The interpretation of baseline atmospheric turbidity measurements at Cape Grim,Tasmania

Five years of turbidity data at Cape Grim have been analysed. The turbidity at 500 nm in clean maritime airmasses from the South to the West shows a seasonal variation, with a minimum in winter. There is also a variation in turbidity with wind speed. The winter minimum can be explained partially by a minimum in wind strength in that season. On the assumption, based on observations at Cape Grim and at other locations, that the boundary layer turbidity is caused by seasalt haze, an attempt is made to interpret the observed turbidity values and their seasonal changes. Optical extinction coefficients at the surface deduced from the measured values of optical depth are compared with extinction coefficients calculated from Mie theory using particle size distributions measured at Cape Grim. Reasonable agreement is obtained when the growth of salt particles in the high maritime humidity is considered, using both theoretical models and previous experimental results together with the rapid increase in salt concentration with wind speed.     

Dimethylsulfide oxidation and the ratio of methanesulfonate to non sea-salt sulfate in the marine aerosol

A box model of DMS oxidation in the clean, low-NO _x marine atmospheric boundary layer has been used to predict the latitude dependence of the aerosol methanesulfonate to non sea-salt sulfate ratio. The observed latitude dependence of this ratio in the Southern Hemisphere can be reproduced reasonably well if the full suite of reactions proposed by Yin et al. (1990a) is employed, and a strong temperature dependence is specified in the rates of decomposition of CH₃SO₂ and CH₃SO₃ radicals.     

Atmospheric Methyl Iodide at Cape Grim, Tasmania, from AGAGE Observations

Atmospheric mixing ratios of methyl iodide (CH₃I) and other methyl halides have been measured at Cape Grim, Tasmania (41°S, 145°E), since early 1998 as part of the Advanced Global Atmospheric Gases Experiment (AGAGE). This paper analyses about 1700 ambient air CH₃I measurements from the 14-month period (March 1998–April 1999). Mixing ratios peaked during the summer, despite faster photolytic loss, suggesting local oceanic emissions were about 2.2–3.6 times stronger in summer than in winter. Back trajectories show that CH₃I levels are strongly dependent on air mass origin, with highest mixing ratios in air from the Tasman Sea/Bass Strait region and lowest levels in air originating from the Southern Ocean at higher latitudes. CH₃I mixing ratios were not well correlated with other methyl halides in unpolluted marine air. The large variations with season and air mass origin suggest that high frequency, continuous data from key locations will make a significant contribution to the understanding of sources and sinks of this important short-lived atmospheric species.     

The annual cycle of peroxides and ozone in marine air at Cape Grim, Tasmania

The concentration of gas-phase peroxides has been measured almost continuously at the Cape Grim baseline station (41° S) over a period of 393 days (7702 h of on-line measurements) between February 1991 and March 1992. In unpolluted marine air a distinct seasonal cycle in concentration was evident, from a monthly mean value of>1.4 ppbv in summer (December) to <0.2 ppbv in winter (July). In the summer months a distinct diurnal cycle in peroxides was also observed in clean marine air, with a daytime build-up in concentration and decay overnight. Both the seasonal and diurnal cycles of peroxides concentration were anticorrelated with ozone concentration, and were largely explicable using a simple photochemical box model of the marine boundary layer in which the central processes were daytime photolytic destruction of ozone, transfer of reactive oxygen into the peroxides under the low-NO_x ambient conditions that favour self-reaction between peroxy radicals, and continuous heterogeneous removal of peroxides at the ocean surface. Additional factors affecting peroxides concentrations at intermediate timescales (days to a week) were a dependence on air mass origin, with air masses arriving at Cape Grim from higher latitudes having lower peroxides concentrations, a dependence on local wind speed, with higher peroxides concentrations at lower wind speeds, and a systematic decrease in peroxides concentration during periods of rainfall. Possible physical mechanisms for these synoptic scale dependencies are discussed.     

Airborne measurements of dimethylsulfide,sulfur dioxide,and aerosol ions over the Southern Ocean South of Australia

Vertical distributions of dimethylsulfide (DMS), sulfur dioxide (SO₂), aerosol methane-sulfonate (MSA), non-sea-salt sulfate (nss-SO₄ ^2-), and other aerosol ions were measured in maritime air west of Tasmania (Australia) during December 1986. A few cloudwater and rainwater samples were also collected and analyzed for major anions and cations. DMS concentrations in the mixed layer (ML) were typically between 15–60 ppt (parts per trillion, 10^–12; 24 ppt=1 nmol m^–3 (20°C, 1013 hPa)) and decreased in the free troposphere (FT) to about <1–2.4 ppt at 3 km. One profile study showed elevated DMS concentrations at cloud level consistent with turbulent transport (cloud pumping) of air below convective cloud cells. In another case, a diel variation of DMS was observed in the ML. Our data suggest that meteorological rather than photochemical processes were responsible for this behavior. Based on model calculations we estimate a DMS lifetime in the ML of 0.9 days and a DMS sea-to-air flux of 2–3 mol m^–2 d^–1. These estimates pertain to early austral summer conditions and southern mid-ocean latitudes. Typical MSA concentrations were 11 ppt in the ML and 4.7–6.8 ppt in the FT. Sulfur-dioxide values were almost constant in the ML and the lower FT within a range of 4–22 ppt between individual flight days. A strong increase of the SO₂ concentration in the middle FT (5.3 km) was observed. We estimate the residence time of SO₂ in the ML to be about 1 day. Aqueous-phase oxidation in clouds is probably the major removal process for SO₂. The corresponding removal rate is estimated to be a factor of 3 larger than the rate of homogeneous oxidation of SO₂ by OH. Model calculations suggest that roughly two-thirds of DMS in the ML are converted to SO₂ and one-third to MSA. On the other hand, MSA/nss-SO₄ ^2- mole ratios were significantly higher compared to values previously reported for other ocean areas suggesting a relatively higher production of MSA from DMS oxidation over the Southern Ocean. Nss-SO₄ ^2- profiles were mostly parallel to those of MSA, except when air was advected partially from continental areas (Africa, Australia). In contrast to SO₂, nss-SO₄ ^2- values decreased significantly in the middle FT. NH₄ ⁺/nss-SO₄ ^2- mole ratios indicate that most non-sea-salt sulfate particles in the ML were neutralized by ammonium.     

Vertical distribution of dimethylsulfide,sulfur dioxide,aerosol ions,and radon over the Northeast Pacific Ocean

Dimethylsulfide (DMS), sulfur dioxide (SO₂), methanesulfonate (MSA), nonsea-salt sulfate (nss-SO₄ ^2–), sodium (Na⁺), ammonium (NH₄ ⁺), and nitrate (NO₃ ^–) were determined in samples collected by aircraft over the open ocean in postfrontal maritime air masses off the northwest coast of the United States (3–12 May 1985). Measurements of radon daughter concentrations and isentropic trajectory calculations suggested that these air masses had been over the Pacific for 4–8 days since leaving the Asian continent. The DMS and MSA profiles showed very similar structures, with typical concentrations of 0.3–1.2 and 0.25–0.31 nmol m^–3 (STP) respectively in the mixed layer, decreasing to 0.01–0.12 and 0.03–0.13 nmol m^–3 (STP) at 3.6 km. These low atmospheric DMS concentrations are consistent with low levels of DMS measured in the surface waters of the northeastern Pacific during the study period.The atmospheric SO₂ concentrations always increased with altitude from <0.16–0.25 to 0.44–1.31 nmol m^–3 (STP). The nonsea-salt sulfate (ns-SO₄ ^2–) concentrations decreased with altitude in the boundary layer and increased again in the free troposphere. These data suggest that, at least under the conditions prevailing during our flights, the production of SO₂ and nss-SO₄ ^2– from DMS oxidation was significant only within the boundary layer and that transport from Asia dominated the sulfur cycle in the free troposphere. The existence of a sea-salt inversion layer was reflected in the profiles of those aerosol components, e.g., Na⁺ and NO₃ ^–, which were predominantly present as coarse particles. Our results show that long-range transport at mid-tropospheric levels plays an important role in determining the chemical composition of the atmosphere even in apparently remote northern hemispheric regions.     

Ozone in the Marine Boundary Layer at Cape Grim: Model Simulation

A photochemical box model has been used to simulate the mixing ratio ofozone under conditions reflecting those encountered in the marine boundarylayer at Cape Grim, Tasmania, where a decade-long record of ozone mixingratio is available. The model is based on the proposition that ozone loss byphotolysis, atmospheric reaction with hydroperoxy and hydroxyl radicals, andsurface deposition is balanced by ozone gain via entrainment from the lowerfree troposphere with a small additional source in summer from photolysis ofnitrogen dioxide. This model simulates very well the observed ozone records,reproducing both the small diurnal cycle in ozone mixing ratio observedduring the summer months, and the factor of two seasonal ozone cycle showinga distinct winter maximum and summer minimum. The model result confirms thatunder the low-NO_x conditions of the clean marine boundarylayer net photochemical loss of ozone occurs at all times of year.     

Identification of Regional Sources of Methyl Bromide and Methyl Iodide from AGAGE Observations at Cape Grim,Tasmania

There are large uncertainties in identifying and quantifying the globally significant sources and sinks of methyl bromide (CH₃Br) and methyl iodide (CH₃I). Long-term, quasi-continuous observations can provide valuable information about their regional sources, which may be significant in the global context. We report 3 years of in situobservations of these trace gases from the AGAGE (Advanced Global Atmospheric Gas Experiment) program at Cape Grim, Tasmania (41 °S, 145 °E). The average background levels of CH₃Br and CH₃I during March 1998–March 2001 were 8.05 and 1.39 ppt (dry air mole fractions expressed in parts per 10¹²), respectively. The CH₃Br background data showed little seasonal variability. Trajectory analyses reveal that air masses showing elevated CH₃Br levels at Cape Grim have had significant contact with coastal-terrestrial and/or coastal-seawater and/or urban source regions. The CH₃I background data showed a seasonal cycle with a 3-year average amplitude of 0.47 ppt and maximum concentrations in summer, suggesting that the Southern Ocean is a significant source.Trajectory analyses reveal that air masses showing highly elevated CH₃I levels at Cape Grim have had significant contact with coastal-terrestrial and/or coastal-seawater regions and/or the open-ocean regions of Bass Strait and the Tasman Sea.     

Regional Sources of Methyl Chloride, Chloroform and Dichloromethane Identified from AGAGE Observations at Cape Grim, Tasmania, 1998–2000

There are large uncertainties in identifying and quantifying the natural and anthropogenic sources of chloromethanes – methyl chloride (CH₃Cl), chloroform (CHCl₃) and dichloromethane (CH₂Cl₂), which are responsible for about 15% of the total chlorine in the stratosphere. We report two years of in situ observations of these species from the AGAGE (Advanced Global Atmospheric Gas Experiment) program at Cape Grim, Tasmania (41° S, 145° E). The average background levels of CH₃Cl, CHCl₃ and CH₂Cl₂ during 1998–2000 were 551± 8, 6.3± 0.2 and 8.9± 0.2 ppt (dry air mole fractions expressed in parts per 10¹²) respectively, with a two-year average amplitude of the seasonal cycles in background air of 25, 1.1 and 1.5 ppt respectively. The CH₃Cl and CHCl₃ records at Cape Grim show clear episodes of elevated mixing ratios up to 1300 ppt and 55 ppt respectively, which are highly correlated, suggesting common source(s). Trajectory analyses show that the sources of CH₃Cl and CHCl₃ that are responsible for these elevated observations are located in coastal-terrestrial and/or coastal-seawater regions in Tasmania and the south-eastern Australian mainland. Elevated levels of CH₂Cl₂ (up to 70 ppt above background) are associated mainly with emissions from the Melbourne/Port Phillip region, a large urban/industrial complex (population 3.5 million) 300 km north of Cape Grim.Now at the Centre for Atmospheric ChemistryNow at School of Environmental Sciences     

AGAGE Observations of Methyl Bromide and Methyl Chloride at Mace Head, Ireland, and Cape Grim, Tasmania, 1998–2001

In situ AGAGE GC-MS measurements of methyl bromide (CH₃Br) and methyl chloride (CH₃Cl) at Mace Head, Ireland and Cape Grim, Tasmania (1998–2001) reveal a complex pattern of sources. At Mace Head both gases have well-defined seasonal cycles with similar average annual decreases of 3.0% yr⁻¹ (CH₃Br) and 2.6% yr⁻¹ (CH₃Cl), and mean northern hemisphere baseline mole fractions of 10.37 ± 0.05 ppt and 535.7 ± 2.2 ppt, respectively. We have used a Lagrangian dispersion model and local meteorological data to segregate the Mace Head observations into different source regions, and interpret the results in terms of the known sources and sinks of these two key halocarbons. At Cape Grim CH₃Br and CH₃Cl also show annual decreases in their baseline mixing ratios of 2.5% yr⁻¹ and 1.5% yr⁻¹, respectively. Mean baseline mole fractions were 7.94 ± 0.03 ppt (CH₃Br) and 541.3 ± 1.1 ppt (CH₃Cl). Although CH₃Cl has astrong seasonal cycle there is no well-defined seasonal cycle in the Cape Grim CH₃Br record. The fact that both gases are steadily decreasing in the atmosphere at both locations implies that a change has occurred which is affecting a common, major source of both gases (possibly biomass burning) and/or their major sink process (destruction by hydroxyl radical).     

2010年民勤沙地近地面沙尘气溶胶浓度特征

为了更好地研究沙尘气溶胶起沙和输送特征,2010年4—5月,在民勤周边沙地利用EZ LIDAR ALS300&ALS450型激光雷达和 GRIMM 180型颗粒物采样器进行了大气气溶胶的外场连续观测,取得了晴天、浮尘、扬沙和沙尘暴天气条件下沙尘气溶胶总后向散射垂直剖面图和PM₁₀、PM_2.5、PM_1.0质量浓度采样资料,其中包含“0424”特强沙尘暴过程资料。结果表明：春季民勤近地层大气中沙尘气溶胶浓度较高,且随气象要素的变化很大;在整个观测期内,PM₁₀、PM_2.5、PM_1.0的平均质量浓度分别为202.3、57.4 μg/m³、16.7 μg/m³。在不同天气条件下,PM₁₀、PM_2.5、PM_1.0质量浓度的变化有很好的相关性,但变化趋势有所不同。在沙尘暴天气条件下,PM₁₀的日平均质量浓度高达2469.1μg/m³,是背景天气条件下PM10日平均质量浓度的100多倍,是浮尘天气条件下PM10日平均质量浓度的8倍,是扬沙天气条件下PM₁₀日平均质量浓度的2倍。PM_2.5在沙尘暴天气下日平均质量浓度为460.3 μg/m³,是背景天气条件下PM_2.5日平均质量浓度的45倍,是浮尘天气条件下PM_2.5日平均质量浓度的6倍,是扬沙天气条件下PM_2.5日平均质量浓度的1.4倍。PM_1.0在沙尘暴天气条件下的日平均浓度为92.7 μg/m³,是背景天气条件下PM_1.0日平均浓度的13倍,是浮尘天气条件下PM_1.0日平均浓度的7倍,是扬沙天气条件下PM_1.0日平均浓度的1.3倍。可见,风速增大时沙尘粒子浓度的增加对粒子粒径是有选择的,小粒子比重随沙尘浓度增加而相对减小,大粒子比重随沙尘浓度增加而相对增多;通过对“0424”特强沙尘暴过程的研究表明,一次沙尘暴过程往往包括沙尘暴、扬沙和浮尘天气中的两种类型;通过对激光雷达数据分析发现,在强沙尘暴发生过程当中,民勤沙地发生了非常严重的风蚀起沙现象。     

TRACE-P期间硫酸盐、硝酸盐和铵盐气溶胶的模拟研究

结合最新评估的东亚地区 1°× 1°污染源资料 ,利用由区域大气模式系统 (RAMS)和区域大气质量模式系统 (CMAQ)耦合的空气质量模式系统 ,对东亚地区 2 0 0 1年春季气溶胶的输送及其化学转化过程进行了研究。为了检验模式系统的模拟效果 ,我们将模拟的硫酸盐、硝酸盐和铵盐气溶胶的浓度与TRACE -P观测期间获取的观测值进行了比较。比较结果显示 ,模拟值与观测值具有相当好的一致性 ,模式很好地反映了气溶胶浓度的分布特征和变化规律 ,再现了许多观测到的重要特征。模拟结果表明 ,中国区域硫酸盐气溶胶浓度高值主要是人为排放的二氧化硫造成的 ,10 0°E以东的中国广大地区的硫酸盐气溶胶柱含量超过了 6mg·m- 2 ,最高值达到 2 4mg·m- 2 ,柱含量 >16mg·m- 2 的区域延伸到中国近海的广大海域。东亚地区的人类活动不仅使污染地区气溶胶柱含量显著增加 ,而且使近海无源区的广大海域的污染加重。本模式系统的建立为今后进一步研究区域大气污染物的变化机理提供了有效的手段。     

Spatial, Temporal and Interannual Variability of Methanesulfonate and Non-Sea-Salt Sulfate in Rainwater in the Southern Indian Ocean (Amsterdam, Crozet and Kerguelen Islands)

Methanesulfonate (MS^–) and non-sea-salt sulfate (nss-SO ₄ ^2– ), two of the major oxidation products of atmospheric dimethylsulfide (DMS), have been continuously measured in rainwater at three remote islands in the Southern Indian Ocean: Amsterdam since 1991, Crozet since 1992, and Kerguelen since 1993. The annual volume weighted mean (VWM) concentrations of nss-SO ₄ ^2– in rainwater were 3.19, 3.04 and 4.57 eq l^–1 at Amsterdam, Crozet, and Kerguelen, respectively while the VWM of MS^– were 0.24, 0.15 and 0.30 eq l^–1, respectively. At all three islands, MS^– presented a well-distinguished seasonal variation with a maximum during summer whereas the seasonal variation of nss-SO ₄ ^2– was less pronounced, possibly due to the increased anthropogenic influence during the winter period. Furthermore, MS^– presented significant interannual variations, in particular at Amsterdam and Crozet, which is closely related to the sea-surface temperature (SST) anomalies). Finally, the nss-SO ₄ ^2– deposition at Crozet Island presented a decreasing interannual trend, reflecting probably reductions in sulfur emissions from Southern Africa. On the contrary no interannual tendency was observed in the nss-SO ₄ ^2– concentrations at Amsterdam Island, indicating that the biogeochemical sulfur cycle at this area is mainly influenced by biogenic emissions.     

Nitrogen and sulfur species in acrosols at Mawson,Antarctica, and their relationship to natural radionuclides

High volume aerosol samples were collected continuously at Mawson, Antarctica (67°36'S, 62°30'E), from February 1987 through October 1989. All samples were analyzed for Na⁺, Cl^-, SO₄ ⁼, NO₃ ^-, methanesulfonate (MSA), NH₄ ⁺,⁷Be, and²¹⁰Pb. The annual mean concentrations of many of the species are very low, substantially lower than even those over the relatively pristine regions of the tropical and subtropical South Pacific. The concentrations at Mawson are comparable both in magnitude and in seasonality to those which have been measured in long term studies at the South Pole and at the coastal German Antarctic research station, Georg von Neumayer (GvN). This comparability suggests that the aerosol composition may be relatively uniform over a broad sector of the Antarctic. The concentrations of most of the species exhibit very strong and sharply-defined seasonal cycles. MSA, non-sea-salt (nss) SO₄ ⁼ and NH₄ ⁺ all exhibit similar cycles, with maxima during the austral summer (December through February) being more than an order of magnitude higher than the winter minima. The limited⁷Be data appears to exhibit a similar cycle. Although nitrate and²¹⁰Pb also exhibit relatively high concentrations during the austral summer, their cycles are far more complex than those of the previous species with indications of multiple peaks. As expected, the concentration of sea-salt (as indicated by Na⁺ and Cl^-) peaks during the winter. The results from multiple variable regression analyses indicate that the dominant source of nss SO₄ ⁼ is the oxidation of dimethylsulfide (DMS) which produces MSA and nss SO₄ ⁼ in a ratio of about 0.31 (about five times higher than that over the tropical and subtropical oceans). However, a very significant fraction (about 25%) of the nss SO₄ ⁼ is associated with NO₃ ^-, The seasonal cycle of NO₃ ^- is similar to that of²¹⁰Pb and distinctly different from that of⁷Be and MSA. These results indicate that the major source of NO₃ ^- over Antarctica is probably continental as opposed to stratospheric or marine biogenic.     

A study of aerosol particle sizes in the atmosphere of Athens, Greece, retrieved from solar spectral measurements

This work aims at determining the aerosol particle radii in the atmosphere of Athens. Such a work is carried out in Athens for the first time. For this purpose, solar spectral direct-beam irradiance measurements were used in the spectral range 310–575 nm. To estimate the particle radius from aerosol optical depth retrieval, a minimization technique was employed based on the golden-section search of the difference between experimental and theoretical values of the aerosol optical depth. The necessary Mie computations were performed based on the algorithm LVEC.In this study, the mean particle radius of a given distribution was calculated every 30 min during cloudless days in the period November 1996 to September 1997. The largest particles were observed in the summer and the smallest during winter. The result was verified by the increased values of the aerosol optical depth and the turbidity factors calculated in the summer. The differences in the diurnal variation from season to season are attributed to the prevailing wind regime, pollutant emission and sink rates in the atmosphere of Athens.     

A review of global stratospheric aerosol: Measurements, importance, life cycle, and local stratospheric aerosol

Stratospheric aerosol, noted after large volcanic eruptions since at least the late 1800s, were first measured in the late 1950s, with the modern continuous record beginning in the 1970s. Stratospheric aerosol, both volcanic and non-volcanic are sulfuric acid droplets with radii (concentrations) on the order of 0.1–0.5 µm (0.5–0.005 cm^− 3), increasing by factors of 2–4 (10–10³) after large volcanic eruptions. The source of the sulfur for the aerosol is either through direct injection from sulfur-rich volcanic eruptions, or from tropical injection of tropospheric air containing OCS, SO₂, and sulfate particles. The life cycle of non-volcanic stratospheric aerosol, consisting of photo-dissociation and oxidation of sulfur source gases, nucleation/condensation in the tropics, transport pole-ward and downward in the global planetary wave driven tropical pump, leads to a quasi steady state relative maximum in particle number concentration at around 20 km in the mid latitudes. Stratospheric aerosol have significant impacts on the Earth's radiation balance for several years following volcanic eruptions. Away from large eruptions, the direct radiation impact is small and well characterized; however, these particles also may play a role in the nucleation of near tropopause cirrus, and thus indirectly affect radiation. Stratospheric aerosol play a larger role in the chemical, particularly ozone, balance of the stratosphere. In the mid latitudes they interact with both nitrous oxides and chlorine reservoirs, thus indirectly affecting ozone. In the polar regions they provide condensation sites for polar stratospheric clouds which then provide the surfaces necessary to convert inactive to active chlorine leading to polar ozone loss. Until the mid 1990s the modern record has been dominated by three large sulfur-rich eruptions: Fuego (1974), El Chichón (1982) and Pinatubo (1991), thus definitive conclusions concerning the trend of non-volcanic stratospheric aerosol could only recently be made. Although anthropogenic emissions of SO₂ have changed somewhat over the past 30 years, the measurements during volcanically quiescent periods indicate no long term trend in non-volcanic stratospheric aerosol.     

基于飞机和MODIS观测的华北地区气溶胶标高分析

为研究华北地区的气溶胶分布情况,利用2012—2014年飞机观测资料和MODIS卫星资料,对石家庄等地的气溶胶标高进行了分析。结果表明:(1)与飞机观测资料对比后认为可以利用MODIS光学厚度和常规能见度资料计算气溶胶标高;(2)华北地区春夏季气溶胶标高一般大于秋冬季;6个主要城市中,位于平原地区的城市气溶胶标高较低,西北山区城市标高较高;(3)在不进行飞行探测,仅使用地面资料和卫星资料,通过计算得到气溶胶垂直分布是可行的,尤其是在对流层中层的结果比底层更可信;(4)分别使用观测资料与拟合数据计算光学厚度,分析其误差后,确认在计算光学厚度的过程中可以使用气溶胶数密度指数递减假设。     

What can we learn from aerosol measurements at baseline stations?

In this paper the results of existing baseline aerosol monitoring programs are reviewed. For this purpose, aerosol data from five baseline stations in both hemispheres are analysed. Their information content is compared to that which can be derived when utilizing experiences of recent field experiments and the present state of aerosol sciences in general. Recommendations for extensions and reductions of baseline aerosol measurements are given.