Hardening of Titan's aerosols by their charging

Titan's haze consists of long chain polymers of pure and N-mixed hydrocarbons (Coustenis et al., 1989, Icarus 80, 54-76, 1991, Icarus 89, 152-167). These polymers have regularly alternating (i.e., conjugated) double/single and triple/single bonds, which open either spontaneously (free aging) or under the action of some external factors (forced aging), the latter being very diverse, e.g., charging, photolysis, radiolysis, thermolysis, chemical effect of environment, etc. An essential of free aging was examined previously (Dimitrov and Bar-Nun, 2002, Icarus 156, 530-538). The main distinction between free and any forced aging is that both of them possess the same thermodynamics while different kinetics, the forced aging in any case being faster, proceeding in different pathways than the free aging. The more extensive is the list of the external effects and the more intensive they are, the faster and more variably the forced aging proceeds. In this paper we quantified the kinetics of forced aging, considering charging of Titan's aerosol population. It was found that forced aging proceeds approximately hundred times faster as compared to the free aging. Various physico-chemical properties of Titan's aerosol material, including coagulation coefficients, depending on particle size and medium conditions, were defined. The comparison of the aging rate, rate of sedimentation and rate of the particle increase proves that Titan's aerosol domain can be subdivided conditionally into two big subdomains. The upper one contains minor portion (<5%) of the total aerosol bulk, unannealed aerosol particles being fine and sticky. The lower subdomain contains the major portion (>95%) of aerosol bulk, which is completely aged, coarsely dispersed particles. We established the border between these subdomains at the altitude Z∼620 km.     

Global climatic change – the latest scientific understanding

IPCCs statement in its 1995 report (IPCC 1996) that a human influence was discernible in global climate has been widely quoted but often misunderstood. The character of the evidence underpinning this detection statement is explained so that its strengths and weaknesses can be better understood and the subtleties of its message better appreciated. To demonstrate the close linkage between the government-approved summary and the underlying chapters of the IPCC report the detailed evolution of the detection statement from first draft through to the form finally approved by the IPCC is described.     

Particulate content of savanna fire emissions

As part of the FOS-DECAFE experiment at Lamto (Ivory Coast) in January 1991, various aerosol samples were collected at ground level near prescribed fires or under local background conditions, to characterize the emissions of particulate matter from the burning of savanna vegetation. This paper deals with total aerosol (TPM) and carbon measurements. Detailed trace element and polycyclic hydrocarbon data are discussed in other papers presented in this issue.Near the fire plumes, the aerosols from biomass burning are primarily of a carbonaceous nature (C%70% of the aerosol mass) and consist predominantly of submicron particles (more than 90% in mass.) They are characterized by their organic nature (black to total carbon ratio Cb/Ct in the range 3–20%) and their high potassium content (K/Cb0.6). These aerosols undergo aging during their first minutes in the atmosphere causing slight alterations in their size distribution and chemical composition. However, they remain enriched in potassium (K/Cb=0.21) and pyrene, a polycyclic aromatic hydrocarbon, such that both of these species may be used as tracers of savanna burning aerosols. We show that during this period of the year, the background atmosphere experiences severe pollution from both terrigenous sources and regional biomass burning (44% of the aerosol). Daynight variations of the background carbon concentrations suggest that fire ignition and spreading occur primarily during the day. Simultaneous TPM and CO₂ real-time measurements point to a temporal and spatial heterogeneity of the burning so that the ratio of the above background concentrations (TPM/CO₂) varies from 2 to 400 g/kg C. Smoldering processes are intense sources of particles but particulate emissions may also be important during the rapidly spreading heading fires in connection with the generation of heavy brown smoke. We propose emission factor values (EF) for aerosols from the savanna biomass burning aerosols: EF (TPM)=11.4±4.6 and 69±25 g/kg C_{dry plant} and EF(Ct)=7.4±3.4 and 56±16 g C/kg C_{dry plant} for flaming and smoldering processes respectively. In these estimates, the range of uncertainty is mostly due to the intra-fire variability. These values are significantly lower than those reported in the literature for the combustion of other types of vegetation. But due to the large amounts of vegetation biomass being burnt in African savannas, the annual flux of particulate carbon into the atmosphere is estimated to be of the order of 8 Tg C, which rivals particulate carbon emissions from anthropogenic activities in temperate regions.     

DMS and SO2 at Baring Head, New Zealand: Implications for the Yield of SO2 from DMS

Atmospheric dimethyl sulfide (DMS) and sulfur dioxide (SO₂) concentrations were measured at Baring Head, New Zealandduring February and March 2000. Anti-correlated DMS and SO₂ diurnalcycles, consistent with the photochemical production of SO₂ from DMS, were observed in clean southerly air off the ocean. The data is used to infer a yield of SO₂ from DMS oxidation. The estimated yields are highly dependent on assumptions about the DMS oxidation rate. Fitting the measured data in a photochemical box model using model-generated OH levels and the Hynes et al. (1986) DMS + OH rate constant suggests that theSO₂ yield is 50–100%, similar to current estimates for the tropical Pacific.However, the observed amplitude of the DMS diurnal cycle suggests that the oxidation rate is higher than that used by the model, and therefore, that theSO₂ yield is lower in the range of 20–40%.     

Influence of Changes in the Prevailing Synoptic Conditions on the Response of Aerosol Characteristics to Land- and Sea-Breeze Circulations at a Coastal Station

The changes in the response of near surfaceaerosol properties to land- and sea-breezecirculations, associated with the changes in the prevailing synoptic meteorological conditions, are examined for a tropical coastal station. Aerosol properties are nearly similar in both the breeze regimes (land and sea) during seasons of marine airmass while they are distinct during seasons of continental airmass. As the prevailing winds shift from continental to marine and the ambient weather changes from winter conditions to the humid monsoon season, the submicron mode, which dominated the aerosol mass-size distribution, is largely suppressed and the dominance of the super micron mode increases. During periods of continental air mass (winter), the aerosol loading is significantly higher in the land-breeze regime, (particularly in the submicron range) but as the winds shift to marine, the loading initially becomes insensitive to the breeze regimes and later becomes higher in the sea-breeze regime, particularly in the super micron range.     

A model study on the decay of volcanic aerosol layer and verification with Pinatubo and El Chichon data

The time evolution of stratospheric aerosol layer formed after a volcanic eruption is studied taking into account the aerosol microphysical processes of growth, coagulation and sedimentation. Using a simple model we could explain the observed evolution of the Pinatubo volcanic layer which decayed in about 3 years. The experimental data obtained by Nd:YAG backscatter lidar over Ahmedabad further supports this finding. The data obtained after the El Chichon volcanic eruption also showed that the El Chichon aerosol layer decayed in about 3 years time. Thus, though the amount of SO₂ injected has been higher, in the case of Pinatubo, about two to three times more than El Chichon, it has resulted in the production of larger aerosol particles due to faster growth and coagulation processes, and subsequently a faster removal rate, to give more or less a similar background aerosol amount at the stratosphere in about 3 years time.     

EXPERIMENTAL STUDY ON EFFECTS OF HUMIDITY AND CHEMICAL COMPOSITION UPON IMAGINARY PART OF REFRACTIVE INDEX OF AEROSOL PARTICLES*

Experimental study is made of the relationship between the imaginary part of refractive index (IRI) of atmospheric aerosol particles and relative humidity,and between IRI and chemical element through the assay of chemical constituents of the particles.Evidence suggests that atmospheric humidity and aerosols' chemical ingredients have great effects on the IRI's and they should thus be considered in the research of the radiation properties of the particles in the atmosphere.     

基于气象要素的气溶胶吸湿增长分析:以浙江省为例

气溶胶粒子的吸湿增长对区域环境、气象与辐射收支都有巨大影响,精确的气溶胶吸湿特性观测对描述气溶胶吸湿增长特性,以及研究气溶胶对气候环境影响,拓展卫星气溶胶产品的应用有非常重要的意义。本研究提出一种基于常规气象观测（能见度、相对湿度）和空气质量观测（PM2.5浓度,即空气动力学当量直径小于等于2.5 μm的颗粒物浓度）相结合的气溶胶吸湿增长估算方法,在此基础上对浙江地区气溶胶吸湿特性的时空变化影响因素进行了探讨。研究发现,沿海的温州瓯海站的吸湿增长能力最高,长三角典型城市环境的杭州和睦小学站的吸湿增长能力次之,而地处较为洁净内陆的衢州实验学校站的吸湿增长能力最低。在时间变化中,同一站点不同湿度条件的吸湿增长变化趋势相同,温州瓯海站的吸湿性变化最为剧烈,杭州和睦小学站的吸湿性变化次之,衢州实验学校站变化较为平缓。本研究表明,浙江地区的气溶胶吸湿增长特性存在较大的时空差异,基于本方法能够在较大的时空范围内描述气溶胶的吸湿增长特性,为有限的精密观测提供重要补充。     

复合体系有机气体氧化生成二次有机气溶胶研究进展

生物源与人为源有机气体氧化形成的二次有机气溶胶(SOA)对气候变化和人类健康具有重要影响。SOA的产生与其前体物研究已取得了一些进展,但由于有机气体之间存在复合相互作用以及SOA形成机制复杂,目前对不同有机气体混合体系中SOA的形成认知还比较匮乏。因此,深入了解有机气体多源、复杂的相互作用,摸清有机气体的大气氧化机制、SOA的形成及影响等对深入理解真实大气有机气体化学演变具有指导意义。本文旨在了解复合体系有机气体氧化生成SOA的相关研究进展。一方面总结了复合体系有机气体产生SOA质量浓度、产率、成分、挥发性、光学性质等的变化,侧重于实验室复合体系有机气体氧化对SOA形成的多重影响以及SOA组成元素、分子构成的变化特征,并总结了目前实验室基于模型对复合体系SOA生成的模拟研究和拟合情况;另一方面探究了环境因素,如相对湿度(RH)、温度(T)以及无机气体,如氮氧化物(NO_x)、二氧化硫(SO₂)、氨气(NH₃)等对复合体系有机气体形成SOA的影响。     

2007-2017年中国沙尘气溶胶的三维分布特征及输送过程

利用最新发布的CALIPSO产品,构建了2007-2017年中国沙尘气溶胶的三维分布,并结合HYSPLIT-4模式和再分析数据,探讨了沙尘的三维输送过程。结果表明：中国的沙尘排放源区主要是塔克拉玛干沙漠和巴丹吉林沙漠,沙尘气溶胶出现频率分别为60%和35%。塔克拉玛干沙漠排放的沙尘主要（50%~70%）停留在源地0~6 000 m高度,少部分向东输送至甘肃和内蒙古;巴丹吉林沙漠排放的沙尘则主要向东输送。中国沙尘排放量在春季最大,向东输送最强;夏季,东亚夏季风限制了沙尘向东输送;秋季,沙尘排放减弱,输送强度和夏季相当;沙尘排放量在冬季最小,输送最弱。夏季,沙尘在输送过程中可被抬升至高度5 000 m以上,春季次之,秋、冬季的沙尘主要在低层大气输送。沙尘在向东输送的过程中被抬升并和当地人为污染物混合变为污染性沙尘,华北地区污染性沙尘出现频率高达30%;输送到海洋的沙尘也会与洋面上（0~3 000 m高度）的海盐气溶胶混合,出现频率约为10%。