Remote sensing of spectral signatures of tropospheric aerosols

With the launch of the German Aerospace Agency's (DLR) Modular Opto-electronic Scanner (MOS) sensor on board the Indian Remote Sensing satellite (IRS-P3) launched by the Indian Space Research Organization (ISRO) in March 1996, 13 channel multi-spectral data in the range of 408 to 1010 nm at high radiometric resolution, precision, and with narrow spectral bands have been available for a variety of land, atmospheric and oceanic studies. We found that these data are best for validation of radiative transfer model and the corresponding code developed by one of the authors at Space Applications Centre, and called ATMRAD (abbreviated for ATMospheric RADiation). Once this model/code is validated, it can be used for retrieving information on tropospheric aerosols over ocean or land. This paper deals with two clear objectives, viz.,

Sulfur,chlorine, and fluorine degassing and atmospheric loading by the 1783–1784 AD Laki (Skaftár Fires) eruption in Iceland

 The 1783–1784 Laki tholeiitic basalt fissure eruption in Iceland was one of the greatest atmospheric pollution events of the past 250 years, with widespread effects in the northern hemisphere. The degassing history and volatile budget of this event are determined by measurements of pre-eruption and residual contents of sulfur, chlorine, and fluorine in the products of all phases of the eruption. In fissure eruptions such as Laki, degassing occurs in two stages: by explosive activity or lava fountaining at the vents, and from the lava as it flows away from the vents. Using the measured sulfur concentrations in glass inclusions in phenocrysts and in groundmass glasses of quenched eruption products, we calculate that the total accumulative atmospheric mass loading of sulfur dioxide was 122 Mt over a period of 8 months. This volatile release is sufficient to have generated ∼250 Mt of H₂SO₄ aerosols, an amount which agrees with an independent estimate of the Laki aerosol yield based on atmospheric turbidity measurements. Most of this volatile mass (∼60 wt.%) was released during the first 1.5 months of activity. The measured chlorine and fluorine concentrations in the samples indicate that the atmospheric loading of hydrochloric acid and hydrofluoric acid was ∼7.0 and 15.0 Mt, respectively. Furthermore, ∼75% of the volatile mass dissolved by the Laki magma was released at the vents and carried by eruption columns to altitudes between 6 and 13 km. The high degree of degassing at the vents is attributed to development of a separated two-phase flow in the upper magma conduit, and implies that high-discharge basaltic eruptions such as Laki are able to loft huge quantities of gas to altitudes where the resulting aerosols can reside for months or even 1–2 years. The atmospheric volatile contribution due to subsequent degassing of the Laki lava flow is only 18 wt.% of the total dissolved in the magma, and these emissions were confined to the lowest regions of the troposphere and therefore important only over Iceland. This study indicates that determination of the amount of sulfur degassed from the Laki magma batch by measurements of sulfur in the volcanic products (the petrologic method) yields a result which is sufficient to account for the mass of aerosols estimated by other methods. Received: 30 May 1995 / Accepted: 19 April 1996     

大气颗粒物中铅的序列提取与分析表征

用石英纤维滤膜采集大气颗粒物样品,采用序列提取的方法把铅的总量分成环境可迁移态、碳酸盐和氧化物态、有机质和残渣态3个分量,用石墨炉原子吸收分光光度法测定铅的浓度,仪器检出限为1μg/L。对实际大气颗粒物样品进行序列提取,5份平行的序列提取3个分量测定及加和值的RSD分别为7.1%、3.3%、7.3%、5.0%。该样品三级序列提取的加和值(756μg/g)约为总量测定(738μg/g)的102%,两组数据一致性良好,且环境可迁移态、碳酸盐和氧化物态、有机质和残渣态的铅分别为加和值的64%、17%和20%。对几种典型的铅污染源排放样品进行序列提取和分析测定,不同源排放样品的形态特征各有特点,说明该序列提取的方案是可行的,达到了将不同形态的铅化合物分开的目的。     

Asian dustfall in the St. Elias Mountains, Yukon, Canada

In April 2001, a major atmospheric dustfall event occurred in the St. Elias Mountains, Yukon Territory, Canada. Field samples were collected and analyzed for particle size, mineralogy, chemical composition and Sr, Nd and Pb isotopes. Dusts found above ∼3000 m had their source in the Gobi desert region of northern China and Inner Mongolia, and were transported to the Yukon following a series of major dust storms that took place in early April. Dusts found below 3000 m had local (Yukon) or mixed source(s). The Asian dusts had a modal volume diameter of ∼4 μm typical of far-traveled mineral aerosols. However larger (>10 μm) particles were also found at ∼5000 m, suggesting a very rapid trans-Pacific transport in the mid-troposphere. We estimate that the April 2001 event deposited from 5500 to 6335 tons of dust over an area of 21,000 km² in the southwestern Yukon, most of which probably fell within a week. Our findings are consistent with instrumental observations and model simulations of the April 2001 event. While the dust cloud was reportedly mixed with volatile pollutants from Asia, we found no evidence of metal pollution associated with the dustfall in the Yukon. Our findings contribute to clarify the dynamics and the geochemical impact of Asian dust long-range transport events, and to better estimate eolian fluxes of dustborne elements (e.g., Fe) to the Ocean associated with such events. They may also assist in identifying past Asian dust events in ice cores drilled from the St. Elias Mountains icefields, to develop a long-term record of their frequency, magnitude and source(s).     

A study of the attachment of radon daughter atoms to aerosol particles

Previous studies of the attachment of radon daughter atoms to aerosol particles in the atmospheric air have given varying results, a few of which did not conform to the diffusion theory developed byLassen andRau (1960). Our studies suggest that the radiolytic aerosols formed by gas-phase reactions in the presence of ionizing radiations interfere in the studies carried out with known aerosols. Radiolytic aerosols are formed spontaneously in the system, depending on the concentrations of aerosol-forming gases in the atmospheric air. It is shown that, under experimental conditions which suppressed the formation of radiolytic aerosols, the attachment rates of Ra-A atoms to aerosol particles in the range of 0.2 to 1.0 m in diameter agree with the diffusion theory developed byLassen andRau (1960). Such investigations of the interactions between atoms, molecules, ions, and aerosol particles are highly useful in atmospheric tracer studies.     

Trends in the Different Grades of Precipitation over South China during 1960–2010 and the Possible Link with Anthropogenic Aerosols简

Using observed daily precipitation data to classify five levels of rainy days by strength in South China （SC）,with an emphasis on the Pearl River Delta （PRD） region,the spatiotemporal variation of different grades of precipitation during the period 1960-2010 was analyzed and the possible link with anthropogenic aerosols examined.Statistical analysis showed that drizzle and small precipitation has significantly decreased,whereas medium to heavy precipitation has increased slightly over the past 50 years （although not statistically significant）.Further data analysis suggested that the decline in drizzle and small precipitation probably has a strong link to increased concentrations of anthropogenic aerosols produced by large-scale human activities related to the rapid socioeconomic development of the PRD region.These aerosols may also have led to the obvious decreasing trend in horizontal visibility and sunshine duration in SC,which is statistically significant according to the t-test.     

Climate Change in the Subtropical Jetstream during 1950–2009

A study of six decades(1950–2009) of reanalysis data reveals that the subtropical jetstream(STJ) of the Southern(Northern) Hemisphere between longitudes 0°E and 180°E has weakened(strengthened) during both the boreal winter(January,February) and summer(July, August) seasons. The temperature of the upper troposphere of the midlatitudes has a warming trend in the Southern Hemisphere and a cooling trend in the Northern Hemisphere. Correspondingly, the north–south temperature gradient in the upper troposphere has a decreasing trend in the Southern Hemisphere and an increasing trend in the Northern Hemisphere, which affects the strength of the STJ through the thermal wind relation. We devised a method of isotach analysis in intervals of 0.1 m s-1in vertical sections of hemispheric mean winds to study the climate change in the STJ core wind speed, and also core height and latitude. We found that the upper tropospheric cooling of the Asian mid-latitudes has a role in the strengthening of the STJ over Asia, while throughout the rest of the globe the upper troposphere has a warming trend that weakens the STJ. Available studies show that the mid-latitude cooling of the upper troposphere over Asia is caused by anthropogenic aerosols(particularly sulphate aerosols) and the warming over the rest of the global mid-latitude upper troposphere is due to increased greenhouse gases in the atmosphere.     

Iron Distribution in Size‐Resolved Aerosols Generated by UV‐Femtosecond Laser Ablation: Influence of Cell Geometry and Implications for In Situ Isotopic Determination by LA‐MC‐ICP‐MS

The influence of ablation cell geometry (Frames single‐ and HelEx two‐volume cells) and laser wavelength (198 and 266 nm) on aerosols produced by femtosecond laser ablation (fs‐LA) were evaluated. Morphologies, iron mass distribution (IMD) and ⁵⁶Fe/⁵⁴Fe ratios of particles generated from magnetite, pyrite, haematite and siderite were studied. The following two morphologies were identified: spherules (10–200 nm) and agglomerates (5–10 nm). Similarity in IMD and ablation rate at 198 and 266 nm indicates similar ablation mechanisms. ⁵⁶Fe/⁵⁴Fe ratios increased with aerodynamic particle size as a result of kinetic fractionation during laser plasma plume expansion, cooling and aerosol condensation. The HelEx cell produces smaller particles with a larger range of ⁵⁶Fe/⁵⁴Fe ratios (1.85‰) than particles from the Frames cell (1.16‰), but the bulk aerosol matches the bulk substrate for both cells, demonstrating stoichiometric fs‐LA sampling. IMD differences are the result of faster wash out of the HelEx cell allowing less time for agglomeration of small, low‐δ ⁵⁶Fe particles with larger, high‐δ ⁵⁶Fe particles in the cell. Even with a shorter ablation time, half the total Fe ion intensity, and half the ablation volume, the HelEx cell produced Fe isotope determinations for magnetite that were as precise as the Frames cell, even when the latter included an aerosol‐homogenising mixing chamber. The HelEx cell delivered a more constant stream of small particles to the ICP, producing a more stable Fe ion signal (0.7% vs. 1.5% RSE for ⁵⁶Fe in a forty‐cycle single analysis), constant instrumental mass bias and thus a more precise measurement.     

Mie 散射激光雷达探测大气气溶胶的进展

简要论述了激光雷达探测大气的优点,以及求解M ie散射激光雷达方程的理论方法,并阐述了国内外近20 a来M ie散射激光雷达探测大气气溶胶的主要成果,及其存在的问题。     

近地面臭氧研究进展

近地面臭氧是空气中氮氧化物和挥发性有机物发生光化学反应的产物,其浓度与气象条件密切相关。晴天少云、紫外辐射较强、温度较高、相对湿度较低以及风速较小的天气,均有利于臭氧的生成,其中紫外辐射是产生臭氧最关键的因素。臭氧前体物（氮氧化物和挥发性有机物）的浓度及其比值是影响近地面臭氧浓度的另外三个重要因素。我国大多数城市的O3处于VOC控制区,即NOx浓度的增加会引起O3浓度的降低,而VOCs浓度的增加则会使其浓度升高。因而VOC源解析问题成为近年来O3研究的一个热点问题。同时,由于气溶胶可以直接吸收、散射太阳紫外辐射、短波辐射以及大气长波辐射,因此气溶胶的存在会影响大气中光化学反应的进程,从而影响臭氧的光化学生成,气溶胶对近地面臭氧的影响已成为目前大气环境的前沿课题。