Aerosol Optical Properties and Its Radiative Forcing over Yulin, China in 2001 and 2002

The aerosol optical properties and direct radiative forcing over the Mu Us desert of northern China, acquired through a CE318 sunphotometer of the ground-based Aerosol Robotic Network （AERONET）, are analyzed. The seasonal variations in the aerosol optical properties are examined. The effect of meteorological elements （pressure, temperature, water vapor pressure, relative humidity and wind speed） on the aerosol optical properties is also studied. Then, the sources and optical properties under two different cases, a dust event and a pollution event, are compared. The results show that the high aerosol optical depth （AOD） found in Yulin was mostly attributed to the occurrence of dust events in spring from the Mu Us desert and deserts of West China and Mongolia, as well as the impacts of anthropogenic pollutant particles from the middle part of China in the other seasons. The seasonal variation and the probability distribution of the radiative forcing and the radiative forcing efficiency at the surface and the top of the atmosphere are analyzed and regressed using the linear and Gaussian regression methods.

A Synergic Algorithm for Retrieval of Aerosol Optical Depth over Land

In this paper, a novel algorithm for aerosol optical depth（AOD） retrieval with a 1 km spatial resolution over land is presented using the Advanced Along Track Scanning Radiometer （AATSR） dual-view capability at 0.55, 0.66 and 0.87μm, in combination with the Bi-directional Reflectance Distribution Function （BRDF） model, a product of the Moderate Resolution Imaging Spectroradiometer （MODIS）. The BRDF characteristics of the land surface, i.e. prior input parameters for this algorithm, are computed by extracting the geometrical information from AATSR and reducing the kernels from the MODIS BRDF/Albedo Model Parameters Product. Finally, AOD, with a i km resolution at 0.55, 0.66 and 0.87 μm for the forward and nadir views of AATSR, can be simultaneously obtained. Extensive validations of AOD derived from AATSR during the period from August 2005 to July 2006 in Beijing and its surrounding area, against in-situ AErosol RObotic NETwork （AERONET） measurements, were performed. The AOD difference between the retrievals from the forward and nadir views of AATSR was less than 5.72%, 1.9% and 13.7%, respectively. Meanwhile, it was found that the AATSR retrievals using the synergic algorithm developed in this paper are more favorable than those by assuming a Lambert surface, for the coefficient of determination between AATSR derived AOD and AERONET mearured AOD, decreased by 15.5% and 18.5%, compared to those derived by the synergic algorithm. This further suggests that the synergic algorithm can be potentially used in climate change and air quality monitoring.

Surface Trace Gases at a Rural Site between the Megacities of Beijing and Tianjin

The North China Plain(NCP) has recently faced serious air quality problems as a result of enhanced gas pollutant emissions due to the process of urbanization and rapid economic growth.To explore regional air pollution in the NCP,measurements of surface ozone(O3),nitrogen oxides(NOx),and sulfur dioxide(SO2) were carried out from May to November 2013 at a rural site(Xianghe) between the twin megacities of Beijing and Tianjin.The highest hourly ozone average was close to 240 ppbv in May,followed by around 160 ppbv in June and July.High ozone episodes were more notable than in 2005 and were mainly associated with air parcels from the city cluster in the hinterland of the polluted NCP to the southwest of the site.For NOx,an important ozone precursor,the concentrations ranged from several ppbv to nearly 180 ppbv in the summer and over 400 ppbv in the fall.The occurrence of high NOx concentrations under calm conditions indicated that local emissions were dominant in Xianghe.The double-peak diurnal pattern found in NOxconcentrations and NO/NOx ratios was probably shaped by local emissions,photochemical removal,and dilution resulting from diurnal variations of surface wind speed and the boundary layer height.A pronounced SO2 daytime peak was noted and attributed to downward mixing from an SO2-rich layer above,while the SO2-polluted air mass transported from possible emission sources,which differed between the non-heating(September and October) and heating(November) periods,was thought to be responsible for night-time high concentrations.

Analysis for retrieval and validation results of FY-3 Total Ozone Unit (TOU)

Retrieval experiment was made for global total column ozone using the first year measurements of Total Ozone Unit (TOU) on board the second generation polar orbiting meteorological satellite of China, FY-3/A. The retrieval results were analyzed and validated by comparison with AURA/OMI, Meteop/GOME-2 global ozone products and ground-based ozone measurement data. The qualititative comparisons over the globe especially over Antarctica and the Tibetan Plateau show that the spatial and temporal distribution characteristics are consistent with OMI and GOME-2 products. The quantitative comparisons with ground-based measurements and AURA/OMI ozone product were made over 74 stations, the TOU total ozone retrieval has a 3% rms relative error compared with AURA/OMI ozone product and 4.2% rms relative error with ground-based measurements. The maximum difference between satellite retrieval and ground-based measurements was found in the Antarctica ozone hole. The TOU global ozone product is operational and distributed to all users.

A new-generation sand and dust storm forecasting system GRAPES_CUACE/Dust:Model development,verification and numerical simulation

Based on the new-generation Global/Regional Assimilation and PrEdiction System(GRAPES) developed by the Numerical Prediction Research Center,China Meteorological Administration and the Chinese Unified Atmospheric Chemistry Environment for Dust Atmospheric Chemistry Module(CUACE/Dust) developed by the Centre for Atmosphere Watch and Services(CAWAS) of the Chinese Academy of Meteorological Sciences(CAMS) ,the China sand and dust storm forecasting system GRAPES /CUACE-Dust model has been established.The latest data of land desertification,optical properties of China sand and dust aerosols,daily soil moisture and snow cover over China main land was introduced in this system.The system showed good performance in mass conservation.The comparisons of real-time prediction outputs with surface observations and aerosol indices derived from TOMS ozone spectrophotometers(TOMS AI) indicate that the model can predict the outbreak,development,transport and depletion processes of sand and dust storms accurately over China and the East Asian region.The system makes real-time quantitative prediction of a series of elements including sand and dust injection from the surface,dry and wet deposition amount,dust concentration and optical depth.We selected 7 major dust storms occurring in April 2006 and analyzed the spatiotemporal distribution patterns of dust emission,dry and wet deposition and atmospheric load in this paper.The results showed that about 225 million tons of dust were emitted into the atmosphere from the deserts over east Asia in that month.The 3 major sand and dust sources were just as the following:The deserts in northern Inner Mongolia and the boundary area around China-Mongolia were the first dust sources with a contribution of 153 million tons accounting for 68%of the total emission.The Taklimakan Desert ranked second and contributed approximately 40 million tons accounting for 17%of the dust emission.The Onqin Daga Sandland emitted about 15 million tons or 7%of the total emission.The contributions from other deserts,sandy lands and abandoned farmlands were about only 8%of the total dust emission.The total deposition over the East Asian region in April 2006 was 136 million tons.The regional distribution of dust deposition showed that the 3 major sources were also the major deposition areas.The deposition amount in the 3 major sources accounted for 78%of the total with about 135 million tons falling back to the source regions.The secondary deposition area was the China mainland downriver,where more than 2 million tons deposited accounting for 16%of the total deposition.The deposition over the region east of 120°E including China off-shore regions,Korean Peninsula,Japan and the West Pacific took only 6%of the total deposition,which was about 850000 tons.The analysis on dry and wet deposition showed that dry deposition dominated in the process,accounting for 94%of the total sand and dust depositions in the period and wet deposition only was around for 6%,since it was generally dry with less rainfall over northern China in April.

Dust direct radiative effects on the earth-atmosphere system over east Asia:Early spring cooling and late spring warming

Focusing on three dust storms occurring in spring 2001,we developed a detailed aerosol parameterization scheme and integrated it in a radiative transfer model to characterize possible impacts of solar altitude angle on dust direct radiative effects over China desert regions and the North Pacific,using actual daily solar altitude angles.Increasing solar altitude angle from early spring (or winter) to late spring (or summer) leads to increase of positive clear sky radiative forcing,and decrease of negative radiative forcing due to dust aerosols at the top of the atmosphere.Because solar altitude angle increases from early to late spring,dust-clear sky radiative forcing may change from negative to positive at the top of atmosphere,showing a change from cooling to heating of the earth-atmosphere system over high-albedo deserts and nearby regions.Over low-albedo ocean negative clear sky radiative forcing by dust may decrease,suggesting a change from strong to weak cooling on the earth-atmosphere system.The impacts of solar altitude angle on cloudy sky radiative forcing due to dust are similar to those of clear sky.Impacts of low cloud on dust radiative forcing are the same as increasing surface albedo.This causes the transition of dust cooling effects into heating effects over deserts to occur earlier,and causes decrease of negative radiative forcing over the ocean and even cause a change from weak negative radiative forcing to weak positive forcing over local areas.Even in the same East Asian desert regions and nearby areas,the strength and sign of the radiative forcings depend on storm dates and thus solar altitude angle.The nearer to early spring (or winter) a dust storm occurs,the easier it leads to negative radiative forcing at the top of atmosphere,which indicates cooling effects on the earth-atmosphere system.In contrast,the nearer to late spring (or summer) a dust storm occurs,the easier it leads to positive radiative forcing at the top of atmosphere,showing heating effects.Over East Asian deserts and nearby regions,dust layers may be regarded as cooling sources in early spring (winter) and warming sources in late spring (summer).

In-situ measurement of atmospheric CFC-11 at the Shangdianzi Global Atmosphere Watch(GAW) Regional Station

An in-situ GC-ECD system was used to measure halocarbons at Shangdianzi(SDZ) GAW regional station.In this paper,we reported observational results of atmospheric CFC-11(CCl3F) mixing ratios from April 2007 to March 2008.The CFC-11 time series showed large variability.Approximately 62% observed values were filtered as non-background data.The median,10% and 90% percentiles of CFC-11 background mixing ratios were 245.4 ppt(10-12 mol/mol),244.6 ppt and 246.1 ppt,respectively;whereas those of non-background CFC-11 mixing ratios were 254.7,246.6 and 272.1 ppt,respectively.Significant differences in background and non-background CFC-11 mixing ratios were observed between summer and autumn,mainly because of the CFC-11 stored in foam being prone to atmospheric release in hot seasons.Comparison of the SDZ data with the five AGAGE stations suggested agreement with mid-high latitude Northern Hemisphere stations MHD,THD and RPB.The SDZ data were higher than that of Southern Hemisphere stations CGO and SMO.Higher CFC-11 mixing ratios measured in different seasons were always associated with winds from the W-WSW-SW sector,indicating that the airflow coming from this wind sector has a positive contribution to CFC-11concentrations.The CFC-11 mixing ratios were higher in autumn and summer than in spring and winter,in which its mixing ratios were very close to the atmospheric background level.This was happened especially when airflow originated from the NNE-NE-ENE-E sector,indicating the air masses coming from these wind directions was relatively clean.

Trends of Tropospheric Ozone over China Based on Satellite Data(1979-2005)

Long-term trends of yearly and seasonal averages of tropospheric ozone over the whole country and some important regions of China during 1979-2005 are analyzed,based on tropospheric ozone residue(TOR) data retrieved from satellite measurements.The relationship between the TOR and Southern Oscillation Index(SOI) is studied.The results show that,over the whole country,there is a slight increase of TOR in summer and a decrease in other seasons,while the overall trend for the whole period is insignificant.There are decreasing trends of TOR over the Pearl River Delta and the Sichuan Basin.Significant increasing trends of TOR are found over the North China Plain(NCP) for all seasons except for winter,with a maximum rate of 1.10 DU per decade for summer.There are significant correlations between TOR and SOI for some regions in China but not for the NCP,suggesting that the observed increasing trend of TOR over the NCP may not be linked with changes in atmospheric circulations.

Soluble species in aerosols collected on the route of the Second Chinese National Arctic Research Expedition

Aerosol samples are collected on the route of the Second Chinese National Arctic Research Expedition from July 15 to September 28,2003. The concentration of water soluble ions （Na^＋, NH4^＋, Ca^2＋, Cl^-, MSA , SO4^2- and so on） are analyzed. By correlation analysis, the ions can be divided into three groups ： （ 1 ） Na^＋ , Mg^2＋, K^＋, Ca^2＋, Cl^-, SO4^2-, mainly from sea salt; （2） NH4^＋, NO3^-, markedly from coastal regions of the continents ; （3） Acetate, MSA, C2O4^2-, from other sources. Marine aerosols are the dominant origin, Cl^- and Na^＋ are the most dominant anion and cation, respectively and these two ions （ Na^＋ ＋Cl^- ） account for 55. 6% of the total aerosol loading. The mean equivalence ratio of NH4^＋/SO4^2- is 0.45, we suggest that ammonium and sulfate exist mainly as NH4HSO4. The concentration of NO3- shows three different patterns on the route of expedition： Japan Sea with median value of 15.2 neq · m^ -3 ; Sea of Okhostk and Bering Sea of 1.8 neq ·m ^-3 and Arctic Ocean of 0.4 neq · m^-3 Bering Sea is a high MSA area. Through the comparison of the concentration of main water soluble ions between the First and Second Chinese National Arctic Research Expedition, the variation matches each other.

Observation and analysis of near-surface atmospheric aerosol optical properties in urban Beijing

Year-round measurements of the mass concentration and optical properties of fine aerosols （PM2s） from June 2009 to May 2010 at an urban site in Beijing were analyzed. The annual mean values of the PM2.5 mass concentration, absorption coefficient （Ab）, scattering coefficient （Sc） and single scattering albedo （SSA） at 525 nm were 67 ± 66 μg/m^3, 64 ± 62 Mm^-1, 360±405 Mm^-1 and 0.82±0.09, respectively. The bulk mass absorption efficiency and scattering efficiency of the PM2.5 at 525 nm were 0.78 m^2/g and 5.55 m^2]g, respectively. The Ab and Sc showed a similar diurnal variation with a maximum at night and a minimum in the afternoon, whereas SSA displayed an opposite diurnal pattern. Significant increases in the Ab and Sc were observed in pollution episodes caused by the accumulation of pollutants from both local and regional sources under unfavorable weather conditions. Aerosol loadings in dust events increased by several times in the spring, which had limited effects on the Ab and Sc due to the low absorption and scattering efficiency of dust particles. The frequency of haze days was the highest in autumn because of the high aerosol absorption and scattering under unfavorable weather conditions. The daily PM2.5 concentration should be controlled to a level lower than 64 μg/m^3 to prevent the occurrence of haze days according to its exponentially decreased relationship with visibility.

RELATIONSHIP BETWEEN HORIZONTAL EXTINCTION COEFFICIENT AND PM_(10) CONCENTRATION IN XI'AN,CHINA,DURING 1980-2002

Based on daily visibility data obtained from 1980-2002 and air pollution index data from 2001-2004 in Xi＇an, long-term variations and relationships for daily horizontal extinction coefficient and mass concentration of PM10 have been evaluated. A decreasing trend was found in horizontal extinction coefficient during the past 23 years, with higher values observed in 1980s relative to 1990s, and the highest and lowest values in winter and summer, respectively. Significant correlation and similar seasonal variations existed between horizontal extinction coefficient and PM10 concentration, suggesting the high influence of PM10 to the visibility drop at a site in the Guanzhong Plain of central China during the past two decades.

Observed levels and trends of gaseous SO_2 and HNO_3 at Mt.Waliguan,China:Results from 1997 to 2009

Long-term measurements of SO2 and HNO3, particularly those from the background sites, are rarely reported. We present for the first time the long-term measurements of SO2 and HNO3 at Waliguan （WLG）, the only global baseline station in the back-land of the Eurasian Continent. The concentrations of SO2 and HNO3 were observed at WLG from 1997 to 2009. The observed annual mean concentrations of SO2 and HNO3 at WLG were 1.28 ± 0.41 and 0.22 ± 0.19 μg/m3, respectively. The HNO3 concentrations were much higher in warmer seasons than in colder seasons, while the SO2 concentrations showed a nearly reversed seasonal pattern. In most months, the concentration of HNO3 was significantly correlated with that of SO2, suggesting that some common factors influence the variations of both gases and the precursors of HNO3 may partially be from the SO2-emitting sources. The SO2 concentration had a very significant （P 〈 0.0001） decreasing trend （-0.2 μg/（m3.yr）） in 1997-2002, but a significant （P 〈 0.05） increasing trend （＋0.06 μg/（m3-yr）） in 2003-2009. The HNO3 concentration showed no statistically significant trend during 1997-2009. While the decrease of SO2 in 1997-2002 agrees with the trend of global SO2 emissions, the increase in 2003-2009 is not consistent with the decreasing trends in many other regions over the world. Trajectory analysis suggests that the airmasses from the northern Qinghai-Tibetan Plateau and the Takla Makan Desert regions contributed significantly to the increasing trends of SO2 and HNO3 at WLG in 2003-2009, with a rate of ＋0.13 μg/（m3.yr） and ＋0.007μg/（m3.yr）, respectively.

An improved GC-ECD method for measuring atmospheric N_2O

Gas chromatography equipped with an electron capture detector （GC-ECD） has been widely used for measuring atmospheric N2O,but nonlinear response and the influence of atmospheric CO2 have been recognized as defects for quantification.An original GCECD method using N 2 as carrier gas was improved by introducing a small flow rate of CO2 makeup gas into the ECD,which could well remedy the above defects.The N2O signal of the improved method was 4-fold higher than that of the original method and the relative standard deviation was reduced from 〉 1% to 0.31%.N2O concentrations with different CO2 concentrations （172.2×10-6-1722×10-6mol/mol） measured by the improved GC-ECD method were in line with the actual N2O concentrations.However,the N2O concentrations detected by the original method were largely biased with a variation range of-4.5%～7%.The N2O fluxes between an agricultural field and the atmosphere measured by the original method were greatly overestimated in comparison with those measured by the improved method.Good linear correlation （R2=0.9996） between the response of the improved ECD and N2O concentrations （93×10-9-1966×10-9mol/mol） indicated that atmospheric N2O could be accurately quantified via a single standard gas.Atmospheric N2O concentrations comparatively measured by the improved method and a high precision GC-ECD method were in good agreement.

Trends of the precipitation acidity over China during 1992–2006

The trends of the precipitation acidity from 1992 to 2006 were studied, based on the long-term acid rain observations at 74 sites in China. The results show that there was no remarkable change or extension of acid rain area (i.e., with annual mean of precipitation pH<5.6) during the 15 years. The largest and continuous acid rain area exists in the south of the Yangtze River, while the acid rain areas north of the Yangtze River remain separate. The severe acid rain area (i.e., with annual mean of precipitation pH<4.5) exists mainly in the south of the Yangtze River. The overall precipitation acidity for the 74 stations showed different trends before 1999 and after 2000. In the period 1992–1999, the precipitation acidity at most of the sites remained steady or showed a decreasing trend. After 2000, however, an increasing trend of the precipitation acidity was observed at many sites in North China, Central China, East China, and South China. As a result, the pattern of acid rain area changed during 1992–2006. The precipitation over North China, Central China, and South China became more acidified in the 15 years, with more pronounced trends in North China and the north of Central China. A slight decrease in the precipitation acidity was found in Southwest China, an area characterized as severest acid rain area for about two decades after the early 1980s. Consequently, the center of severe acid rain area in the south of the Yangtze River moved eastwards. The non-hydrogen conductivity (NHC), which is defined as the difference between the measured precipitation conductivity and the H+ conductivity calculated from measured pH, was estimated and treated as a proxy of soluble ions in precipitation. The result shows that the overall trend of the NHC before 1999 was pronounced and positive, while the trend after 2000 was inconspicuous or slightly negative. During 2000–2006, the change rate of pH was positively correlated to that of the NHC at 21 sites, implying that the increasing acidities found at these sites may partly be attributed to the decrease in the concentration of airborne particulate matter in recent years.

Chemical characteristics of precipitation at Nanping Mangdang Mountain in eastern China during spring

To study the characteristics of precipitation in eastern China, an automatic sampler was used to collect rainwater samples from 19 precipitation events at Mangdang Mountain, Nanping City, Fujiang Province, in the spring of 2009. We used ion chromatography to analyze the ionic components and concentrations, and inductively coupled plasma mass spectrometry （ICP-MS） to analyze dement compositions and contents. The results demonstrated remarkable acidic characteristics： in more than 80% of precipitation events the pH was less than 5.6, with an average of 4.81. Mass concentration results showed SO42- was the main anionic component （36.2% of the total anion mass）, while N/-/4＋ was the main cationic component （47.7% of the total cation mass） and main ion for acidity neutralization in the rainwater. Organic acid content accounted for 30.9% of total anion mass. The main trace metals were Ca, K, and Na. The S042-/N03- ratio was 1.4, indicating that precipitation in this region was influenced by complex air pollution - the product of individual coal-burning combined with vehicle exhaust pollution. Correlation analysis of the chemical composition of the precipitation indicated that acidity in this region was determined by a combination of all acidic and neutralization ions rather than any single ion component. The results also showed that Na＋ and C1- contributions were mainly by seawater; Mg2＋ by seawater and crustal materials; the NH4＋, K~, Ca2＋, NO3- and SO42- by anthropogenic sources; the trace metals were from the Earth＇s crust; and organic acids were potentially from combustion of biomass.

Impacts of aerosol chemical compositions on optical properties in urban Beijing,China

The optical properties of aerosols and their chemical composition, including water-soluble ions, organic carbon （OC）, and elemental carbon （EC） in PM2.5 and PM10, were measured from 26 May to 30 June of 2012 at an urban site in Beijing. The daily average concentrations of PM2.5 and PM10 were 103.2 and 159.6 μg/m^3, respectively. On average, the OC and EC contributed 20.1% and 4.3%, respectively, to PM2.5 and 16.3% and 3.9%, respectively, to PM10. Secondary ions （SO4^2-, NO3-, and NH4^＋） dominated the water-soluble ions and accounted for 57.9% and 62.6% of PM2.5 and PM10, respectively. The wind dependence of PM2.5, OC, SO4^2-, and NO3 implied that the pollution sources mainly came from south and southeast of Beijing during the summer. The monthly mean values of the scattering coefficient （σsc） and absorption coefficient （σab） at 525 nm were 312.9 and 28.7 Mm^-1, respectively, and the mean single-scattering albedo （ω） was 0.85. The wind dependence of σsc revealed that this value was mainly influenced by regional transport during the summer, and the relationship between aab and wind indicated that a high crab resulted from the joint effects of local emissions and regional transport. The reconstructed σsc that was derived from the revised IMPROVE equation agreed well with the observations. The contribution of different chemical species to crsc was investigated under different pollution levels, and it was found that secondary inorganic aerosols accounted for a large part of σsc during pollution episodes （35.7%）, while organic matter was the main contributor to σsc under clean conditions （33.6%）.

Climatic Trend of Cloud Amount Related to the Aerosol Characteristics in Beijing During 1950-2005

This paper analyzes the correlation between variations of total and low cloud amounts and the varying features of aerosols related to urban development of Beijing by using the cubic spline fitting method based on the monthly meteorological data of temperature,humidity,precipitation,clouds,and aerosol optical depth （AOD） during 1950-2005.The statistics on the development of the city of Beijing in this period,including the total industrial output,population,residential housing development,highway construction,charcoal production,etc.,is revealed.Accompanying the rapid urban development of Beijing over the past 55 years or so,the urban aerosol concentration and composition have changed.The results indicate that：1） there is a general trend of climate warming and drying in Beijing;2） the total cloud amount in all seasons declines drastically,but lower cloud amount climbs up slightly;3） the high correlations between cloud amount and the indices of Beijing urban development such as the housing area,charcoal production,and road construction show that the variation of cloud amount is closely related to the urban development;4） the changing trend of AOD coincides more closely with the variation of low cloud amount.The evident drop of total cloud amount is in agreement with the trend of climate warming and drying,while the slight growth of low cloud amount is likely caused by more haze and fog occurrences in the lower troposphere in association with the pollution responsible for the＂darkening＂of Beijing and the surrounding areas.