Relationships between interannual variations in stratospheric warmings, tropospheric circulation, and sea surface temperature in the Northern Hemisphere

The leading modes of interannual and long-term variations in the stratospheric and tropospheric circulation and total ozone (TOMS data) and their relations to Northern Hemisphere sea surface temperature (SST) anomalies are investigated using the monthly mean NCEP/NCAR reanalysis data for the winter months of 1958–2003. Strong correlations are indicated between the interannual total ozone variations over Labrador and the North Atlantic and changes in the stratospheric polar vortex. The onset of major stratospheric warmings is connected not only with the strengthening of westerlies at the 500-hPa level in the midlatitude Atlantic, but also with the weakening of tropospheric winds over the north of eastern Siberia and strengthening over the Far East. In years with major stratospheric warmings, abnormally cold winters are observed in Eurasia, especially in eastern Siberia and northeastern China. The calculated simultaneous (with no time lags) correlations of the stratospheric circulation changes with El Niño/La Niña events give evidence of low correlations between the tropical Pacific SST anomalies and the stratospheric dynamics in the Arctic. However, there are high correlations of the extratropical Pacific and Atlantic SST anomalies with interannual tropospheric and stratospheric circulation variations, the stratospheric dynamics being more strongly connected with Pacific SST than with Atlantic SST anomalies. The interannual changes in tropospheric circulation are coupled to SST anomalies in both the Pacific and the Atlantic. Mechanisms of long-term changes in the interactive ocean-atmosphere-ozone layer system are discussed.     

Interannual variations and trends in zonal mean series of total ozone, temperature, and zonal wind

The paper considers zonal mean (65° S–65° N, with a step of 5°) monthly mean NCEP/DOE reanalysis data on zonal wind and temperature at levels of 20 to 100 mb and the TOMS data of version 8 on total ozone (TO) for the period 1979–2005. The results of calculating linear-trend coefficients, correlation coefficients, and characteristic decay times and the data of spectral analysis are presented. In recent decades, the decrease in TO and the cooling of the lower stratosphere were accompanied by a weakening of the westerly wind. For deseasonalized series, the significance of their linear trends are evaluated with the use of the Monte Carlo method and it is shown that TO trends are significant at a level of 0.99 in extratropical latitudinal zones and that temperature trends are significant everywhere except in a narrow equatorial zone and in latitudes south of 50° S, whereas wind trends are significant only at a 50-mb level in the latitudinal belt 30°–50° in both hemispheres. According to the results of spectral analysis, for the majority of latitudinal zones, a triplet in the range of quasibiennial oscillations and oscillations with periods of about 4–6 and 9–13 years manifest themselves most persistently in the series of temperature, wind, and TO. Maximum correlation coefficients of the series of TO, wind, and temperature are observed over the equator, and, depending on altitude and latitude, TO variations may lag or lead temperature and wind variations in phase. Latitudinal distributions of characteristic decay times show an increase in this parameter in tropical and equatorial zones and its opposite behavior with altitude for temperature and wind fields.     

Dynamics of surface-air pollution during the passage of a cold front

The dynamics of meteorological parameters, of sodar data on the temperature stratification of the atmospheric boundary layer, and of surface contents of pollutants (nitrogen oxides, carbon monoxide, and ozone) during the passage over Moscow of a structurally complex prominent cold front are discussed. It is shown that the cold front passage is accompanied by stepwise increases in the NO, NO₂, and CO surface contents. A probable cause of this phenomenon is a quick entrainment of smoke plumes from high-altitude sources of pollution into the surface turbulent air near the frontal boundary. Intense advection of cold air at the rear of the cyclone can lead to the development of an unstable stratification in the atmospheric boundary layer even in the nighttime. Under these conditions, the minute-scale variability of contents of trace gases increases abruptly as compared to that occurring in the frontal zone of the cyclone prior to the passage of the front. This effect is statistically significant. The dynamics of surface ozone reflects an increase in its background concentrations in arctic air masses.     

Effect that jet streams have on the vertical ozone distribution and characteristics of tropopause inversion layer in the far east region

The paper describes a lidar and presents the results of lidar sensing of the vertical ozone distribution (VOD); the lidar measurements are analyzed together with data from a network of meteorological stations situated along the 132° E meridian. VODs over Primorye and Japan in the winter period are compared. An analysis showed that an interrelation exists between the subtropical jet stream and the structures of VOD and tropopause inversion layer. Specifically, the region of the VOD local maximum above the tropopause is in the upper part of the tropopause inversion layer and the width of the maximum depends on the distance from the core of the subtropical jet stream. It is found that the local ozone minimum in the lower stratosphere corresponds to the local minimum of the squared Brunt-Vaisala frequency within this same altitude range in the winter season, when two tropopauses frequently overlap. It is conjectured that the local ozone maximum and tropopause inversion layer may be associated with mixing processes in the layer where stratospheric and tropospheric circulation cells come into contact near the core of the subtropical jet stream.     

Spatio-Temporal Variability of the Phase of Total Ozone Quasi-Decennial Oscillations

The SBUV/SBUV2 (65° S–65° N) and Bodeker Scientific (90° S–90° N) satellite databases have been used for composite and cross-wavelet analyses of the spatio-temporal variability of phase relations between a 11-year cycle of solar activity (SA) and quasi-decennial oscillations (QDOs) of total ozone content (TOC). For globally average TOC values, the QDO maxima coincide in phase with the solar-activity maxima, and amplitude variations of TOC correlate with those of the 11-year solar cycle. According to the analysis of amplitude and phase of QDOs for the zonal average TOC fields, a QDO amplitude is about 6–7 Dobson Units (DU) in the high northern and southern latitudes, and it does not exceed 2–3 DU in the tropic regions. The latitudinal TOC variations are distinguished by a delay of the quasi-decennial oscillation phase in the southern latitudes in comparison with the northern latitudes. The TOC maxima phase coincides with the SA maxima phase in the tropic regions; the TOC variations go ahead of the SA variations, on average, in moderate and high latitudes of the Northern Hemisphere; the TOC variations are behind the SA variations in the Southern Hemisphere. The phase delay between TOC QDO maxima in the northern and southern latitudes appears to increase in the course of time, and the TOC quasi-decennial variations in the Arctic and Antarctic subpolar regions occur approximately in an antiphase over the last two decades.     

Effect of certain geo-and heliophysical factors on the variability of ozone and UV irradiance fields in the tropics

The variability of the fields of the total ozone content (TOC) and UV erythemal irradiance in the tropical region (30°S–30°N) is studied. The fields of monthly means of the TOC and erythemal irradiance that are based on the TOMS 8 and SBUV 8 satellite observations over the period from 1979 through 2003, with preliminarily eliminated the linear trend and the seasonal cycle, were used as the initial data. The application of the method of empirical orthogonal functions (EOFs) to analysis of initial series made it possible to identify the characteristic spatial and temporal patterns in the fields of TOC and UV-irradiance anomalies that are closely related to solar activity and elements of the atmospheric general circulation, such as the quasi-biennial oscillation and El Niño (La Niña) phenomena. Quantitative estimates and analysis of the fields of TOC and UV-irradiance variations are presented in the study. The revealed spatial, temporal, and phase relations of the fields of ozone variations to some geo-and heliophysical factors are used in the regression model proposed for estimating monthly means of TOC in the tropics and based on the EOF decomposition.     

Fe–Mn-(hydr)oxide-carbonate crusts from the Kebrit Deep,Red Sea: Precipitation at the seawater/brine redoxcline

Lithified crusts located within the sediment and recovered from the Kebrit Deep (Red Sea) are composed of Fe- and Mn-(hydr)oxides, carbonates, and sulfides. Mineralogical and geochemical features of these crusts suggest that they are metalliferous layers lithified by carbonates and formed in the narrow band where the transition zone between the anoxic brine and deep seawater crossed the seafloor. Carbonates cementing the Fe–Mn-(hydr)oxides precipitated from normal saline seawater at T = 20–30 °C. Precipitation of Fe–Mn-(hydr)oxides was superimposed the carbonate precipitation in the transition zone. A pumping mechanism involving cyclic Fe- and Mn-(hydr)oxide precipitation/redissolution operated through the transition zone and produced an enrichment of a number of elements in the crusts. The microbiota played an important role in the geochemical cycle of the elements through the redoxcline and in the mineralogy of the sediments underlying the redoxcline waters. Diagenetic processes led to formation of bi- and ternary carbonates, and disulfides.     

气候变化和污染源对中国华北地区臭氧的影响

中国近年来空气污染严重,尤其是臭氧污染问题日益突出,因此,探讨全球变暖下未来气候变化和污染源等综合作用如何影响中国臭氧污染,对中国未来污染控制具有重要意义.本研究主要利用Atmospheric Chemistry and Climate Model Intercomparison Project(ACCMIP)中GFD...     

A model of the impact of solar proton events on the ionic and gaseous composition of the mesosphere

A one-dimensional ionic-photochemical model of the gaseous composition of the atmosphere that describes the formation of the D layer of the ionosphere is presented. Based on this model, the vertical profiles of the concentration of electrons and ions in the D layer of the ionosphere were calculated, as were the vertical distributions of minor gaseous constituents in the atmosphere up to a height of 86 km for undisturbed conditions and after a powerful solar proton events (SPE) at the end of October 2003. The calculations showed that SPEs significantly increase NO_x in the mesosphere of polar latitudes. In the lower mesosphere of polar caps, the NO_x mixing ratio increases by 20–50 ppb; in the upper mesosphere it increases by 100 ppb and more. High NO_x levels in zones of their formation can be retained for several weeks, producing a long-term but comparatively small ozone decrease in the lower mesosphere. The main ozone decrease is caused by a short-term HO_x increase after SPEs and is also of a short-term character in the conditions of the illuminated mesosphere. After the SPE in October 2003, model calculations yield an ozone concentration decrease by 40% in the middle and upper mesosphere at 75 ° S and by 70% at the same heights at 70 ° N. The results of modeling NO_x and O₃ changes after the SPE in October 2003 agree well with the data of satellite measurements. The changes in minor gases of the mesosphere after the SPE obtained in the model with parameterized sources of HO_x and NO_x are compared with their changes obtained in the complete ionic-photochemical model. The changes in HO_x, NO_x, and O₃ coincide rather well, whereas the changes in ClO noticeably differ, especially in the lower mesosphere. Thus, at a height of about 60 km, the parameterized photochemical model underestimated twofold the ClO formation after the SPE.     

Concentration of surface ozone, Obninsk, 2004–2010

The results of measurements of surface ozone in central European Russia in 2004–2010 are presented. The variation coefficient for hourly, monthly, and annual mean ozone concentrations is 78, 26, and 12%, respectively. The measurements established a link between increased (>60 μg/m³) and minimum (<12 μg/m³) hourly mean ozone concentrations with the existence of a temperature inversion in the lower 300-m atmospheric layer. Sixty-seven percent of the total number of increased hourly mean ozone concentrations over the 2004–2010 period took place in 2010. A maximum hourly mean ozone concentration of 218.5 μg/m³ was recorded at 17:00 on August 1, 2010. The annual mean ozone concentration in a climatically significant range of hourly mean concentrations from 12 to 60 μg/m³ increased by 45% in a linear approximation over the period of record. The spectral analysis of monthly mean concentrations of surface ozone identified composite oscillations with periods from 3 to 60 months. To approximate the temporal dynamics of ozone, a statistical model was used. This model satisfactorily describes the experimental monthly and annual mean concentrations.