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1.
Three-year summertime surface atmospheric N2O concentrations were observed for the first time on the Fildes Peninsula, maritime Antarctica, and the relationships among the N2O concentration, total atmospheric O3 amount, and sunspot number were analyzed. Solar activity had an important effect on surface N2O concentration and total O3 amount, and increases of sunspot number were followed by decreases in the N2O concentration and total O3 amount. A corresponding relationship exists between the N2O concentration and total atmospheric O3, and ozone destruction was preceded by N2O reduction. We propose that the extended solar activity in the Antarctic summer reduces the stratospheric N2O by converting it into NOx, increases the diffusion of N2O from the troposphere to the stratosphere, decreases the surface atmospheric N2O, and depletes O3 via the chemical reaction between O3 and NOx. Our observation results are consistent with the theory of solar activity regarding the formation of the Antarctic O3 hole.  相似文献   

2.
The impacts of solar activity on climate are explored in this two-part study.Based on the principles of atmospheric dynamics,Part I propose an amplifying mechanism of solar impacts on winter climate extremes through changing the atmospheric circulation patterns.This mechanism is supported by data analysis of the sunspot number up to the predicted Solar Cycle 24,the historical surface temperature data,and atmospheric variables of NCEP/NCAR Reanalysis up to the February 2011 for the Northern Hemisphere winters.For low solar activity,the thermal contrast between the low-and high-latitudes is enhanced,so as the mid-latitude baroclinic ultra-long wave activity.The land-ocean thermal contrast is also enhanced,which amplifies the topographic waves.The enhanced mid-latitude waves in turn enhance the meridional heat transport from the low to high latitudes,making the atmospheric "heat engine" more efficient than normal.The jets shift southward and the polar vortex is weakened.The Northern Annular Mode(NAM) index tends to be negative.The mid-latitude surface exhibits large-scale convergence and updrafts,which favor extreme weather/climate events to occur.The thermally driven Siberian high is enhanced,which enhances the East Asian winter monsoon(EAWM).For high solar activity,the mid-latitude circulation patterns are less wavy with less meridional transport.The NAM tends to be positive,and the Siberian high and the EAWM tend to be weaker than normal.Thus the extreme weather/climate events for high solar activity occur in different regions with different severity from those for low solar activity.The solar influence on the midto high-latitude surface temperature and circulations can stand out after removing the influence from the El Nin o-Southern Oscillation.The atmospheric amplifying mechanism indicates that the solar impacts on climate should not be simply estimated by the magnitude of the change in the solar radiation over solar cycles when it is compared with other external radiative forcings that do not influence the climate in the same way as the sun does.  相似文献   

3.
A 3-D chemical transport model (OSLO CTM2) is used to investigate the impact of the increase of NOx emission over China. The model is capable to reproduce basically the seasonal variation of surface NOx and ozone over eastern China. NOx emission data and observations reveal that NOx over eastern China increases quite quickly with the economic development of China. Model results indicate that NOx concentration over eastern China increasingly rises with the increase of NOx emission over China, and accelerates to increase in winter. When the NOx emission increases from 1995 to its double, the ratio of NO2/NOx abruptly drops in winter over northern China. Ozone at the surface decreases in winter with the continual enhancement of the NOx level over eastern China, but increases over southern China in summertime. It is noticeable that peak ozone over northern China increases in summer although mean ozone changes little. In summer, ozone increases in the free troposphere dominantly below 500 hPa.Moreover, the increases of total ozone over eastern China are proportional to the increases of NOx emission.In a word, the model results suggest that the relationship between NOx and ozone at the surface would change with NOx increase.  相似文献   

4.
The air quality model CMAQ-MADRID (Community Multiscale Air Quality-Model of Aerosol Dynamics, Reaction, Ionization and Dissolution) was employed to simulate summer O3 formation in Beijing China, in order to explore the impacts of four heterogeneous reactions on O3 formation in an urban area. The results showed that the impacts were obvious and exhibited the characteristics of a typical response of a VOC-limited regime in the urban area. For the four heterogeneous reactions considered, the NO2 and HO2 heterogeneous reactions have the most severe impacts on O3 formation. During the O3 formation period, the NO2 heterogeneous reaction increased new radical creation by 30%, raising the atmospheric activity as more NO→NO2 conversion occurred, thus causing the O3 to rise. The increase of O3 peak concentration reached a maximum value of 67 ppb in the urban area. In the morning hours, high NO titration reduced the effect of the photolysis of HONO, which was produced heterogeneously at night in the surface layer. The NO2 heterogeneous reaction in the daytime is likely one of the major reasons causing the O3 increase in the Beijing urban area. The HO2 heterogeneous reaction accelerated radical termination, resulting in a decrease of the radical concentration by 44% at the most. O3 peak concentration decreased by a maximum amount of 24 ppb in the urban area. The simulation results were improved when the heterogeneous reactions were included, with the O3 and HONO model results close to the observations.  相似文献   

5.
During the period between 18 August and 22 September 2006, an ultraviolet photometric O3 analyzer, a NO-NO2-NOx chemiluminescence analyzer, and a quartz micro-oscillating-scale particle concentration analyzer were simultaneously used for monitoring at three different heights each at Beijing (325-m tower) and Tianjin (255-m tower). These towers belong to the Institute of Atmospheric Physics (IAP) of the Chinese Academy of Sciences (CAS) and to the Tianjin Municipal Meteorological Bureau, respectively. These measurements were used to continuously measure the atmospheric O3 and NOx volume-by-volume concentrations and the PM2.5 mass concentration within a vertical gradient. When combined with meteorological data and information on the variation of vertical characteristics of the various atmospheric pollutants in the two cities, analysis shows that these two cities were seriously polluted by both PM2.5 and O3 during summer and autumn. The highest daily-average concentrations of PM2.5 near the ground in Beijing and Tianjin reached 183 μg m-3 and 165 μg m-3, respectively, while the O3 concentrations reached 52 ppb and 77 ppb, and NOx concentrations reached 48 ppb and 62 ppb for these two cities, respectively. The variations in the daily-average concentrations of PM2.5 between Beijing and Tianjin were demonstrated to be consistent over time. The concentrations of PM2.5 measured in Beijing were found to be higher than those in Tianjin. However, the overall O3 concentrations near the ground in Tianjin were higher than in Beijing. NOx concentrations in Tianjin were consistently lower than in Beijing. It was also found that PM2.5 pollution in Beijings atmosphere may also be affected by the pollutants originating in and delivered from Tianjin, and that Ti  相似文献   

6.
Production and destruction processes of carbon monoxide (CO) and ozone (O3) are examined in the light of increasing amount of atmospheric carbon dioxide (CO2). It is found that doubling of CO2 will increase the stratospheric concentration of CO and will have positive effect on O3 concentration.  相似文献   

7.
The seasonal cycle of atmospheric CO2 at surface observation stations in the northern hemisphere is driven primarily by net ecosystem production (NEP) fluxes from terrestrial ecosystems. In addition to NEP from terrestrial ecosystems, surface fluxes from fossil fuel combustion and ocean exchange also contribute to the seasonal cycle of atmospheric CO2. Here the authors use the Goddard Earth Observing System-Chemistry (GEOS-Chem) model (version 8-02-01), with modifications, to assess the impact of these fluxes on the seasonal cycle of atmospheric CO2 in 2005. Modifications include monthly fossil and ocean emission inventories. CO2 simulations with monthly varying and annual emission inventories were carried out separately. The sources and sinks of monthly averaged net surface flux are different from those of annual emission inventories for every month. Results indicate that changes in monthly averaged net surface flux have a greater impact on the average concentration of atmospheric CO2 in the northern hemisphere than on the average concentration for latitudes 30-90°S in July. The concentration values differ little between both emission inventories over the latitudinal range from the equator to 30°S in January and July. The accumulated impacts of the monthly averaged fossil and ocean emissions contribute to an increase of the total global monthly average of CO2 from May to December.An apparent discrepancy for global average CO2 concentration between model results and observation was because the observation stations were not sufficiently representative. More accurate values for monthly varying net surface flux will be necessary in future to run the CO2 simulation.  相似文献   

8.
We used a fully coupled chemistry–climate model(version 3 of the Whole Atmosphere Community Climate Model,WACCM3) to investigate the effect of methane(CH4) emission increases,especially in East Asia and North America,on atmospheric temperature,circulation and ozone(O3). We show that CH4 emission increases strengthen westerly winds in the Northern Hemisphere midlatitudes,accelerate the Brewer–Dobson(BD) circulation,and cause an increase in the mass flux across the tropopause. However,the BD circulation in the tropics between 10?S and 10?N at 100 h Pa weakens as CH4 emissions increase in East Asia and strengthens when CH4 emissions increase in North America. When CH4 emissions are increased by 50% in East Asia and 15% globally,the stratospheric temperature cools by up to 0.15 K,and the stratospheric O3 increases by 45 ppbv and 60 ppbv,respectively. A 50% increase of CH4 emissions in North America(with an amplitude of stratospheric O3 increases by 60 ppbv) has a greater influence on the stratospheric O3 than the same CH4 emissions increase in East Asia. CH4 emission increases in East Asia and North America reduce the concentration of tropospheric hydroxyl radicals(4% and 2%,respectively) and increase the concentration of mid-tropospheric O3(5% and 4%,respectively) in the Northern Hemisphere midlatitudes. When CH4 emissions increase in East Asia,the increase in the tropospheric O3 concentration is largest in August. When CH4 emissions increase in North America,the increase in the O3 concentration is largest in July in the mid-troposphere,and in April in the upper troposphere.  相似文献   

9.
The long-term trends of total surface solar radiation(SSR),surface diffuse radiation,and surface air temperature were analyzed in this study based on updated 48-yr data from 55 observational stations in China,and then the correlation between SSR and the diurnal temperature range(DTR) was studied.The effect of total solar radiation on surface air temperature in China was investigated on the basis of the above analyses.A strong correlation between SSR and DTR was found for the period 1961-2008 in China.The highest correlation and steepest regression line slope occurred in winter,indicating that the solar radiation effect on DTR was the largest in this season.Clouds and water vapor have strong influences on both SSR and DTR,and hence on their relationship.The largest correlations between SSR and DTR occurred in wintertime in northern China,regardless of all-day(including clear days and cloudy days) or clear-day cases.Our results also showed that radiation arriving at the surface in China decreased significantly during 1961-1989(dimming period),but began to increase during 1990-2008(brightening period),in agreement with previous global studies.The reduction of total SSR offset partially the greenhouse warming during 1961-1989.However,with the increase of SSR after 1990,this offsetting effect vanished;on the contrary,it even made a contribution to the accelerated warming.Nonetheless,the greenhouse warming still played a controlling role because of the increasing of minimum and mean surface temperatures in the whole study period of 1961-2008.We estimated that the greenhouse gases alone may have caused surface temperatures to rise by 0.31-0.46℃(10 yr) 1 during 1961-2008,which is higher than previously estimated.Analysis of the corresponding changes in total solar radiation,diffuse radiation,and total cloud cover indicated that the dimming and brightening phenomena in China were likely attributable to increases in absorptive and scattering aerosols in the atmosphere,respectively.  相似文献   

10.
11.
The heterogeneous interaction of nitrogen dioxide with ammonium chloride was investigated in a molecular diffusion tube experiment at 295–335 K and interpreted using Monte Carlo trajectory calculations. The surface residence time (τsurf) of NO2 on NH4Cl is equal to 15 μs at 295 K, increases with temperature up to 323 K (τsurf = 45 μs) and probably decreases beyond 323 K. The same experiment also yields uptake coefficients, γ, which are derived from the absolute number of surviving molecules effusing out of the diffusion tube. The rate of uptake of NO2 on NH4Cl followed a rate law first order in [NO2] and the uptake coefficient γ is equal to 7 × 10−5 at 295 K, increases with temperature up to 323 K (γ = 2.1 × 10−4) and probably decreases beyond 323 K. Nitrous acid, water and nitrogen were detected as products. From these products, it is concluded that the reaction of NO2 with NH4Cl is a reverse disproportionation reaction where two moles of NO2 result in ammonium nitrite, NH4NO2, as an intermediate, and nitryl chloride, NO2Cl. NH4NO2 decomposes in two pathways, one to nitrous acid, HONO and NH3, the other to nitrogen and water. The branching ratio for the production of HONO + NH3 to that of N2 + H2O is approximately 20 at 298 K and increases with increasing temperature.  相似文献   

12.
The gas-phase degradation of NH3 in the atmosphere still has many uncertainties. One of them is the possible isomerisation of NH2O to NHOH, as indicated by kinetic studies. Since NH2O is formed during the gas-phase oxidation of ammonia in the troposphere, this reaction can potentially influence the subsequent production of N2O and NOx. So far, the isomerisation has never been implemented into current chemical schemes describing the atmospheric gas-phase degradation of NH3 and its atmospheric relevance has never been assessed. The N2O yield from NH3 degradation is calculated to be in the range of 10–43 %. It depends on the NO2 and O3 concentrations, but is independent of the NH3 concentration. Compared with the results from recent literature, the N2O yield derived from the new mechanism is 20–80% lower, implying a smaller global N2O source strength of 0.4 Tg yr- 1. The production of NH2SO2 seems to be less important for the atmospheric degradation of NH3. NH3 oxidation is a sink for NOx at NOx mixing ratios of more than about 1 ppb and a source at lower NOx burdens.  相似文献   

13.
A new complex earth system model consisting of an atmospheric general circulation model, an ocean general circulation model, a three-dimensional ice sheet model, a marine biogeochemistry model, and a dynamic vegetation model was used to study the long-term response to anthropogenic carbon emissions. The prescribed emissions follow estimates of past emissions for the period 1751–2000 and standard IPCC emission scenarios up to the year 2100. After 2100, an exponential decrease of the emissions was assumed. For each of the scenarios, a small ensemble of simulations was carried out. The North Atlantic overturning collapsed in the high emission scenario (A2) simulations. In the low emission scenario (B1), only a temporary weakening of the deep water formation in the North Atlantic is predicted. The moderate emission scenario (A1B) brings the system close to its bifurcation point, with three out of five runs leading to a collapsed North Atlantic overturning circulation. The atmospheric moisture transport predominantly contributes to the collapse of the deep water formation. In the simulations with collapsed deep water formation in the North Atlantic a substantial cooling over parts of the North Atlantic is simulated. Anthropogenic climate change substantially reduces the ability of land and ocean to sequester anthropogenic carbon. The simulated effect of a collapse of the deep water formation in the North Atlantic on the atmospheric CO2 concentration turned out to be relatively small. The volume of the Greenland ice sheet is reduced, but its contribution to global mean sea level is almost counterbalanced by the growth of the Antarctic ice sheet due to enhanced snowfall. The modifications of the high latitude freshwater input due to the simulated changes in mass balance of the ice sheet are one order of magnitude smaller than the changes due to atmospheric moisture transport. After the year 3000, the global mean surface temperature is predicted to be almost constant due to the compensating effects of decreasing atmospheric CO2 concentrations due to oceanic uptake and delayed response to increasing atmospheric CO2 concentrations before.  相似文献   

14.
Black carbon(BC) reduces the photolysis coefficient by absorbing solar radiation, thereby affecting the concentration of ozone(O_3) near the ground. The influence of BC on O_3 has thus received much attention. In this study, Mie scattering and the tropospheric Ultraviolet and Visible radiation model are used to analyze the effect of BC optical properties on radiation. Combined with data of O_3 precursors in Nanjing in 2014, an EKMA curve is drawn, and the variations in O_3 concentration are further investigated using a zero-dimensional box mechanism model(NCAR MM). When O_3 precursors are unchanged, radiation and O_3 show a highly similar tendency in response to changing BC optical properties(R=0.997).With the increase of modal radius, the attenuation of fresh BC to radiation and O_3 first trends upward before decreasing. In the mixing process, the attenuation of BC to radiation and O_3 presents an upward tendency with the increase of relative humidity but decreases rapidly before increasing slowly with increasing thickness of coating. In addition, mass concentration is another major factor. When the BC to PM2.5 ratio increases to 5% in Nanjing, the radiation decreases by approximately 0.13%–3.71% while O_3 decreases by approximately 8.13%–13.11%. The radiative effect of BC not only reduces O_3 concentration but also changes the EKMA curve. Compared with the NOx control area, radiation has a significant influence on the VOCs control area. When aerosol optical depth(AOD) increases by 17.15%, the NOx to VOCs ratio decreases by 8.27%, and part of the original NOx control area is transferred to the VOCs control area.  相似文献   

15.
中国地区臭氧前体物对地面臭氧的影响   总被引:5,自引:1,他引:4  
利用GEOS-Chem模式的数值试验结果,研究中国地区NOx和两类VOCs对O3质量浓度分布及其化学机理的影响。研究表明,NOx的减少会使得中国西部O3质量浓度显著降低,但在冬季NOx的减少会使得东北、华北地区O3质量浓度上升。而京津唐地区由于VOCs/NOx比值偏低,不能通过单一减少NOx来控制O3质量浓度。VOCs排放的减少会使得我国东部地区O3质量浓度大幅减少,其中人为VOCs的减少能降低我国东部地面O3质量浓度,而生物VOCs的减少只能在夏秋季有效减少我国东部地区35°N以南区域的地面O3质量浓度。控制地面O3质量浓度时,中国西部主要考虑NOx的减排,东部35°N以北主要考虑AVOCs的减排,而30~35°N应同时考虑AVOCs和BVOCs的减排,在30°N以南的地区,则需要全面考虑NOx和VOCs的减排。  相似文献   

16.
根据1993年10月,1995年5月和1997年4月在农业生态环境“全球500佳”-安徽省颖上县小张庄(34°47′N,116°23′E)所进行的近地面污染气体(SO2,O3,NOx)和气溶胶的观测结果,给出了这些微量气体的浓度平均概况及随时间和季节变化的一些特征,这三次观测表明,小张庄大气环境质量是持续好的,地面O3浓度主要取决于地面总辐射强度控制下的光化学反应过程;小张庄大气气溶胶粒子99%是  相似文献   

17.
应用查表法模拟区域对流层O3、Nox分布和演化的研究   总被引:2,自引:0,他引:2  
应用STEM-II气相光化学模式探讨了影响对流层O3、NOx气相光化学转化率的各物理、化学因子。表明在我国多数地区光化学污染物特征(NMHC/NOx较高)下,光辐射强度、温度、初始O3浓度和NOx浓度是影响O3、NOx气相光化学转化率的主要因子。将以上因子分档组合,计算并建立了各种情况下O3、NOx气相光化学转化率的查算表,并将之用于模拟区域O3、NOx的演化和分布。结果表明,与光化学模式直接耦合计算法相比,该方法既能显著缩短计算时间,又能基本反映大气化学反应的非线性过程,并与直接耦合法符合得较好。  相似文献   

18.
Recent studies demonstrate that the Antarctic Ozone Hole has important influences on Antarctic sea ice.While most of these works have focused on effects associated with atmospheric and oceanic dynamic processes caused by stratospheric ozone changes,here we show that stratospheric ozone-induced cloud radiative effects also play important roles in causing changes in Antarctic sea ice.Our simulations demonstrate that the recovery of the Antarctic Ozone Hole causes decreases in clouds over Southern Hemisphere(SH)high latitudes and increases in clouds over the SH extratropics.The decrease in clouds leads to a reduction in downward infrared radiation,especially in austral autumn.This results in cooling of the Southern Ocean surface and increasing Antarctic sea ice.Surface cooling also involves ice-albedo feedback.Increasing sea ice reflects solar radiation and causes further cooling and more increases in Antarctic sea ice.  相似文献   

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