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.     

Sulfate and methanesulfonate in the maritime aerosol at Cape Grim,Tasmania

High-volume aerosol filters, exposed in maritime air masses at Cape Grim since late 1976, were analysed for excess sulfate (not of seasalt origin) and methanesulfonate. The mean concentrations (standard errors) of 2.80(0.59) and 0.176(0.027) nmole/m³ respectively are about half those reported in a recent study of aerosol samples from various locations in the Atlantic and Pacific oceans.Methanesulfonate concentration varied seasonally by at least an order of magnitude with a summer maximum and winter minimum. No comparable cycle was found for excess sulfate.     

Observed changes in aerosol physical and optical properties before and after precipitation events

Precipitation scavenging of aerosol particles is an important removal process in the atmosphere that can change aerosol physical and optical properties. This paper analyzes the changes in aerosol physical and optical properties before and after four rain events using in situ observations of mass concentration, number concentration, particle size distribution, scattering and absorption coefficients of aerosols in June and July 2013 at the Xianghe comprehensive atmospheric observation station in China. The results show the effect of rain scavenging is related to the rain intensity and duration, the wind speed and direction. During the rain events, the temporal variation of aerosol number concentration was consistent with the variation in mass concentration, but their size-resolved scavenging ratios were different. After the rain events, the increase in aerosol mass concentration began with an increase in particles with diameter 0.8 μm [measured using an aerodynamic particle sizer(APS)], and fine particles with diameter 0.1 μm [measured using a scanning mobility particle sizer(SMPS)]. Rainfall was most efficient at removing particles with diameter ～0.6 μm and greater than 3.5 μm. The changes in peak values of the particle number distribution(measured using the SMPS) before and after the rain events reflect the strong scavenging effect on particles within the 100–120 nm size range. The variation patterns of aerosol scattering and absorption coefficients before and after the rain events were similar, but their scavenging ratios differed, which may have been related to the aerosol particle size distribution and chemical composition.     

Airborne and lidar measurements of aerosol and cloud particles in the troposphere over Alert Canada in April 1986

As a component of the Canadian Arctic Haze Study, held coincident with the second Arctic Gas and Aerosol Sampling Program (AGASP II), vertical profiles of aerosol size distribution (0.17 m), light scattering parameters and cloud particle concentrations were obtained with an instrumented aircraft and ground-based lidar system during April 1986 at Alert. Northwest Territories. Average aerosol number concentrations range from about 200 cm^–3 over the Arctic ice cap to about 100 cm^–3 at 6 km. The aerosol size spectrum is virtually free of giant or coarse aerosol particles, and does not vary significantly with altitude. Most of the aerosol volume is concentrated in the 0.17–0.50 m size range, and the aerosol number concentration is found to be a good surrogate for the SO₄ ⁼ concentration of the Arctic haze aerosol. Comparison of the aircraft and lidar data show that, when iced crystal scattering is excluded, the aerosol light scattering coefficient and the lidar backscattering coefficient are proportional to the Arctic haze aerosol concentration. Ratios of scattering to backscattering, scattering to aerosol number concentration, and backscattering to aerosol number concentration are 15.3 steradians, 1.1×10^–13 m², and 4.8×10^–15 m² sr^–1, respectively. Aerosol scattering coefficients calculated from the measured size distributions using Mie scattering agree well with measured values. The calculations indicate the aerosol absorption optical depth over 6 km to range between 0.011 and 0.018. The presence of small numbers of ice crystals (10–20 crystals 1^–1 measured) increased light scattering by over a factor of ten.     

On the effect of the chemical composition of atmospheric aerosol particles on nucleation scavenging and the formation of a cloud interstitial aerosol

Nucleation scavenging and the formation of a cloud interstitial aerosol (CIA) were theoretically studied in terms of the chemical composition of atmospheric aerosol particles. For this study, we used our air-parcel cloud model, which includes the entrainment of air and detailed microphysics, for determining the growth and interaction of aerosol particles and drops. Maritime and remote continental aerosol particle spectrums were used whose size distributions were superpositions of three log-normal distributions, each of a prescribed chemical composition. Our results show (1) that the CIA exhibits a size distribution with a distinctive cut-off at a specific radius of the dry as well as of the wet particle size distribution. All particles above this limiting size become activated to cloud drops and, thus, are not present in the CIA spectrum. This limiting size was found to be independent of the chemical composition of the particles and only dependent on the prevailing supersaturation. Below this specific size, the CIA spectrum becomes depleted of dry aerosol particles in a manner which does depend on their chemical composition and on the supersaturation in the air. (2) The number of aerosol particles nucleated to cloud drops depends critically on the chemical composition of the particles and on the prevailing supersaturation.     

Characterization of organic aerosols in Beijing using an aerodyne high-resolution aerosol mass spectrometer

Fine particle of organic aerosol(OA), mostly arising from pollution, are abundant in Beijing. To achieve a better understanding of the difference in OA in summer and autumn, a high-resolution time-of-flight aerosol mass spectrometer(HRTo F-AMS, Aerodyne Research Inc., USA) was deployed in urban Beijing in August and October 2012. The mean OA mass concentration in autumn was 30 ± 30 μg m-3, which was higher than in summer(13 ± 6.9 μg m-3). The elemental analysis found that OA was more aged in summer(oxygen-to-carbon(O/C) ratios were 0.41 and 0.32 for summer and autumn,respectively). Positive matrix factorization(PMF) analysis identified three and five components in summer and autumn, respectively. In summer, an oxygenated OA(OOA), a cooking-emission-related OA(COA), and a hydrocarbon-like OA(HOA)were indentified. Meanwhile, the OOA was separated into LV-OOA(low-volatility OOA) and SV-OOA(semi-volatile OOA);and in autumn, a nitrogen-containing OA(NOA) was also found. The SOA(secondary OA) was always the most important OA component, accounting for 55% of the OA in the two seasons. Back trajectory clustering analysis found that the origin of the air masses was more complex in summer. Southerly air masses in both seasons were associated with the highest OA loading, while northerly air masses were associated with the lowest OA loading. A preliminary study of OA components,especially the POA(primary OA), in different periods found that the HOA and COA all decreased during the National Day holiday period, and HOA decreased at weekends compared with weekdays.     

Future impact of anthropogenic sulfate aerosol on North Atlantic climate

We examine the simulated future change of the North Atlantic winter climate influenced by anthropogenic greenhouses gases and sulfate aerosol. Two simulations performed with the climate model ECHAM4/OPYC3 are investigated: a simulation forced by greenhouse gases and a simulation forced by greenhouse gases and sulfate aerosol. Only the direct aerosol effect on the clear-sky radiative fluxes is considered. The sulfate aerosol has a significant impact on temperature, radiative quantities, precipitation and atmospheric dynamics. Generally, we find a similar, but weaker future climate response if sulfate aerosol is considered additionally. Due to the induced negative top-of-the-atmosphere radiative forcing, the future warming is attenuated. We find no significant future trends in North Atlantic Oscillation (NAO) index in both simulations. However, the aerosol seems to have a balancing effect on the occurence of extreme NAO events. The simulated correlation patterns of the NAO index with temperature and precipitation, respectively, agree well with observations up to the present. The extent of the regions influenced by the NAO tends to be reduced under strong greenhouse gas forcing. If sulfate is included and the warming is smaller, this tendency is reversed. Also, the future decrease in baroclinicity is smaller due to the aerosols’ cooling effect and the poleward shift in track density is partly offset. Our findings imply that in simulations where aerosol cooling is neglected, the magnitude of the future warming over the North Atlantic region is overestimated, and correlation patterns differ from those based on the future simulation including aerosols.     

近10a中国沙尘气溶胶研究进展

沙尘气溶胶对全球气候变化的影响是当前国内外研究的热点问题。我国学者对沙尘气溶胶也开展了广泛的研究,尤其是在近10年,科研工作者对沙尘气溶胶的物理化学特性及其对气候的影响进行了重点研究。本文主要对沙尘气溶胶的物理特性（浓度、粒径谱分布、垂直分布特征及光学特性）、化学特性以及气候效应等方面的研究进行了综述,并对今后沙尘气溶胶研究中所面临的科学问题进行了展望。     

The characterization and distribution of aerosol and gaseous species in the winter monsoon over the western pacific ocean

During the winters of 1981 and 1982, measurements were taken on two Japanese islands of the aerosol and gaseous species which had been carried by northwesterly monsoons over the Pacific Ocean. The aerosols were characterized as sea-salt particles; soil particles, and as particles of sulfate, nitrate, organics and elemental carbon. At Chichi-jima island, which is about 800 km away from the main islands of Japan, it was found that the level of the anthropogenic components of the aerosols was considerably higher than their background level. The mean concentrations of the species on the islands are given in tabular forms. According to a survey made on board a ferry boat, the aerosol and gaseous species were fairly uniformly distributed along the southern coast of the main Japanese islands.     

基于能见度数据分析的气溶胶吸湿增长特征研究

基于相对湿度、能见度等气象数据,分析气溶胶吸湿增长特性,有助于了解气溶胶对大气环境和区域气候的影响。利用南京地区2016年1—12月、2017年2—12月、2018年1—8月和12月相对湿度和能见度等数据,通过非线性拟合研究气溶胶吸湿增长因子(f(RH))与相对湿度(RH)之间的关系。结果表明,吸湿增长因子在RH值较低(<80%)时,增长率较小;当RH值较高(>80%)时,增长率迅速增大。吸湿增长因子随着月RH值变化而表现出较大差异。此外,当南京地区盛行西风时,高能见度出现的时次较多。f(RH)与PM_2.5/PM₁₀成正比,PM_2.5/PM₁₀值越高,对应的气溶胶光学吸湿增长因子往往会越高。     

Shortwave aerosol optical depth of Arctic haze measured on board the NOAA WP-3D during AGASP-II,April 1986

Measurements of spectral aerosol optical depth in the Alaskan and Canadian Arctic were made from the NOAA Lockheed WP-3D aircraft as part of the second Arctic Gas and Aerosol Sampling Program (AGASP-II) during April 1986. The flight tracks and altitudes flown enabled measurements of the vertical and horizontal distribution of aerosol optical depth in the troposphere as well as direct determination of the stratospheric component. Tropospheric aerosol optical depth ranged from about 0.1 to 0.7. The factor of 7 variability sometimes occurred within 50 km horizontally; comparable variability occurred within less than 1 to 2 km vertically. The Angstrom exponents of the spectral optical depths ranged from 0.5 to 2.0, and some of the variability was apparently related to distinct aerosol regimes.     

冬季南京北郊大气气溶胶中水溶性阴离子特征

2009年冬季在南京北郊进行24 h采样,运用离子色谱法研究大气PM₁₀中水溶性阴离子的分布特征。结果表明:PM₁₀中阴离子的平均总质量浓度在白天和夜间分别为658.21、622.84 μg/m³;PM_2.1则分别为337.86、319.97 μg/m³,阴离子主要存在于细粒子中;主要水溶性阴离子均为SO₄^2-,且海盐对南京北郊大气PM₁₀和PM_2.1中的SO₄^2-质量浓度影响很小。SO₄^2-、Cl^-和F^-粒径谱分布相似,均呈双模态;NO₃^-和NO₂^-主要呈现单模态。SO₄^2-与NO₃^-、F^-与NO₃^-、SO₄^2-与Cl^-的相关系数均大于0.8,相关显著,说明其存在一定的同源性。NO₃^-/SO₄^2-的平均值在白天、夜间分别为0.058 2、0.048 4,说明南京北郊大气污染以固定源为主。分析NO₃^-、SO₄^2-前体物的转化率知道,采样期间SOR和NOR的平均值均大于10%,即SO₄^2-部分来源于SO₂的二次转化,而不是单一来源于一次污染物。     

Impact of dust aerosol on glacial-interglacial climate

The temperature anomaly and dust concentrations recorded from central Antarctic ice core records display a strong negative correlation. The dust concentration recorded from an ice core in central Antarctica is 50-70 times higher during glacial periods than interglacial periods. This study investigated the impact of dust aerosol on glacial-interglacial climate, using a zonal energy balance model and dust concentration data from an Antarctica ice core. Two important effects of dust, the direct radiative effect and dust-albedo feedback, were considered. On the one hand, the direct radiative effect of dust significantly cooled the climate during the glacial period, with cooling during the last glacial maximum being as much as 2.05℃ in Antarctica. On the other hand, dust deposition onto the ice decreased the surface albedo over Antarctica, leading to increased absorption of solar radiation, inducing a positive feedback that warmed the region by as much as about 0.9℃ during the glacial period. However, cooling by the direct dust effect was found to be the controlling effect for the glacial climate and may be the major influence on the strong negative correlation between temperature and dust concentration during glacial periods.     

南京细颗粒物对城市热岛强度的影响

随着城市化和工业化进程的加快,南京城市热岛效应显著,细颗粒物污染加剧,对大气环境、气候变化和人体健康产生重要影响.本文基于观测资料,分析了南京市不同颗粒物浓度水平下城市热岛强度的变化特征;利用光学特性模型OPAC（optical properties of aerosols and clouds model）和辐射传输模型TUV（troposphere ultraviolet-visible model）估计了气溶胶的光学厚度及辐射强迫;定量分析了细颗粒物对城市热岛强度的影响及其可能机制.结果表明：南京城市热岛强度范围为-0.51.3K,冬季强于夏季.细颗粒物质量浓度范围为32 135 μg/m3,冬季高于夏季,城区和郊区差别不大;当大气中细颗粒物质量浓度较高时,城市热岛强度相对较弱;南京城郊气溶胶光学厚度变化范围为0.28 1.01,在地面产生的辐射强迫达-3.88-4.72 W＆#183;m-2;由于城区和郊区下垫面、人为热、细颗粒物浓度水平的差异,造成城郊近地面降温的不同,导致细颗粒物对城市热岛强度的削弱,夏季减弱0.1K,冬季减弱0.2K.     

沈阳地区大气气溶胶消光特性的观测研究

利用沈阳地区2010年全年大气总消光系数、气体分子吸收系数、气溶胶吸收和散射系数以及大气可吸入颗粒物数浓度的小时数据,对沈阳地区的大气消光特别是气溶胶消光性质进行了高时间分辨率的研究。结果表明:总消光系数和气溶胶散射系数在一天内呈单周期峰谷型分布,05—06时(北京时间,下同)达到峰值,15时达到谷值。大气总消光系数在雪天最大、霾天次之、晴天最小。气溶胶消光系数与粒子数浓度的相关性随着粒径的减小而增大。     

Thin coating on ultrafine aerosol particles

This article presents the results of an experimental investigation on gas-phase coating of nanometer-sized NaCl aerosol particles with a condensing vapor of ZnCl₂. The coating process has been carried out in a commercially available Venturi aspirator, where the NaCl at ambient temperature is mixed with the supersaturated ZnCl₂ vapor. The operating conditions (ZnC1₂ vapor temperature, and ZnCl₂/NaCl flow rate ratio) at which the ZnCl₂ vapor preferentially nucleates onto the surface of the seed NaCl particles forming a coating layer on them, have been determined. Particle size growth as a function of the original seed diameter has also been determined. Smaller particles undergo a larger relative size growth ratio. It has also been shown that the presence of a coating layer does not affect the charge distribution of the original seed particles.     

Elemental composition of particulate material sampled from the Arctic haze aerosol

Thirty-six aerosol filter samples collected in tropospheric Arctic haze layers, in the stratosphere, and in the marine boundary layer during the 1983 Arctic Gas and Aerosol Sampling Program were analyzed for trace elements using instrumental neutron activation analysis. Average crustal dust concentrations were 540 ng/m³ and 330 ng/m³ for samples collected in Arctic haze over the North American and Norwegian Arctic, respectively. An average marine salt concentration of 120 ng/m³ was obtained for haze samples collected above the marine boundary layer on both sides of the Arctic.Meteorological and wind trajectory information were used to identify specific haze transport pathways, which brought relatively unmixed aerosol from the central Soviet Union into the AGASP sampling areas. Results from individual filters collected within these transport zones are discussed, with emphasis on certain trace metal ratos which have been proposed by other researchers as discriminators of aerosols from different source regions. Our aircraft-collected data are compared with previously-collected ground-based measurements, and show reasonably good agreement for most tracer elements and ratios. Specifically, we have determined the As/Sb ratio tracer, named by other researchers as the most effective elemental discriminator of aerosol from the central Soviet Union, to be approximately 5–6. This relatively high tracer value is consistent with previous ground-based findings. A significantly lower V/Sb ratio was observed throughout this study, possibly indicating a change in the source signature.     

Phase partitioning of aerosol particles in clouds at Kleiner Feldberg

The partitioning of aerosol particles between cloud droplets and interstitial air by number and volume was determined both in terms of an integral value and as a function of size for clouds on Mt. Kleiner Feldberg (825 m asl), in the Taunus Mountains north-west of Frankfurt am Main, Germany. Differences in the integral values and the size dependent partitioning between two periods during the campaign were observed. Higher number and volume concentrations of aerosol particles in the accumulation mode were observed during Period II compared to Period I. In Period I on average 87±11% (±one standard deviation) and 73±7% of the accumulation mode volume and number were incorporated into cloud droplets. For Period II the corresponding fractions were 42±6% and 12±2% in one cloud event and 64±4% and 18±2% in another cloud event. The size dependent partitioning as a function of time was studied in Period II and found to have little variation. The major processes influencing the partitioning were found to be nucleation scavenging and entrainment.     

华东地区气溶胶分布和变化特征研究

利用中分辨率光谱仪(MODIS)获得的气溶胶光学厚度(AOD)、细粒子比例(FMF)和臭氧检测仪(OMI)获得的气溶胶指数(AI)统计分析了2005—2014年我国华东地区气溶胶光学性质的时空分布特征,同时利用潜在源分析(PSCF)模型对我国华东地区AOD和AI的潜在源区进行分析。研究结果表明:华东地区的AOD、FMF和AI时空分布存在较大的差异,2005—2014年AOD和AI的平均值高值主要分布在华东地区北部,FMF的高值区则分布在华东南部地区;10 a间华东地区AOD呈现出先升高后降低的趋势,FMF波动幅度不明显,AI值有所上升;整个华东地区AOD的季节变化较为明显,春夏两季AOD明显高于秋冬两季。华东北部和中部地区夏季由于较高的相对湿度,AOD最大可达0.8以上。而在华东南部地区,夏季受到降水的影响,AOD维持在0.2~0.4之间。FMF季节变化趋势与AOD不同,夏季最大达到0.58,春季最小仅为0.26。AI平均值在冬季最大高达0.63,夏季最小,为0.27。PSCF分析显示华东地区AOD主要源区以局地排放为主,同时也存在由河南、湖北和湖南等周边省市近距离输送影响;AI以局地和北方远距离输送为主,同时也受到河南、湖北等周边省市近距离输送的影响。