On the optical properties of the polluted Athens atmosphere,during May 1995

Using ground-based spectral solar extinction data taken over the Athens atmosphere, reduced (total minus Rayleigh) and aerosol (Angstrom) spectral optical depths of the atmosphere, have been retrieved, under different polluted conditions. The results suggest that the optical depth, on days with relatively low pollution, exhibits slight variation with wavelength denoting that aerosols deplete all wavelengths almost equally. In contrast, under dense pollution, small particles scattering and trace gases absorption, are the dominant processes, resulting in steeper optical depth’s slopes, mainly in the ultraviolet domain. The Angstrom’s parameters β and α were determined through a least-squares fitting method. The turbidity β coefficient always shows a temporal pattern with high values in the morning and afternoon and low values midday.     

Atmospheric composition change: Climate–Chemistry interactions

Chemically active climate compounds are either primary compounds like methane (CH₄), removed by oxidation in the atmosphere, or secondary compounds like ozone (O₃), sulfate and organic aerosols, both formed and removed in the atmosphere. Man-induced climate–chemistry interaction is a two-way process: Emissions of pollutants change the atmospheric composition contributing to climate change through the aforementioned climate components, and climate change, through changes in temperature, dynamics, the hydrological cycle, atmospheric stability, and biosphere-atmosphere interactions, affects the atmospheric composition and oxidation processes in the troposphere. Here we present progress in our understanding of processes of importance for climate–chemistry interactions, and their contributions to changes in atmospheric composition and climate forcing. A key factor is the oxidation potential involving compounds like O₃ and the hydroxyl radical (OH). Reported studies represent both current and future changes. Reported results include new estimates of radiative forcing based on extensive model studies of chemically active climate compounds like O₃, and of particles inducing both direct and indirect effects. Through EU projects like ACCENT, QUANTIFY, and the AeroCom project, extensive studies on regional and sector-wise differences in the impact on atmospheric distribution are performed. Studies have shown that land-based emissions have a different effect on climate than ship and aircraft emissions, and different measures are needed to reduce the climate impact. Several areas where climate change can affect the tropospheric oxidation process and the chemical composition are identified. This can take place through enhanced stratospheric–tropospheric exchange of ozone, more frequent periods with stable conditions favoring pollution build up over industrial areas, enhanced temperature induced biogenic emissions, methane releases from permafrost thawing, and enhanced concentration through reduced biospheric uptake. During the last 5–10 years, new observational data have been made available and used for model validation and the study of atmospheric processes. Although there are significant uncertainties in the modeling of composition changes, access to new observational data has improved modeling capability. Emission scenarios for the coming decades have a large uncertainty range, in particular with respect to regional trends, leading to a significant uncertainty range in estimated regional composition changes and climate impact.     

Modeling of temporal variations of vertical concentration profile of 7Be in the atmosphere

Study of the vertical concentration profile and of the deposition of cosmogenic radionuclides provides information on the vertical transport in the stratosphere and troposphere and the processes of scavenging of aerosol particles by precipitation. Information on the distribution of atmospheric aerosols is important for the understanding of the physical processes relating to the studies in weather climate, air pollution, and aerosol physics. In this work the one-dimensional steady-state model of vertical concentration profile was established and the values of turbulent diffusion coefficient and scavenging coefficient determined by model using experimental data of the ⁷Be monthly average atmospheric activity concentrations and monthly deposition fluxes in Bratislava are presented. The temporal variations of the vertical distribution profiles of ⁷Be for each month are also calculated.     

Atmospheric turbidity in Kuwait

The paper discusses the effect or atmospheric constituents on the depletion or beam radiation in Kuwait with particular emphasis on the effect or aerosol particles. It is shown that atmospheric turbidity is particularly large during June and July as compared to other months of the year. It is also shown that for a good part of the year the effect of aerosol particles on beam radiation attenuation is equivalent to, or larger than, the combined effects of ozone, water vapor and gas molecules.     

Transport impacts on atmosphere and climate: Metrics

The transport sector emits a wide variety of gases and aerosols, with distinctly different characteristics which influence climate directly and indirectly via chemical and physical processes. Tools that allow these emissions to be placed on some kind of common scale in terms of their impact on climate have a number of possible uses such as: in agreements and emission trading schemes; when considering potential trade-offs between changes in emissions resulting from technological or operational developments; and/or for comparing the impact of different environmental impacts of transport activities.Many of the non-CO₂ emissions from the transport sector are short-lived substances, not currently covered by the Kyoto Protocol. There are formidable difficulties in developing metrics and these are particularly acute for such short-lived species. One difficulty concerns the choice of an appropriate structure for the metric (which may depend on, for example, the design of any climate policy it is intended to serve) and the associated value judgements on the appropriate time periods to consider; these choices affect the perception of the relative importance of short- and long-lived species. A second difficulty is the quantification of input parameters (due to underlying uncertainty in atmospheric processes). In addition, for some transport-related emissions, the values of metrics (unlike the gases included in the Kyoto Protocol) depend on where and when the emissions are introduced into the atmosphere – both the regional distribution and, for aircraft, the distribution as a function of altitude, are important.In this assessment of such metrics, we present Global Warming Potentials (GWPs) as these have traditionally been used in the implementation of climate policy. We also present Global Temperature Change Potentials (GTPs) as an alternative metric, as this, or a similar metric may be more appropriate for use in some circumstances. We use radiative forcings and lifetimes from the literature to derive GWPs and GTPs for the main transport-related emissions, and discuss the uncertainties in these estimates. We find large variations in metric (GWP and GTP) values for NO_x, mainly due to the dependence on location of emissions but also because of inter-model differences and differences in experimental design. For aerosols we give only global-mean values due to an inconsistent picture amongst available studies regarding regional dependence. The uncertainty in the presented metric values reflects the current state of understanding; the ranking of the various components with respect to our confidence in the given metric values is also given. While the focus is mostly on metrics for comparing the climate impact of emissions, many of the issues are equally relevant for stratospheric ozone depletion metrics, which are also discussed.     

Radiative effects of aerosols over Indo-Gangetic plain: environmental (urban vs. rural) and seasonal variations

Aerosol radiative effects over two environmentally distinct locations, Kanpur (urban site) and Gandhi College (rural location) in the Indo-Gangetic plain (IGP), a regional aerosol hot spot, utilizing the measured optical and physical characteristics of aerosols, an aerosol optical properties model and a radiative transfer model, are examined. Shortwave aerosol radiative forcing (ARF) at the top of the atmosphere (TOA) is 30 W m(?-?2)). Shortwave atmospheric heating due to aerosols is >0.4 K/day over IGP and peaks during premonsoon at >0.6 K/day due to lower single scattering albedo (SSA) and higher surface albedo. TOA forcing is always less negative over Kanpur when compared to Gandhi College due to lower surface albedo except in postmonsoon owing to higher SSA. This happens as TOA forcing depends on SSA and surface albedo in addition to aerosol optical depth. The magnitude of longwave forcing and atmospheric cooling in an absolute sense is significantly small and contributes only about 20% or less to the net (shortwave + longwave) forcing. Aerosol radiative effects over these two locations, despite differences in aerosol characteristics, are similar, thus confirming that aerosols and their radiative influence get transported due to circulation. ARF over Kanpur and Gandhi College is an order of magnitude higher when compared to greenhouse gas forcing. A large reduction in surface reaching solar irradiance accompanied by large atmospheric warming can have implications on precipitation and hydrological cycle, and these aerosol radiative effects should be included while performing regional-scale aerosol climate assessments.     

The impacts of combustion emissions on air quality and climate – From coal to biofuels and beyond

Combustion processes have inherent characteristics that lead to the release in the environment of both gaseous and particulate pollutants that have primary and secondary impacts on air quality, human health, and climate. The emissions from the combustion of fossil fuels and biofuels and their atmospheric impacts are reviewed here with attention given to the emissions of the currently regulated pollutant gasses, primary aerosols, and secondary aerosol precursors as well as the emissions of non-regulated pollutants. Fuels ranging from coal, petroleum, liquefied petroleum gas (LPG), natural gas, as well as the biofuels; ethanol, methanol, methyl tertiary-butyl ether (MTBE), ethyl tertiary-butyl ether (ETBE), and biodiesel, are discussed in terms of the known air quality and climate impacts of the currently regulated pollutants. The potential importance of the non-regulated emissions of both gasses and aerosols in air quality issues and climate is also discussed with principal focus on aldehydes and other oxygenated organics, polycyclic aromatic hydrocarbons (PAHs), and nitrated organics. The connection between air quality and climate change is also addressed with attention given to ozone and aerosols as potentially important greenhouse species.     

Uncertainty Requirements in Radiative Forcing of Climate Change

Abstract

The continuing increase in atmospheric carbon dioxide (CO₂) makes it essential that climate sensitivity, the equilibrium change in global mean surface temperature that would result from a given radiative forcing, be quantified with known uncertainty. Present estimates are quite uncertain, 3 ± 1.5 K for doubling of CO₂. Model studies examining climate response to forcing by greenhouse gases and aerosols exhibit large differences in sensitivities and imposed aerosol forcings that raise questions regarding claims of their having reproduced observed large-scale changes in surface temperature over the 20th century. Present uncertainty in forcing, caused largely by uncertainty in forcing by aerosols, precludes meaningful model evaluation by comparison with observed global temperature change or empirical determination of climate sensitivity. Uncertainty in aerosol forcing must be reduced at least three-fold for uncertaintyin climate sensitivity to be meaningfully reduced and bounded.     

A quantitative comparison of α-Å turbidity parameter retrieved in different spectral ranges based on spectroradiometer solar radiation measurements

Spectroradiometric direct irradiance measurements in the 300–1100 nm wavelength range with a spectral resolution of 6.2 nm have been used in a study of the variation in the Ångström turbidity parameter α and its dependence on the spectral range used in its determination. The measurements have been carried out under clear sky conditions at two different climate stations in Spain. Least-square fits of the experimental spectral aerosol optical depth (AOD) to the Ångström formula in different spectral ranges, selected for convenience depending on the objective or application (e.g., UV–VIS (350–400 nm), VIS (400–670 nm), VIS–NIR (370–870 nm), etc.), result in different sets for the α parameter. Due to this dependence on the spectral range, where the α-values are determined, a quantitative comparative analysis is carried out in order to assess the differences for a given data-base covering very different atmospheric conditions. The study reveals the necessity of a ‘standard spectral range’ to achieve confident data comparisons. We show some applications that are relevant for aerosol studies, from UV absorption by aerosols to satellite remote sensing.     

Uncertainty requirements in radiative forcing of climate change

The continuing increase in atmospheric carbon dioxide (CO2) makes it essential that climate sensitivity, the equilibrium change in global mean surface temperature that would result from a given radiative forcing, be quantified with known uncertainty. Present estimates are quite uncertain, 3 +/- 1.5 K for doubling of CO2. Model studies examining climate response to forcing by greenhouse gases and aerosols exhibit large differences in sensitivities and imposed aerosol forcings that raise questions regarding claims of their having reproduced observed large-scale changes in surface temperature over the 20th century. Present uncertainty in forcing, caused largely by uncertainty in forcing by aerosols, precludes meaningful model evaluation by comparison with observed global temperature change or empirical determination of climate sensitivity. Uncertainty in aerosol forcing must be reduced at least three-fold for uncertainty in climate sensitivity to be meaningfully reduced and bounded.     

Atmospheric turbidity over Kathmandu valley

The atmosphere of Kathmandu Valley has been investigated by using Sunphotometer and Nephelometer during the pre-monsoon period of 1999. The atmospheric turbidity parameters (extinction coefficient for 500 nm wavelength τ_AG and Angstrom coefficient β) are found high in the morning and show decreasing trends from morning to late afternoon on average. Vertical dispersion of pollutants and increasing pollutant flushing rate by increasing wind speed from morning to late afternoon is the cause for this decreasing trend of turbidity over the valley. Being surrounded by high hills all around the valley, horizontal exit of pollutants without vertical dispersion is not possible. The scattering coefficient b_scat of aerosols in ground level troposphere is also found high in the morning, which decreases and becomes minimum during afternoon. During late afternoon, b_scat again shows a slightly increasing trend. The reason is the increasing vehicular emission during late afternoon rush period. The average values of Angstrom exponent α, β, τ_AG and b_scat are found to be 0.624±0.023, 0.299±0.009, 0.602±0.022 and 0.353±0.014 km⁻¹, respectively. About 76.8% of the observed values of β lie above 0.2 indicating heavy particulate pollution in the valley. A comparison of observed values of turbidity parameters with other major cities of the world shows that Kathmandu is as polluted as cities like Jakarta, Kansas, Beijing, Vienna, etc.     

State of mixture of atmospheric submicrometer black carbon particles and its effect on particulate light absorption

The state of mixture of light-absorbing carbonaceous particles was investigated in relation to light absorption properties using electron microscopic examinations, black carbon (BC) analyses of quartz filter by thermal/optical reflectance (TOR) method, measurements with two continuous light-absorbing photometers at a suburban site of Tsukuba, about 60 km northeast of Tokyo. The volume fraction of water-soluble material (?) in individual particles is important for assessing particulate light-absorbing and/or scattering of atmospheric aerosols. The values of ? in BC particles were evaluated by electron micrographs before and after dialysis (extraction) of water-soluble material. The mass absorption coefficient (MAC in units of m² g^?1) tended to increase with increasing the average ? in BC particles with the radius range of 0.05–0.5 μm. Thus, our results indicate that coatings of water-soluble material around BC particles can enhance the absorption of solar radiation. Moreover, the single scattering albedo (SSA) will increase because a large amount of coating material will scatter more light.     

Factors influencing concentrations of dissolved gaseous mercury (DGM) and total mercury (TM) in an artificial reservoir

The effects of various factors including turbidity, pH, DOC, temperature, and solar radiation on the concentrations of total mercury (TM) and dissolved gaseous mercury (DGM) were investigated in an artificial reservoir in Korea. Episodic total mercury accumulation events occurred during the rainy season as turbidity increased, indicating that the TM concentration was not controlled by direct atmospheric deposition. The DGM concentration in surface water ranged from 3.6 to 160 pg/L, having a maximum in summer and minimum in winter. While in most previous studies DGM was controlled primarily by a photo-reduction process, DGM concentrations tracked the amount of solar radiation only in winter when the water temperature was fairly low in this study. During the other seasons microbial transformation seemed to play an important role in reducing Hg(II) to Hg(0). DGM increased as dissolved organic carbon (DOC) concentration increased (p-value < 0.01) while it increased with a decrease of pH (p-value < 0.01).     

Effect of composition on aerosol light scattering efficiencies

Forecasts of the impact of emissions changes on visibility use light scattering efficiencies—the change in the amount of light scattered with a change in mass of an aerosol constituent. This paper demonstrates how light scattering efficiencies depend on interactions between the aerosol constituents. Calculations are presented for two model aerosols: NH₄HSO₄ droplets and a ‘typical’ urban aerosol. These calculations demonstrate that the traditional means of predicting visibility impairment for increases in atmospheric emissions is not generally appropriate. Different light scattering efficiencies are needed for distinct meteorological conditions and aerosol compositions thus for typical high and low visibility events.     

Air pollution,greenhouse gases and climate change: Global and regional perspectives

Greenhouse gases (GHGs) warm the surface and the atmosphere with significant implications for rainfall, retreat of glaciers and sea ice, sea level, among other factors. About 30 years ago, it was recognized that the increase in tropospheric ozone from air pollution (NO_x, CO and others) is an important greenhouse forcing term. In addition, the recognition of chlorofluorocarbons (CFCs) on stratospheric ozone and its climate effects linked chemistry and climate strongly. What is less recognized, however, is a comparably major global problem dealing with air pollution. Until about ten years ago, air pollution was thought to be just an urban or a local problem. But new data have revealed that air pollution is transported across continents and ocean basins due to fast long-range transport, resulting in trans-oceanic and trans-continental plumes of atmospheric brown clouds (ABCs) containing sub micron size particles, i.e., aerosols. ABCs intercept sunlight by absorbing as well as reflecting it, both of which lead to a large surface dimming. The dimming effect is enhanced further because aerosols may nucleate more cloud droplets, which makes the clouds reflect more solar radiation. The dimming has a surface cooling effect and decreases evaporation of moisture from the surface, thus slows down the hydrological cycle. On the other hand, absorption of solar radiation by black carbon and some organics increase atmospheric heating and tend to amplify greenhouse warming of the atmosphere.ABCs are concentrated in regional and mega-city hot spots. Long-range transport from these hot spots causes widespread plumes over the adjacent oceans. Such a pattern of regionally concentrated surface dimming and atmospheric solar heating, accompanied by widespread dimming over the oceans, gives rise to large regional effects. Only during the last decade, we have begun to comprehend the surprisingly large regional impacts. In S. Asia and N. Africa, the large north-south gradient in the ABC dimming has altered both the north-south gradients in sea surface temperatures and land–ocean contrast in surface temperatures, which in turn slow down the monsoon circulation and decrease rainfall over the continents. On the other hand, heating by black carbon warms the atmosphere at elevated levels from 2 to 6 km, where most tropical glaciers are located, thus strengthening the effect of GHGs on retreat of snow packs and glaciers in the Hindu Kush-Himalaya-Tibetan glaciers.Globally, the surface cooling effect of ABCs may have masked as much 47% of the global warming by greenhouse gases, with an uncertainty range of 20–80%. This presents a dilemma since efforts to curb air pollution may unmask the ABC cooling effect and enhance the surface warming. Thus efforts to reduce GHGs and air pollution should be done under one common framework. The uncertainties in our understanding of the ABC effects are large, but we are discovering new ways in which human activities are changing the climate and the environment.     

Fractal modelling of carbonaceous aerosols—application to car exhaust plumes

Most commonly, atmospheric aerosol particles are ideally modelled as spheres allowing for straightforward calculations of their geometrical properties (diameter, surface and volume) and ensuing radiative, dynamical and chemical characteristics. However, particles issued particularly from combustion processes display various structural types, from linear clusters to quasi-spherical ones. Such various shapes result in quite different physical and chemical particle characteristics: e.g. the processes of absorption, coagulation/sintering and deposition are strongly affected by the fractal morphology of such aerosols. Whereas only one discretization parameter (diameter, d) is required for the spectral distribution n(d) of spherical particles, it is necessary to use a 2D distribution n(v,a) for fractal ones, v and a being, respectively, the volume and area of particles. For the coagulation process the associated governing aerosol population balance equation not only involves a collision term but also another term for more or less complete coalescence (sintering). For example, in view of the general texture of carbonaceous aerosols proposed by Strommen and Kamens (Environmental Science and Technology 31 (1997) 2983), let us consider two colliding particles each made of elementary carbon spherules immersed within a viscous organic liquid. They tend to more or less rapidly and completely merge, according to their bulk viscosities and surface tensions. In a first limit case, particles only stick together, displaying a maximum overall area. The other limit case is obtained through full particle merging into spherical structures. The new fractal model proposed, appropriate for describing such diverse particle morphologies, is then applied to car exhaust plumes.     

Chemical compositions and radiative properties of dust and anthropogenic air masses study in Taipei Basin, Taiwan, during spring of 2004

Asia is one of the major sources of not only mineral dust but also anthropogenic aerosols. Continental air masses associated with the East Asian winter monsoon always contain high contents of mineral dust and anthropogenic species and transported southeastward to Taiwan, which have significant influences on global atmospheric radiation transfer directly by scattering and absorbing solar radiation in each spring. However, few measurements for the long-range transported aerosol and its optical properties were announced in this area, between the Western Pacific and the southeastern coast of Mainland China. The overall objective of this work is to quantify the optical characteristics of different aerosol types in the Eastern Asian. In order to achieve this objective, meteorological parameters, concentrations of PM₁₀ and its soluble species, and optical property of atmospheric scattering coefficients were measured continuously with 1 h time-resolved from 11 February to 7 April 2004 in Taipei Basin (25°00′N, 121°32′E). In this work, the dramatic changes of meteorological parameters such as temperature and winds were used to determine the influenced period of each air mass. Continental, strong continental, marine, and stagnant air masses defined by the back-trajectory analysis and local meteorology were further characterized as long-range transport pollution, dust, clean marine, and local pollution aerosols, respectively, according to the diagnostic ratios. The aerosol mass scattering efficiency of continental pollution, dust, clean marine, and local pollution aerosols were ranged from 1.3 to 1.6, 0.7 to 1.0, 1.4 and 1.4 to 2.3 m² g⁻¹, respectively. Overall, there are two distinct populations of aerosol mass scattering efficiencies, one for an aerosol chemical composition dominated by dust (<1.0 m² g⁻¹) and the other for an aerosol chemical composition dominated by anthropogenic pollutants (1.3–2.3 m² g⁻¹), which were similar to the previous measurements with high degree of temporal resolution.     

Identification of C6 – C15 γ-Lactones in atmospheric aerosols

γ-Lactones with 6 – 15 carbons have been detected for the first time in atmospheric aerosols. Their concentrations ranged from 0.07 ng/m³ to 0.7 ng/m³.     

我国大气污染化学研究进展

本文综述了我国大气污染化学研究的概况。阐明了大气颗粒物（气溶胶）的表征研究，包括颗粒物的物理化学特性和环境化学行为；大气污染物的迁移、转化和归宿的规律，包括化学过程和大气化学模式的研究等。介绍了某些大气污染物的特殊分析测试方法和采样技术，对今后发展大气化学的展望和战略作了讨论。     

Carbon content of common airborne fungal species and fungal contribution to aerosol organic carbon in a subtropical city

Interest in the role and contribution of fungi to atmospheric aerosols and processes grows in the past decade. Substantial data or information such as fungal mass or carbon loading to ambient aerosols is however still lacking. This study aimed to quantify the specific organic carbon content (OC per spore) of eleven fungal species commonly found airborne in the subtropics, and estimated their contribution to organic carbon in aerosols. The specific OC contents showed a size-dependent relationship (r = 0.64, p < 0.05) and ranged from 3.6 to 201.0 pg carbon per spore or yeast cell, giving an average of 6.0 pg carbon per spore (RSD 51%) for spore or cell size less than 10 μm. In accounting for natural variations in the composition and abundance of fungal population, weighted-average carbon content for field samples was adopted using the laboratory determined specific OC values. An average of 5.97 pg carbon per spore (RSD 3.8%) was enumerated from 28 field samples collected at the university campus. The mean fungal OC concentration was 3.7, 6.0 and 9.7 ng m^?3 in PM_2.5, PM_2.5–10 and PM₁₀, respectively. These corresponded to 0.1%, 1.2% and 0.2% of the total OC in PM_2.5, PM_2.5–10 and PM₁₀, respectively. In the study period, rain provided periods with low total OC but high fungal prevalence and fungi contributed 7–32% OC in PM_2.5–10 or 2.4–7.1% OC in PM₁₀. More extensive studies are deserved to better understand the spatial-, temporal- and episodic dependency on the fungal OC contribution to the atmospheric aerosols.