临安大气气溶胶理化特性季节变化

分别利用碳成分分析仪、离子色谱仪和原子吸收光谱仪等获取浙江省临安地区大气气溶胶在春、夏、秋、冬四季的质量浓度、离子与碳成分特性，并对不同粒径气溶胶成分分布特点作了较详细分析。结果表明:气溶胶质量浓度、可溶性离子浓度以及碳成分浓度具有明显的季节变化趋势。整个尺度范围内，气溶胶质量浓度季节变化特点为春季浓度最高，达到534 μg/m3；冬季次之，质量浓度为117.21 μg/m3；夏季浓度最低，平均为65.7 μg/m3；秋季质量浓度98.6 μg/m3。可溶性离子成分在气溶胶中所占比例具有明显的季节性，其中夏季最高为49.4%，春季最低为11.3%。硫酸根离子SO₄2-和氨根离子NH₄+和硝酸根离子NO₃- 3种离子浓度之和约占离子总量的75%~83%。受温度影响，硝酸根离子NO₃-浓度随季节变化幅度较大，夏季平均浓度为1.7 μg/m3, 冬季平均浓度为11.5 μg/m3，是夏季浓度的6.8倍。碳浓度分布特点显示，气溶胶中元素碳浓度春季最高，夏季最低。有机碳浓度春季最高，冬季最低。气溶胶粒度分布特点也非常明显。四季中粒径小于11 μm（PM₁₁）的气溶胶均占气溶胶总量的90%以上，粒径小于2.1 μm（PM_2.1）的气溶胶占到气溶胶总量的53%以上。可溶性离子在粒径小于2.1 μm气溶胶颗粒中，以硫酸根离子、氨根离子和硝酸根离子为主。碳成分尺度分布特征为颗粒越小，有机碳及元素碳浓度越高。     

Effect of Atmospheric Haze on the Deterioration of Visibility over the Pearl River Delta

The studies on the effect of atmospheric aerosol on climate and environment are hot issues in the current circle of international science and technology. In recent years the pollution of aerosol is getting worse and worse over the Pearl River Delta. The clouds of aerosol occur all year round, with heavy pollution area located at the western side at the mouth of Pearl River. The haze weather mainly occurs from October to April next year, resulting in visibility deterioration. From the beginning of 1980s, visibility dramatically deteriorated, obviously increasing haze weather, in which there are three big fluctuations, showing the periods of pollutions of dust, sulphate and dust, fine particle from photochemical process and sulphate and dust accompanying with the development of economy respectively. The long-term tendency of visibility caused by fog and light fog does not show a tendency due to human activities or economic development, which mainly shows the interannual and interdecadal variation of climate. The deterioration of visibility has close relation to the fine particles over Pearl River Delta, with half of PM10 overpass the limited value set by national second graded standard (150μg m-3), meanwhile, all values of PM2.5 overpass the day-mean limited value of American national standard (65μg m-3), especially from October to January next year, monthly mean values of PM2.5 almost reach two times of standard value, indicating the fine particle concentration is very high. The ratio of PM2.5 to PM10 is also very high, reaching 58%-77%, higher especially in dry season than in rainy season. Thus it is the fine particle pollution in aerosol pollution over the Pearl River Delta. Compared with the data of 15 years ago, the ratio of fine particle to aerosol has obviously increased.     

利用多角度POLDER偏振资料实现陆地上空大气气溶胶光学厚度和地表反照率的同时反演 I. 理论与模拟

陆地上空标量辐射对地表反射率和大气气溶胶散射都具有很强的敏感性,而偏振反射只对大气气溶胶敏感,对地表不敏感。根据这个原理并结合POLDER(POLarization and Directionality of Earth Reflectance)资料的特点,作者提出综合利用标量辐射和偏振反射信息来实现陆地上空大气气溶胶和地表反照率的同时反演。首先,利用多角度偏振辐射观测提取大气气溶胶光学参数,再利用标量辐射测量对偏振反演结果作进一步筛选和订正,同时获得地表反射率。数值模拟试验结果证明,仅利用偏振信息只能获取大气气溶胶信息,而且其结果误差较大,特别是对于散射作用较强的短波长通道如670 nm误差更大,但经过标量辐射订正后的结果得到明显改善,气溶胶光学厚度和地表反射率与真实值之间相关系数都达到0.99以上。为提高查找表的计算效率,提出并建立了反演方案所需要的半参数化数值表,利用内插方法寻求气溶胶光学厚度和地表反射率的数值解的反演方法。     

南极威德尔海周边雪冰和大气气溶胶中的MSA,nssSO_4~(2-)浓度及其比率研究

分析了威德尔海周边雪冰和大气中ＭＳＡ和ｎｓｓＳＯ２－４浓度资料。结果表明,威德尔海是造成这一地区大气中高含量生物硫化物的“源”,其周边岛屿及冰架表层雪冰记载和反映了大气中生物硫化物的空间分布和季节变化特点。源区产出硫化物的强度存在显著差异：靠近南极半岛一侧高于靠近Ｆｉｌｃｈｎｅｒ－Ｒｏｎｎｅ冰架一侧。尽管诸多因素对输运和沉降过程发生影响,表层积雪ＭＳＡ和ｎｓＳＯ２－４浓度仍呈现出很有规律性的空间分布：随沉降地点离海距离和海拔高度的增加,浓度值递减;但在一定海拔之下,“高程效应”不显著。冰芯中ＭＳＡ浓度垂向分布显示出季节分配“滞后”现象,在表层表现为受天气条件制约的输运过程造成的相位差,在深层则归因于有待验证的“迁移”机制作用的结果。大气和雪冰样品对比研究结果表明,在类似威德尔海这样的高纬地区,大气中的ＳＯ２－４和ＭＳＡ“信号”在雪冰样品中会遭到不同程度的减弱。但就空间变化趋势和季节分布而言,表层雪冰仍是大气中组分（在本文是ＳＯ２－４和ＭＳＡ）的良好载体。十分接近的大气和雪冰ＭＳＡ对ｎｓｓＳＯ２－４（或ＳＯ２－４）比率证实,这两种大气组分在由大气洗净和沉降到冰雪过程中只发生微弱的分离作用。这也就是大气和雪冰中     

探讨气候变化的新热点:大气气溶胶的气候效应

气溶胶的气候效应是近年来研究的热点问题。针对这一问题已开展过许多观测研究和模式研究。但是由于气溶胶问题的复杂性以及对气溶胶的观测历史短,至今尚缺少全球范围的气溶胶系统观测资料,所以目前气溶胶的辐射强迫仍是个很不确定的量。这直接影响对全球气候变化的预测。目前国内外正在加强这方面的研究工作,并且有了一些初步的结果。概述了近期国内外对气溶胶的气候效应的研究状况及结果,介绍了今后国际上将要在这一领域开展的研究工作。     

An application of Mie's series to soft particles

Summary The scattering of electromagnetic radiation from soft particles has been studied by a new method which allows to transform the Mie series into a simplified form through the use of some auxiliary expansions derived in the Appendix of this article. This simplified form (eq. 1) converts into the Hulst and Rayleigh-Debye-Gans' formulae if the parameters of eq. I are properly restricted. A further simplified form (eq. II), improves the well-known Hulst approximation.     

Measurement of lower-stratospheric aerosol by a balloon-borne photometer

Height distribution of the stratospheric aerosol extinction coefficient was measured in the altitude range 10 to 20 km by a balloon-borne multi-color sunphotometer in May 1978. It is demonstrated that detailed structures of the distribution of stratospheric aerosol can be remotely measured by the solar occultation method as well as by lidar andin situ particle counter observations. In the aerosol layer appearing at 18 km altitude the extinction coefficient at 800–1000 nm wavelength reached to 3×10^–7 m^–1, which was reasonable compared with lidar observations. Wavelength dependence of the aerosol optical depth was crudely estimated to be proportional to ^–1.5.     

A Three-Dimensional Global Model Study of Carbonyl Sulfide in the Troposphere and the Lower Stratosphere

Global distributions of carbonyl sulfide and carbon disulfide have been calculated with a three-dimensional global model of the atmospheric general circulation (ECHAM). The model calculates a global sink strength for carbonyl sulfide of 0.3 Tg S yr^-1, with vegetation uptake being the largest sink. With this sink strength, the sources have to be close to the lower limit of the present estimate in the literature. The calculated mixing ratios are higher in the Southern Hemisphere than in the Northern Hemisphere. This interhemispheric gradient is the opposite of what is observed demonstrating that the present knowledge of the distribution of sinks and sources is not fully adequate. The model calculations support the idea that the open oceans could act as a net sink of carbonyl sulfide. The calculated stratospheric photolysis of carbonyl sulfide constitutes about 4% of the total sink of carbonyl sulfide. A stratospheric production of sulfate from carbonyl sulfide of 0.013 Tg S yr^-1 is obtained, which is 3 to 12 times less than what is needed to maintain the stratospheric sulfate aerosol layer. Although these results are associated with uncertainties, due to the low upper boundary and coarse vertical resolution of the model, they support recent findings of a low stratospheric production of sulfate from carbonyl sulfide. Instead, sulfur dioxide transported from the troposphere is calculated to be the most important precursor for the stratospheric sulfate aerosol layer.     

The Henry's Law Constants of the Haloacetic Acids

Henry's law constants K_H (mol kg^-1 atm^-1) have been measured between 278.15 K and 308.15 K for the following organic acids: CH₂FCOOH (ln(K_H[298.15 K]) = 11.3 ± 0.2), CH₂ClCOOH (11.59 ± 0.14), CH₂BrCOOH (11.94 ± 0.21), CHF₂COOH (10.32 ± 0.10), CHCl₂COOH (11.69 ± 0.11), CHBr₂COOH (12.33 ± 0.29), CBr₃COOH (12.61 ± 0.21), and CClF₂COOH (10.11 ± 0.12). The variation of K_H with temperature was determined for all acids except CH₂FCOOH and CBr₃COOH, with _r H° for the dissolution reaction ranging from –85.2 ± 2.6 to –57.1 ± 2.5 kJ mol^-1, meaning that their solubility is generally more sensitive to temperature than is the case for the simple carboxylic acids. The Henry's law constants show consistent trends with halogen substitution and, together with their high solubility compared to the parent (acetic) acid (ln(K_H[298.15 K]) = 8.61), present a severe test of current predictive models based upon molecular structure. The solubility of haloacetic acids and strong dissociation at normal pH mean that they will partition almost entirely into cloud and fog in the atmosphere (0.05–1.0 g H₂O m^-3), but can reside in both phases for the liquid water contents typical of aerosols (10^-5-10^-4 g H₂O m^-3).