Measurements of aerosol optical depth above 3570 m asl in the North Atlantic free troposphere: results from ACE‐2

As part of the 2nd A erosol C haracterisation E xperiment (ACE‐2), conducted during summer 1997 in the North Atlantic region between the Canary Islands and Portugal, we measured aerosol optical depths (AOD) at a mid‐tropospheric site, near the top of the volcanic mountain "El Teide"(28°16'N, 16°36' W, 3570 m asl). Our instrument was located at the highest altitude in a network of sunphotometers that extended down to sea level. Clear conditions dominated the ACE‐2 period, and, although suggested by back‐trajectories at 300 hPa, no evidence of anthropogenic pollution was found in our data. Three distinct dust episodes were observed. Vertical soundings and back trajectories suggested mineral dust from the Sahel region as a source. During these episodes, AOD increased an order of magnitude with respect to background conditions (from 0.017 up to 0.19 at λ=500 nm). A shift towards neutrality of the extinction spectral dependence (Ångstrom exponent α down to 0.13), indicated that the coarse mode (particle diameter >2 μm) dominated the aerosol size distribution. For 6 days during the episodes of mineral dust, a monomodal size distribution between 2 and 20 μm diameter was obtained from Mie based size distribution calculations. Estimates, at 500 nm, of the single scattering albedo ω₀(0.87–0.96), and the aerosol asymmetry parameter g (0.72–0.73) suggest that the dust layer causes a net cooling forcing at the top of the atmosphere.     

Size‐segregated chemical, gravimetric and number distribution‐derived mass closure of the aerosol in Sagres, Portugal during ACE‐2

During the ACE‐2 field campaign in the summer of 1997 an intensive, ground‐based physical and chemical characterisation of the clean marine and continentally polluted aerosol was performed at Sagres, Portugal. Number size distributions of the dry aerosol in the size range 3–10 000 nm were continuously measured using DMPS and APS systems. Impactor samples were regularly taken at 60% relative humidity (RH) to obtain mass size distributions by weighing the impactor foils, and to derive a chemical mass balance by ion and carbon analysis. Hygroscopic growth factors of the metastable aerosol at 60% RH were determined to estimate the number size distribution at a relative humidity of 60%. A size segregated 3‐way mass closure study was performed in this investigation for the first time. Mass size distributions at 60% RH derived from number size distribution measurements and impactors samples (weighing and chemical analysis) are compared. A good agreement was found for the comparison of total gravimetrically‐determined mass with both number distribution‐derived (slope=1.23/1.09; R²>0.97; depending on the parameters humidity growth and density) and chemical mass concentration (slope=1.02; R²= 0.79) for particles smaller than 3 μm in diameter. Except for the smallest impactor size range relatively good correlations (slope=0.86–1.42) with small deviations (R²=0.76–0.98) for the different size fractions were found. Since uncertainties in each of the 3 methods are about 20% the observed differences in the size‐segregated mass fractions can be explained by the measurement uncertainties. However, the number distribution‐derived mass is mostly higher than the chemically and gravimetrically determined mass, which can be explained by sampling losses of the impactor, but as well with measurement uncertainties as, e.g., the sizing of the DMPS/APS.     

Fine mode aerosol chemistry over a tropical urban atmosphere: characterization of ionic and carbonaceous species

An extensive aerosol sampling program was conducted during January-December 2006 over Kolkata (22o33?? N and 88o20?? E), a mega-city in eastern India in order to understand the sources, distributions and properties of atmospheric fine mode aerosol (PM_2.5). The primary focus of this study is to determine the relative contribution of natural and anthropogenic as well as local and transported components to the total fine mode aerosol loading and their seasonal distributions over the metropolis. The average concentrations of fine mode aerosol was found to be 71.2?±?25.2???gm^-3 varying between 34.5???gm^-3 in monsoon and 112.6???gm^-3 in winter. The formation pathways of major secondary aerosol components like nitrate and sulphate in different seasons are discussed. A long range transport of dust aerosol from arid and semi-arid regions of western India and beyond was observed during pre-monsoon which significantly enriched the total aerosol concentration. Vehicular emissions, biomass burning and transported dust particles were the major sources of PM_2.5 from local and continental regions whereas sea-salt aerosol was the major source of PM_2.5 from marine source regions.     

A simple non‐linear analytical relationship between aerosol accumulation number and sub‐micron volume, explaining their observed ratio in the clean and polluted marine boundary layer

We propose an analytical expression for the relation between aerosol accumulation number and sub‐micron volume over the marine boundary layer (MBL), based on a simple balance equation. By providing appropriate source and sink terms which account for entrainment, coagulation, in‐cloud scavenging and condensational growth, the model is able to reproduce the observed ratio between MBL particles larger than 80 nm diameter (as a proxy for accumulation mode number) and submicron aerosol volume, from freshly polluted to background conditions. Entrainment and coagulation are essential in predicting the observed ratio. Budget and lifetime calculations show that, due to relatively low source rates of oceanic non‐sea‐salt‐sulfate and sea‐salt, the anthropogenic signature in aerosol volume remains significant even after 8 days of MBL transport.     

Dimethylsulphide production in the subantarctic southern ocean under enhanced greenhouse conditions

Dimethylsulphide (DMS) is an important sulphur‐containing trace gas produced by enzymatic cleavage of its precursor compound, dimethylsulphoniopropionate (DMSP), which is released by marine phytoplankton in the upper ocean. After ventilation to the atmosphere, DMS is oxidised to form sulphate aerosols which in the unpolluted marine atmosphere are a major source of cloud condensation nuclei (CCN). Because the micro‐physical properties of clouds relevant to climate change are sensitive to CCN concentration in air, it has been postulated that marine sulphur emissions may play a rôle in climate regulation. The Subantarctic Southern Ocean (41–53°S) is relatively free of anthropogenic sulphur emissions, thus sulphate aerosols will be mainly derived from the biogenic source of DMS, making it an ideal region in which to evaluate the DMS‐climate regulation hypothesis. We have extended a previous modelling analysis of the DMS cycle in this region by employing a coupled general circulation model (CGCM) which has been run in transient mode to provide a more realistic climate scenario. The CGCM output provided meteorological data under the IPCC/IS92a radiative forcing scenario. A DMS production model has been forced with the CGCM climate data to simulate the trend in the sea‐to‐air DMS flux for the period 1960 to 2080, corresponding to equivalent CO₂ tripling relative to pre‐industrial levels. The results confirm a minor but non‐negligible increase in DMS flux in this region, in the range +1% to +6% predicted over the period simulated. Uncertainty analysis of the DMS model predictions have confirmed the positive sign for the change in DMS flux, that is a negative DMS feedback on warming.     

An analysis of ozone measurements at Cerro Tololo (30°S, 70°W, 2200 m.a.s.l.) in Chile

Increases in tropospheric ozone (O₃) abundance are likely to take place in the near future in the populous and rapidly developing countries in the tropics and subtropics. An accurate evaluation of the future impact of increasing industrial activities in tropical and subtropical areas requires knowledge of the background levels of ozone. New ozone monitoring stations have been installed at several sites by the World Meteorological Organization (WMO) since the mid‐90s. We analyze ozone data collected during two years since April 1996 at Cerro Tololo (30°S, 70°W, 2200 m.a.s.l.) some 50 km east from the city of La Serena. In this paper, we describe some of the atmospheric chemistry and meteorology that characterizes the Tololo site. The data show a seasonal variation with maximum mixing ratios in late winter and spring and minimum mixing ratios in late summer and early fall. These variations are most likely associated with the large‐scale subsidence of the Hadley circulation and the location of the subtropical jet stream (STJ). Also, there is a diurnal variation that is probably partly associated with a mountain wind flow which is strongest in late spring and summer months. No significant mixing with marine boundary layer air perturbed by anthropogenic activities is apparent from the data. We find the Cerro Tololo site to be generally representative for background conditions of free‐tropospheric air in the subtropics of the Southern Hemisphere. This work is done within the framework of a larger effort recently started by several Chilean institutions in cooperation with research centers abroad.     

An overview of the ACE‐2 CLOUDYCOLUMN closure experiment

CLOUDYCOLUMN is one of the 6 ACE‐2 projects which took place in June‐July 1997, between Portugal and the Canary Islands. It was specifically dedicated to the study of changes of cloud radiative properties resulting from changes in the properties of those aerosols which act as cloud condensation nuclei. This process is also refered to as the aerosol indirect effect on climate. CLOUDYCOLUMN is focused on the contribution of stratocumulus clouds to that process. In addition to the basic aerosol measurements performed at the ground stations of the ACE‐2 project, 5 instrumented aircraft carried out in situ characterization of aerosol physical, chemical and nucleation properties and cloud dynamical and microphysical properties. Cloud radiative properties were also measured remotely with radiometers and a lidar. 11 case studies have been documented, from pure marine to significantly polluted air masses. The simultaneity of the measurements with the multi‐aircraft approach provides a unique data set for closure experiments on the aerosol indirect effect. In particular CLOUDYCOLUMN provided the 1st experimental evidence of the existence of the indirect effect in boundary layer clouds forming in polluted continental outbreacks. This paper describes the objectives of the project, the instrumental setup and the sampling strategy. Preliminary results published in additional papers are briefly summarized.     

A physically‐based algorithm for estimating the relationship between aerosol mass and cloud droplet number

In this study, we present a relationship between total accumulation mode aerosol mass concentrations and cloud droplet number concentrations ( N _d). The fundamental aim with the present method is to arrive at a physically‐based conversion algorithm in which each step in the conversion is based on real physical processes that occur and can be observed in the atmosphere, and in which all of the fields involved can be observed or modeled. In the last conversion (the critical part in the algorithm), we use measurements of the size distributions of cloud droplet residual particles for different pollution conditions. This conversion assumes that the size of the residual particles can be described with a lognormal distribution function and uses the Hatch–Choate relationship to convert between residual volume and number. The relatively sparse data set with which we have developed the present algorithm results in a course classification of the aerosol mass field. Consequently, uncertainties need to be recognized when using the algorithm in its present form in model calculations. The algorithm has been used on data from 15 days and the agreement between calculated and observed N _d values is, with one exception, within a factor of 2 and for many of these cases also much better than a factor of 2. In addition to the results of the algorithm itself, we also present a least‐squares fit to the predicted N _d values. To improve the algorithm in the longer‐term requires more data of scavenging fractions, particle chemical composition and density, and residual particle size distributions as a function of aerosol mass loading and cloud type.     

Chemical components of lower tropospheric aerosols in the high arctic: Six years of observations

Six years of observations (1980 to 1986) of the composition of lower tropospheric aerosols at Alert on northern Ellesmere Island in the Canadian high Arctic yield insight into the seasonal variation of Arctic air pollutants as well as of substances of natural origin. A principal component analysis of 138 observations of 21 aerosol constituents (major ions, metals, nonmetallic trace elements) for the most polluted period of December to April identified not only a soil, sea salt and anthropogenic aerosol component, but also one associated with photochemical reactions in the atmosphere that occur at polar sunrise. Depending on the source of their gaseous precursors, elements in the photochemical component can be natural or anthropogenic in origin. For instance, SO₄ ^2-, existing mostly as H₂SO₄, originates probably from both anthropogenic and natural sources while Br^– is likely of marine origin. In contrast, SO₄ ^2- in the anthropogenic component has the stoichiometry of NH₄HSO₄. In the winter months, over 90% of Arctic SO₄ ^2- is in the anthropogenic and photochemical components.In winter, a substantial portion (11 to 35%) of Na⁺ is associated with the anthropogenic aerosol component suggesting either that marine aerosols have been physically or chemically modified by interactions with air pollution or that there are anthropogenic sources of Na⁺.The aerosol soil component is controlled by both local and distant dust sources. During a year, it has two peaks at Alert, one in April/May coinciding with the Asian dust storm season and one in September.There is a marked difference in the seasonal variation of particulate Br^– and iodine concentrations in the air. Both have a peak in April/May associated with polar sunrise and, hence, photochemical reactions in the atmosphere. However, iodine also peaks in early fall. This may be a product of biogenic iodine emissions to the atmosphere during secondary blooms in northern oceans in late summer.Presented at the Second Conference on Baseline Observations in Atmospheric Chemistry (SABOAC II) in Melbourne, Australia, November 1988     

Clear‐sky closure studies of lower tropospheric aerosol and water vapor during ACE‐2 using airborne sunphotometer, airborne in‐situ, space‐borne, and ground‐based measurements

We report on clear‐sky column closure experiments (CLEARCOLUMN) performed in the Canary Islands during the second Aerosol Characterization Experiment (ACE‐2) in June/July 1997. We present CLEARCOLUMN results obtained by combining airborne sunphotometer and in‐situ (optical particle counter, nephelometer, and absorption photometer) measurements taken aboard the Pelican aircraft, space‐borne NOAA/AVHRR data and ground‐based lidar and sunphotometer measurements. During both days discussed here, vertical profiles flown in cloud‐free air masses revealed 3 distinctly different layers: a marine boundary layer (MBL) with varying pollution levels, an elevated dust layer, and a very clean layer between the MBL and the dust layer. A key result of this study is the achievement of closure between extinction or layer aerosol optical depth (AOD) computed from continuous in‐situ aerosol size‐distributions and composition and those measured with the airborne sunphotometer. In the dust, the agreement in layer AOD (λ=380–1060 nm) is 3–8%. In the MBL there is a tendency for the in‐situ results to be slightly lower than the sunphotometer measurements (10–17% at λ=525 nm), but these differences are within the combined error bars of the measurements and computations.     

Analysis of regional budgets of sulfur species modeled for the COSAM exercise

The COSAM intercomparison exercise (comparison of large‐scale sulfur models) was organized to compare and evaluate the performance of global sulfur cycle models. Eleven models participated, and from these models the simulated surface concentrations, vertical profiles and budget terms were submitted. This study focuses on simulated budget terms for the sources and sinks of SO₂ and sulfate in three polluted regions in the Northern Hemisphere, i.e., eastern North America, Europe, and Southeast Asia. Qualitatively, features of the sulfur cycle are modeled quite consistently between models, such as the relative importance of dry deposition as a removal mechanism for SO₂, the importance of aqueous phase oxidation over gas phase oxidation for SO₂, and the importance of wet over dry deposition for removal of sulfate aerosol. Quantitatively, however, models may show large differences, especially for cloud‐related processes, i.e., aqueous phase oxidation of SO₂ and sulfate wet deposition. In some cases a specific behavior can be related to the treatment of oxidants for aqueous phase SO₂ oxidation, or the vertical resolution applied in models. Generally, however, the differences between models appear to be related to simulated cloud (micro‐)physics and distributions, whereas differences in vertical transport efficiencies related to convection play an additional rôle. The estimated sulfur column burdens, lifetimes and export budgets vary between models by about a factor of 2 or 3. It can be expected that uncertainties in related effects which are derived from global sulfur model calculations, such as direct and indirect climate forcing estimates by sulfate aerosol, are at least of similar magnitude.     

Ground‐based lidar measurements of aerosols during ACE‐2: instrument description, results, and comparisons with other ground‐based and airborne measurements

A micro‐pulse lidar system (MPL) was used to measure the vertical and horizontal distribution of aerosols during the Aerosol Characterization Experiment 2 (ACE‐2) in June and July of 1997. The MPL measurements were made at the Izaña observatory (IZO), a weather station located on a mountain ridge (28°18' N, 16°30' W, 2367 m asl) near the center of the island of Tenerife, Canary Islands. The MPL was used to acquire aerosol backscatter, extinction, and optical depth profiles for normal background periods and periods influenced by Saharan dust from North Africa. System tests and calibration procedures are discussed, and an analysis of aerosol optical profiles acquired during ACE‐2 is presented. MPL data taken during normal IZO conditions (no dust) showed that upslope aerosols appeared during the day and dissipated at night and that the layers were mostly confined to altitudes a few hundred meters above IZO. MPL data taken during a Saharan dust episode on 17 July showed that peak aerosol extinction values were an order of magnitude greater than molecular scattering over IZO, and that the dust layers extended to 5 km asl. The value of the dust backscatter–extinction ratio was determined to be 0.027±0.007 sr⁻¹. Comparisons of the MPL data with data from other co‐located instruments showed good agreement during the dust episode.     

A pseudo-Lagrangian study of the sulfur budget in the remote Arctic marine boundary layer

The atmospheric sulfur cycle of the remote Arctic marine boundary layer is studied using trajectories and measurements of sulfur compounds from the International Arctic Ocean Expedition 1991, along with a pseudo-Lagrangian approach and an analytical model. The dimethyl sulfide [DMS(g)] turnover time was  h. Only  % of DMS(g) followed reaction paths to sulfur dioxide [SO₂(g)], sub-micrometre aerosol non-seasalt sulfate (nss-SO₄²⁻) or methane sulfonate (MSA). During the first 3 d of transport over the pack ice, fog deposition and drizzle resulted in short turnover times;  h for SO₂(g),  h for MSA and  h for nss-SO₄²⁻. Therefore, DMS(g) will, owing to its origin along or south of the ice edge and longer turnover time, survive the original sub-micrometre sulfur aerosol mass and gradually replace it with new biogenic sulfur aerosol mass. The advection of DMS(g) along with heat and moisture will influence the clouds and fogs over the Arctic pack ice through the formation of cloud condensation nuclei (CCN). If the pack ice cover were to decrease owing to a climate change, the total Arctic Ocean DMS production would change, and potentially there could be an ice–DMS–cloud–albedo climate feedback effect, but it would be accompanied by changes in the fog aerosol sink.     

利用MODIS光学厚度遥感产品研究北京及周边地区的大气污染

对2001年在北京地区利用太阳光度计观测的气溶胶光学厚度和NASA发布的MODIS气溶胶产品进行了比较,验证了这一卫星遥感产品的可靠性;比较了2001年MODIS气溶胶光学厚度(AOD)产品和由空气污染指数(API)计算的每日平均可吸入颗粒物(PM10)浓度,得到了比较高的相关系数,证实该气溶胶产品可用于污染分析.将北京地区AOD与气象能见度观测资料进行比较,得到了不同季节的气溶胶"标高".利用统计的不同季节的气溶胶标高,从光学厚度的季节分布得到了能见度(能见距离)的季节分布.气溶胶光学厚度图像的个例分析表明,除局地排放外,周边区域(主要为西南和南向)的输送对北京市区的空气污染贡献份额较大.卫星遥感气溶胶可以比较直观地再现污染物的区域分布和输送,不仅为研究全球气候变化也为研究区域环境的空气质量提供了一种有效手段.     

Sulfur budget above the Eastern Mediterranean: relative contribution of anthropogenic and biogenic sources

To access the relative contribution of anthropogenic and biogenic sulfur sources to the sulfur budget in the Eastern Mediterranean, an area characterized by very high nss-     levels, measurements of both wet and dry deposition of sulfur were performed at a remote area on the island of Crete (Finokalia) during a 3-yr period (1996–1999). The estimation of dry deposition is based on both gaseous sulfur dioxide (SO₂) and particulate phase non-sea-salt sulfate (nss-     ) and methane sulfonate (MSA) measurements. During the dry period, deposition of SO₂ from long-range transport is the main component of anthropogenic sulfur deposition in the area. The results of the wet and dry deposition obtained at Finokalia have been compared with DMS emission from seawater obtained during two yearly surveys (1997–1998) in the Cretan Sea. Our results indicate that the contribution from biogenic sources to the sulfur budget in the Eastern Mediterranean, although negligible during winter, can account for up to 26% during summer.     

Sulfur emissions to the atmosphere from natural sourees

Emissions of sulfur gases from both natural and anthropogenic sources strongly influence the chemistry of the atmosphere. To assess the relative importance of these sources we have combined the measurements of sulfur gases and fluxes during the past decade to create a global emission inventory. The inventory, which is divided into 12 latitude belts, takes into account the seasonal dependence of sulfur emissions from biogenic sources. The total emissions of sulfur gases from natural sources are approximately 0.79 Tmol S/a. These emissions are 16% of the total sulfur emissions in the Northern Hemisphere and 58% in the Southern Hemisphere. The inventory clearly shows the impact of anthropogenic sulfur emissions in the region between 35° and 50°N.     

中国3个典型城市气溶胶光学厚度地基观测及其MODIS气溶胶产品精度分析

利用中国太阳分光观测网的观测资料结合MODIS(中分辨率成像光谱仪)的气溶胶产品分析了北京、兰州、上海3个典型区域城市的气溶胶光学特性。结果表明:北京AOD(气溶胶光学厚度)年平均为0.41±0.35,春夏高,秋冬低,Angstrm波长指数α年平均为1.40±0.85表现为细模态粒子,MODIS的光学厚度为0.52±0.39与地面观测相关系数为0.91,存在系统性高估;兰州AOD年平均为0.55±0.21,夏季最低,秋冬较高,α年平均为0.95±0.20表现为粗模态粒子,MODIS光学厚度为0.43±0.21与地面观测相关系数仅为0.07,存在系统性低估;上海AOD年平均为0.55±0.21,无明显季节变化,α平均为1.03±0.25,MODIS光学厚度为0.74±0.30与地面观测相关系数为0.75,存在系统性高估。城市地理位置和复杂地表等原因造成反照率的不确定,MODIS气溶胶产品在这3个城市的反演效果仍有很大提升空间。     

Spatial and temporal variations of methanesulfonic acid and non sea salt sulfate in Antarctic ice

A simultaneous glaciochemical study of methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO₄ ^-) has been conducted on the Antarctic plateau (South Pole, Vostok) and in more coastal regions. The objective was to investigate marine sulfur emissions in very remote areas. Firstly, our data suggest that MSA and nss-SO₄ present in antarctic ice are mainly marine in origin and that DMS emissions have been significantly modulated by short term (eg. El Nino Southern Oscillation events) as well as long term climatic changes in the past. Secondly, our study of spatial variations of these two sulfur species seems to indicate that the atmosphere of coastal antarctic regions are mainly supplied by local DMS emissions whereas the atmosphere of the high plateau is also influenced by DMS emissions from more temperate marine latitudes. Thirdly, our study of the partitioning between MSA and nss-SO₄ suggest that the temperature could have been an important parameter controlling the final composition of the high southern latitude atmosphere over the last climatic cycle; colder temperature favoring the formation of MSA. However, our data also support a possible role played by changes in the transport pattern of marine air to the high antarctic plateau.     

Atmospheric concentrations and deposition of oxidised sulfur and nitrogen species at Petaling Jaya, Malaysia, 1993–1998

Wet‐only rainwater composition, acid‐precursor gas mixing ratios and aerosol loading were determined from weekly‐averaged samples at Petaling Jaya, Malaysia, over the five year period from March 1993 to March 1998. Annual deposition fluxes of acidic sulfur and nitrogen species estimated from these data show this site to be heavily impacted by acidic deposition, with total oxidised sulfur plus nitrogen deposition in the range 277–480 meq m⁻² yr⁻¹. Average contributions were 56% as sulfur species, 44% as nitrogen species, with wet deposition in this region of high rainfall accounting for 67% of total deposition. Thus total acid deposition fluxes were equivalent to levels that provided motivation for emissions reduction programs in both Europe and North America. The possibility of adverse environmental effects in Malaysia caused by acid deposition therefore merits serious consideration and assessment.