Radiative Forcing of SO2 and NOx： A Case Study in Beijing

A case study was performed in Beijing in 2000 to observe concentrations of SO2 and NOx in the atmosphere and to evaluate their radiative impact. It was found that the concentrations of these gases are usually high in the morning due to a temperature inversion in the boundary layer. The average concentrations obtained from the observations are much higher than those used in the McClatchey reference atmosphere. The radiative impacts of these gases are calculated using a line-by-line radiative transfer model. The results show that the radiative forcing at the surface due to SO2 is 0.0576 W m-2 and that due to NOx is 0.0032 W m-2. These figures are almost compatible with that due to CFC11.     

Application and Study of Precipitation Schemes in Weather Simulation in Summer and Winter over China

Through simulation of summer and winter precipitation cases in China, the cloud precipitation schemes of model were examined. Results indicate that it is discrepant between convective precipitation simulated by the Kain-Fritsch (KF) scheme and Betts-Miller (BM) scheme in summer, the former scheme is better than the latter in this case. The ambient atmosphere may be varied by different convective schemes. The air is wetter and the updraft is stronger in the KF scheme than in the BM scheme, which can induce the more grid scale precipitation in the KF scheme, i.e., the different cumulus schemes may have the different and important effect on the grid scale precipitation. However, there is almost no convective rain in winter in northern China, so the effect of cumulus precipitation on the grid scale precipitation can be disregarded. Therefore, the gird scale precipitation is primary in the winter of northern China.     

Characteristics of Atmospheric Circulation Associated with Cold Surge Occurrences in East Asia： A Case Study During 2005/06 Winter

The characteristics of the upper-level circulation and thermodynamical properties for the period when two distinct cold surges broke out over East Asia during the 2005/06 winter are investigated. From early December 2005 to early January 2006, exceptionally cold weather lasted for approximately one month due to two successive cold surges that took place on 2 December 2005 and 2 January 2006, respectively. This study reveals that both involve the upper-tropospheric circulation, which induces the amplification and expansion of the surface Siberian high toward East Asia, but arose from different causes： the former is caused by the upper-level blocking originated from the North Pacific and the latter is caused by the upper-level wave train across the Eurasian Continent. In particular, it is suggested that the lower-tropospheric anomalous wind caused by upper-level circulation anomalies and a steep meridional temperature gradient amplified by phase-locked annual cycle combined to induce very strong cold advection in East Asia, which resulted in exceptionally cold weather that lasted for several weeks. The present results emphasize that the characteristics of the upper-tropospheric circulation can be considered as important precursors to cold surge occurrences in East Asia.     

Dust Storms in North China in 2002： A Case Study of the Low Frequency Oscillation

The low frequency oscillation in both hemispheres and its possible role in the dust weather storm events over North China in 2002 are analyzed as a case study. Results show that the Aleutian Low is linked with the Circumpolar Vortex in the Southern Hemisphere on a 30-60-day oscillation, with a weak Circumpolar Vortex tending to deepen the Aleutian Low which may be helpful for the generation of dust storm events. The possible mechanism behind this is the inter-hemispheric interaction of the mean meridional circulation, with the major variability over East Asia. The zonal mean westerly wind at high latitudes of the Southern Hemisphere in the upper level troposphere may lead that of the Northern Hemisphere, which then impacts the local circulation in the Northern Hemisphere. Thus, the low frequency oscillation teleconnection is one possible linkage in the coupling between the Southern Hemisphere circulation and dust events over North China. However, the interannual variation of the low frequency oscillation is unclear.     

Integration of Multi-source Measurements to Monitor Dust over North China：A Case Study

The aerosol optical depth （AOD） data from the Moderate Resolution Imaging Spectroradiometer （MODIS） aboard Satellite Aqua, along with the altitude-resolved aerosol subtypes product from the Cloud-Aerosol LIdar with Orthogonal Polarization （CALIOP）, as well as surface PM 10 measurements, were utilized to investigate the dust activities common in springtime of northern China. Specifically, a dust storm episode that occurred over the North China Plain （NCP） during 17-21 March 2010 was identified. The PM 10 concentration at Beijing （39.8 °N, 116.47 °E） reached the peak value of 283 μgm -3 on 20 March 2010 from the background value of 15 μg m-3 measured on 17 March 2010, then dropped to 176 μgm-3 on 21 March 2010. Analysis of the CALIOP aerosol subtypes product showed that numerous large dust plumes floated over northern China, downwind of main desert source regions, and were lifted to altitudes as high as 3.5 km during this time period. The MODIS AOD data provided spatial distributions of dust load, broadly consistent with ground-level PM 10 , especially in cloud free areas. However, inconsistency between the MODIS AOD and surface PM 10 measurements under cloudy conditions did exist, further highlighting the unique capability of the CALIOP lidar. CALIOP can penetrate the cloud layer to give unambiguous and altitude-resolved dust measurements, albeit a relatively long revisit period （16 days） and narrower swath （90 m）. A back trajectory simulation using the Hybrid Single-Particle Lagrangian Integrated Trajectory （HYSPLIT） model was performed, and it was found that the sand-dust storm originated from the Gobi Desert on 18 March 2010 travelled approxi-mately 1200-1500 km day-1 eastward and passed over the NCP on 19 March 2010, in good agreement with previous findings. In addition, the multi-sensor measurements integrated with the HYSPLIT model output formed a three-dimensional view of the transport pathway for this dust episode, indicating that this episode was largely associated with the desert source regions to the northwest of the NCP. The results imply the importance of integration of multi-sensor measurements for clarifying the overall structure of dust events over northern China.     

Roles of Mesoscale Terrain and Latent Heat Release in Typhoon Precipitation： A Numerical Case Study

The mesoscale orographic effects on typhoon Aere＇s precipitation are simulated using an Advanced Regional Eta-coordinate Model （AREM） version 3.0. In particular, the effects of the latent heat release are studied by two comparable experiments： with and without condensational heating. The results show that the typhoon rainfall is tripled by the southeastern China mesoscale terrain, and the condensational heating is responsible for at least half of the increase. One role of the latent heat release is to warm the atmosphere, leading to a depression of the surface pressure, which then causes a larger pressure difference in the zonal direction. This pressure gradient guides the water vapour to flow into the foothills, which in turn amplifies the water vapour flux divergence amplified, causing the typhoon rainfall to increase eventually. The other role of the latent heat release is to make the convection more organized, resulting in a relatively smaller rain area and stronger precipitation.     

A Numerical Simulation Study of Impacts of Historical Land-Use Changes on the Regional Climate in China Since 1700

By using the improved regional climate model (BCC_RegCM1.0), a series of modeling experiments are undertaken to investigate the impacts of historical land-use changes (LUCs) on the regional climate in China. Simulations are conducted for 2 years using estimated land-use for 1700, 1800, 1900, 1950, and 1990. The conversion of land cover in these periods was extensive over China, where large areas were altered from forests to either grass or crops, or from grasslands to crops. Results show that, since 1700, historical LUCs have significant effects on regional climate change, with rainfall increasing in the middle and lower reaches of the Yangtze River Basin, Northwest China, and Northeast China, but decreasing by different degrees in other regions. The air temperature shows significant warming over large areas in recent hundred years, especially from 1950 to 1990, which is consistent with the warming caused by increasing greenhouse gases. On the other hand, historical LUCs have obvious effects on mean circulation, with the East Asian winter and summer monsoonal flows becoming more intensive, which is mainly attributed to the amplifled temperature difference between ocean and land due to vegetation change. Thus, it would be given more attention to the impacts of LUCs on regional climate change.     

兰州市区2002年春季3～4月近地层大气气溶胶的监测与分析

对兰州市区2002年春季3~4月近地层TSP连续观测资料进行分析,结果表明:(1)兰州市区TSP的质量浓度随着沙尘天气的发生而显著增加,沙尘天气越强,TSP的质量浓度越高,对兰州市区的空气污染越严重;(2)在不同天气情况下,兰州市区TSP与PM10的质量浓度有很好的对应关系,沙尘天气越强,其质量浓度都越高,但两者增减的比例各不相同;(3)在不同天气情况下,同级粒径粒子的质量浓度各不相同,但在同种天气情况下,各级粒径粒子质量浓度的分布规律却相同;(4)TSP样品色度的3个独立分量与空气质量有一定的对应关系,L*、a*、b*值越大,空气中沙尘含量越高,空气污染越严重,兰州市区在一般天气情况下L*、a*、b*值均较小,说明兰州市区空气污染主要以本地排放的黑色有机物为主。     

Intercomparison of NO<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>, SO<Subscript>2</Subscript>, O<Subscript>3</Subscript>, and aromatic hydrocarbons measured by a commercial DOAS system and traditional point monitoring techniques

A field-based intercomparison study of a(DOAS) instrument (OPSIS AB, Sweden) andcommercial Differential Optical Absorption Spectroscopydifferent point-sample monitoring techniques (PM, basedon an air monitoring station, an air monitoring vehicle, and various chemical methods) was conducted inBeijing from October 1999 to January 2000. The mixing ratios of six trace gases including NO, NO2, SO2,03, benzene, and toluene were monitored continuously during the four months. A good agreement betweenthe DOAS and PM data was found for NO2 and SO2. However, the concentrations of benzene, toluene,and NO obtained by DOAS were significantly lower than those measured by the point monitors. Theozone levels monitored by the DOAS were generally higher than those measured by point monitors. Theseresults may be attributed to a strong vertical gradient of the NO-O3-NO2 system and of the aromatics atthe measurement site. Since the exact data evaluation algorithm is not revealed by the manufacturer ofthe DOAS system, the error in the DOAS analysis can also not be excluded.     

Urban Atmospheric Chemistry During the PUMA Campaign 2: Radical Budgets for OH,HO<Subscript>2</Subscript> and RO<Subscript>2</Subscript>

A detailed photochemical box model was used to investigate the key reaction pathways between OH, HO₂ and RO₂ radicals during the summer and winter PUMA field campaigns in the urban city-centre of Birmingham in the UK. The model employed the most recent version of the Master Chemical Mechanism and was constrained to 15-minute average measurements of long-lived species determined in situ at the site. The results showed that in the summer, OH initiation was dominated by the reactions of ozone with alkenes, nitrous acid (HONO) photolysis and the reaction of excited oxygen atoms atoms with water. In the winter, ozone+alkene reactions were the primary initiation route, with a minor contribution from HONO photolysis. Photolysis of aldehydes was the main initiation route for HO₂, in both summer and winter. RO₂ initiation was dominated by the photolysis of aldehydes in the summer with a smaller contribution from ozone+alkenes, a situation that was reversed in the winter. At night, ozone+alkene reactions were the main radical source. Termination, under all conditions, primarily involved reactions with NO (OH) and NO₂ (OH and RCO₃). These results demonstrate the importance of ozone+alkene reactions in urban atmospheres, particularly when photolysis reactions were less important during winter and at nighttime. The implications for urban atmospheric chemistry are discussed.     

兰州市气象与污染环境背景综述

利用 196 0～ 2 0 0 0年气候统计资料和 1975～ 2 0 0 0年环境监测资料 ,从地理位置、大、小尺度气候背景、兰州市区污染源概况及主要污染物的时空分布等方面 ,分析该市的气候与污染环境背景 ,为兰州市空气质量预报方法和模式的建立提供依据     

Sources,transport, and sinks of SO<Subscript>2</Subscript> over the equatorial Pacific during the Pacific Atmospheric Sulfur Experiment

The Pacific Atmospheric Sulfur Experiment (PASE) is the first sulfur-budget field experiment to feature simultaneous flux measurements of DMS marine emissions and SO₂ deposition to the ocean surface. We make use of these data to constrain a 1-D chemical transport model to study the production and loss pathways for DMS and SO₂ over the equatorial Pacific. Model results suggest that OH is the main sink for DMS in the boundary layer (BL), and the average DMS-to-SO₂ conversion efficiency is ~73%. In an exploratory run involving the addition of 1 pptv of BrO as a second oxidant, a 14% increase in the DMS flux is needed beyond that based on OH oxidation alone. This BrO addition also reduces the DMS-to-SO₂ conversion efficiency from 73% to 60%. The possibility of non-DMS sources of marine sulfur influencing the estimated conversion efficiency was explored and found to be unconvincing. For BL conditions, SO₂ losses consist of 48% dry deposition, while transport loss to the BuL and aerosol scavenging each account for another 19%. The conversion of SO₂ to H₂SO₄ consumes the final 14%. In the BuL, cloud scavenging removes 85% of the SO₂, thus resulting in a decreasing vertical profile for SO₂. The average SO₂ dry deposition velocity from direct measurements (i.e., 0.36 cm sec⁻¹) is approximately 50% of what is calculated from the 1-D model and the global GEOS-Chem model. This suggests that the current generation of global models may be significantly overestimating SO₂ deposition rates over some tropical marine areas. Although the specific mechanism cannot be determined, speculation here is that the dry deposition anomalous results may point to the presence of a micro-surface chemical phenomenon involving partial saturation with either S(IV) and/or S(VI) DMS oxidation products. This could also appear as a pH drop in the ocean’s surface microfilm layer in this region. Finally, we propose that the enhanced SO₂ level observed in the lower free troposphere versus that in the upper BuL during PASE is most likely the result of transported DMS/SO₂-rich free-tropospheric air parcels from the east of the PASE sampling area, rather than an inadequate representation in the model of local convection.     

Urban Atmospheric Chemistry During the PUMA Campaign 1: Comparison of Modelled OH and HO<Subscript>2</Subscript> Concentrations with Measurements

Photochemical box modelling was undertaken to investigate OH and HO₂ radical chemistry during summer and winter field campaigns in the urban city-centre of Birmingham in the UK. The model employed the most recent version of the Master Chemical Mechanism (v3.1) and was constrained to 15-minute average measurements of long-lived species determined in situ at the site. The model was used to predict OH and HO₂ concentrations for comparison with measurements made by the fluorescence assay by gas expansion technique. Whilst there was generally good agreement between the modelled and measured OH concentrations, particularly during summer, there was sometimes a significant model under-prediction during daylight hours, which significantly skews the overall model: measured agreement. There were less measured data available for HO₂, but the agreement between model and measurement for the days where measurements existed were less good than for OH, with one or two exceptions. The modelled:measured ratios between the hours of 11:00–15:00 h for OH were 0.58 and 0.50 for summer and winter respectively. For HO₂, the same ratios were 0.56 in the summer and 0.49 in the winter. Sensitivity studies were conducted to attempt to understand the model-measurement discrepancy. The predicted radical concentrations were particularly sensitive to changes in NO_X concentrations. Constraining the model to the observed HO₂ concentrations made the OH predictions worse. These results highlight the fact that there are many complexities in urban areas and that more highly-instrumented campaigns are required in the future to further our understanding.     

Environmental Process and Convergence Belt of Atmospheric NO2 Pollution in North China

Both surface environmental monitoring and satellite remote sensing show that North China is one ofthe regions that are heavily polluted by NO2. Using the NO2monitoring data from 18 major cities inthe region, the tropospheric NO2 column density data from the Ozone Monitoring Instrument (OMI) onthe Aura satellite, and the observations from the China Meteorological Administration network, this paperanalyzes a regional NO2 pollution event in February 2007 over North China, examines the convergence of thepollutant, and identifies its correlation with the atmospheric background conditions. The results show thatdaily mean NO2 concentrations derived from surface observations are consistent with the mean values of theOMI measurements, with their correlation coefficient reaching 0.81. The correlations of NO2 concentrationwith general weather patterns and sequential changes of temperature structure from 925 hPa down to thesurface indicate that the weather fronts, high pressure and low pressure systems in the atmosphere play arole in changing the temporal and spatial evolutions of NO2 through removing, accumulating or convergingof the pollutant, respectively. It is also found that the eastern Taihang Mountains is most heavily pollutedby NO2 in North China. Based on a model that correlates NO2 column density with surface wind vector,the relation of the NO2 concentrations in six major cities in North China to the surrounding wind fieldis analyzed. The results show that the maximum wind field is associated with the highest frequency ofpollution events, and under certain large-scale atmospheric conditions together with the topographic effect,small- and meso-scale wind fields often act to transport and converge pollutants, and become a major factorin forming the heaviest NO2 pollution event in North China. Analysis of the causes for the severe NO2pollution event in this study may shed light on understanding, forecasting, and mitigating occurrences ofheavy NO2 pollution.     

1961-2010年安徽省大气环境容量系数变化特征分析

基于1961-2010年安徽省气象台站的定时观测资料,采用国标法计算安徽省近50年大气稳定度、混合层厚度和大气环境容量系数,并结合合肥市空气质量逐日观测数据初步分析了大气环境容量系数对空气质量的影响。结果表明：安徽省大气稳定度以中性类居多,稳定类其次;近50年来,中性类稳定度呈明显下降趋势,不稳定类和稳定类呈显著上升;不稳定类和稳定类有明显的季节差异,中性类不明显。年平均混合层厚度显著下降;春季混合层厚度在2000年左右发生转折,夏、秋、冬三季下降趋势显著;春、夏季混合层厚度高于秋、冬季,冬季最低,春季最高。安徽省大气环境容量系数以沿淮中部、大别山区南部和沿江中西部最大,淮北大部、大别山区北部和江南南部最小,各地均呈现一致的显著下降趋势,并具有明显的年代际变化特征。年内大气环境容量系数呈"双峰型"分布,秋、冬季为低值时段,大气对污染物容纳能力较差,不利于扩散和清除,空气质量较差。总的来看,1961-2010年安徽省大气稳定度显著增加,混合层厚度较明显下降、风速快速减弱是全省大气环境容量系数变小、大气自净能力减弱的最主要原因。     

Spectra of CO<Subscript>2</Subscript> and Water Vapour in the Marine Atmospheric Surface Layer

Spectra of CO₂ and water vapour fluctuations from measurements made in the marine atmospheric surface layer have been analyzed. A normalization of spectra based on Monin–Obukhov similarity theory, originally developed for wind speed and temperature, has been successfully extended also to CO₂ and humidity spectra. The normalized CO₂ spectra were observed to have somewhat larger contributions from low frequencies compared to humidity spectra during unstable stratification. However, overall, the CO₂ and humidity spectra showed good agreement as did the cospectra of vertical velocity with water vapour and CO₂ respectively. During stable stratification the spectra and cospectra displayed a well-defined spectral gap separating the mesoscale and small-scale turbulent fluctuations. Two-dimensional turbulence was suggested as a possible source for the mesoscale fluctuations, which in combination with wave activity in the vertical wind is likely to explain the increase in the cospectral energy for the corresponding frequency range. Prior to the analysis the turbulence time series of the density measurements were converted to time series of mixing ratios relative to dry air. Some differences were observed when the spectra based on the original density measurements were compared to the spectra based on the mixing ratio time series. It is thus recommended to always convert the density time series to mixing ratio before performing spectral analysis.     

The Heterogeneous Reaction of NO<Subscript>2</Subscript> with NH<Subscript>4</Subscript>Cl: A Molecular Diffusion Tube Study

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 (τ_surf) of NO₂ on NH₄Cl is equal to 15 μs at 295 K, increases with temperature up to 323 K (τ_surf = 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.