Impact of aerosols on total columnar ozone measurements—a case study using satellite and ground-based instruments

Long-term record of global distribution of ozone during 1979 to 2001, from Total Ozone Mapping Spectrometer (TOMS), over a tropical urban environment has been analyzed and compared with ground measurements. Increase in atmospheric UV-absorbing aerosol loading has been observed after 1991. TOMS columnar ozone during 1979 to 2001 suggested a clear Gaussian pattern of minimum concentration in winter months and maximum in summer months. TOMS ozone showed good correlation with the ground measured columnar ozone during winter months and negative correlation with Sunburning Ultraviolet (SUV) (280–370 nm), UVA and aerosol optical depth (AOD).     

IPCC第二次气候变化科学评估报告的主要科学成果和问题

介绍了政府间气候变化委员会(IPCC)最近出版的第二次气候变化科学评估报告中的主要科学成果,并说明了今后3～4年中IPCC从科学上主要关注的问题。     

Lidar Measurements of Aerosols in the Tropical Atmosphere

Measurements of atmospheric aerosols and trace gases using the Laser radar (lidar) techniques, have been in pro-gress since 1985 at the Indian Institute of Tropical Meteorology, Pune (18o32’N, 73o51’E, 559 m AMSL), India. These observations carried out during nighttime in the lower atmosphere (up to 5.5 km AGL), employing an Argon ion / Helium-Neon lidar provided information on the nature, size, concentration and other characteristics of the constituents present in the tropical atmosphere. The time-height variations in aerosol concentration and associated layer structure exhibit marked differences between the post-sunset and pre-sunrise periods besides their seasonal va-riation with maximum concentration during pre-monsoon / winter and minimum concentration during monsoon months. These observations also revealed the influence of the terrain of the experimental site and some selected me-teorological parameters on the aerosol vertical distributions. The special observations of aerosol vertical profiles ob-tained in the nighttime atmospheric boundary layer during October 1986 through September 1989 showed that the most probable occurrence of mixing depth lies between 450 and 550 m, and the multiple stably stratified aerosol lay-ers present above the mixing depth with maximum frequency of occurrence at around 750 m. This information on nighttime mixing depth / stable layer derived from lidar aerosol observations showed good agreement with the height of the ground-based shear layer / elevated layer observed by the simultaneously operated sodar at the lidar site.     

NUMERICAL SIMULATIONS OF THE EFFECTS OF AEROSOLS IN THE ATMOSPHERIC BOUNDARY LAYER ON THE CLIMATE*

The climatic effects of the atmospheric boundary aerosols are studied by the use of a three-dimensional climate model.Simulated results show that the climate states both at the surface and in the atmosphere change remarkably when the aerosols with different optical thicknesses and properties are introduced into the atmospheric boundary layer of the model.The aerosols absorb and scatter the solar shortwave radiation,therefore,they reduce the solar energy reaching the ground surface and decrease the surface and the soil temperatures.The temperature in the boundary layer increase because of the supplementary absorption of radiation by the boundary aerosols.In the atmosphere,the temperatures at all isobaric surfaces rise up except for the 100 hPa level.The atmospheric temperatures below the 500 hPa level are directly influenced by the boundary aerosols,while the atmospheric temperatures above the 500 hPa level are influenced by the heating due to convective condensation and the changes in the vertical motion field.Cyclonic differential circulations appear over the desert areas at the low levels,and anticyclonic differential circulations exist at the upper levels in the horizontal flow fields.The vertical motions change in correspondence with the differential circulations.The changes in precipitation are directly related to that of vertical motions.The mechanisms of climate effects of the boundary aerosols are also discussed in this paper.     

Formation and chemical composition of atmospheric aerosols in an equatorial forest area

The physical properties and the chemical composition of atmospheric aerosols have been studied in an equatorial region in the southern Congo (Africa). Field experiments were conducted between 1978 and 1983 in the equatorial forest of the Mayombe during periods where the influence of biomass burning was minimum. The results indicate that the forest is a net source of both fine particles resulting primarily from gas-to-particle conversion and coarse particles produced by mechanical processes. Carbonaceous matter is the major component of these biogenic particles but the forest is also a significant source of sulfate, nitrate, ammonium and potassium. Half of this carbon is attached to submicron particles and likely derives from organic gaseous precursors naturally emitted by the local biosphere.Presented at the international Symposium Influence of marine and terrestrial biosphere on the chemical composition of the atmosphere, held in Mainz, F.R.G., on 16–22 March 1986.     

Source terms and source strengths of the carbonaceous aerosol in the tropics

Atmospheric aerosol samples were collected in the Ivory Coast, primarily at Lamto (6°N, 5°W) between 1979 and 1981. The samples were analysed for total particulate carbon concentration and isotopic composition (¹³C/¹²C) by mass spectrometry. Observed concentrations were found high compared to values reported for temperate regions. Fine particulate carbon in the submicrometersize range accounted for 50 to 80% of the reported concentrations. At Lamto, both particulate carbon concentrations and isotopic ratios exhibit a large temporal variability which is shown to reflect the diversity of sources and their seasonal evolution. Natural emissions from the equatorial forest during the wet season, and biomass burning during the dry season, appear to be the major sources. The latter, though active during only a third of the year, is, on an annual basis, the most important source. Based on the data obtained at Lamto, an attempt has been made to estimate the flux of fine particulate carbon emitted from the tropical regions into the global troposphere. This flux, which is of the order of 20×10¹² g C/yr, appears to be equivalent to the flux of fine particulate carbon emitted from industrial sources. These results suggest that the tropospheric burden of fine particulate carbon in lowlatitude regions is dominated by the long-range transport of carbonaceous aerosols originating from the Tropics.     

The role of gravitophotophoresis for stratospheric and mesospheric particulates

Gravitophotophoresis, a type of photophoresis related to the direction of gravity, is examined in view of its possible importance to some aerosols in stratosphere and mesosphere. particles of various materials from about 1 to 100 m in size show levitation by photophoretic forces under laboratory simulation of irradiation by the sun at air densities of the middle atmosphere. Minimum air densities for levitation are about 2–3 g m^–3 with mineral and metallic powders, about 0.08 g m^–3 with carbonaceous powders. The fraction of rising particles can be about 0.01 to 1%. Velocities of ascent are in the range of 0.001 to 0.01 m s^–1 at a pressure of several mbar. The magnitude and the mechanical character of the force of gravitophotophoresis can be explained if it is identified with a radiometer force caused by a difference of the accommodation coefficient on the surface. It is suggested that gravitophotophoresis can be important to the residence time and the maximum altitude of carbonaceous and mineral particles, such as volcanic ash or products of meteorite impact, and to the presence of microorgnisms in the middle atmosphere.     

Organic matter of the troposphere — V: Application of molecular marker analysis to biogenic emissions into the troposphere for source reconciliations

Organic matter in tropospheric aerosols is derived from two major sources and is admixed depending on the geographic area. These sources are biogenic detritus and anthropogenic emissions. The biogenic materials in the solvent-extractable organic matter are comprised predominantly of higher plant waxes, with lesser amounts of resin and microbial detritus and the anthropogenic components are primarily vehicular emissions (e.g. oils, soot, etc.) and input from combustion (e.g. charcoal, thermally-altered biogenic matter, etc.). Both biogenic detritus and anthropogenic emissions contain organic compounds (C₁₂–C₄₀₊), which can be identified with unique and distinguishable distribution patterns. Molecular composition analysis has been applied to such extracts after suitable chemical separation into subfractions (i.e. hydrocarbons, ketones, aldehydes, carboxylic acids, alcohols, and wax esters). Both homologous compound series and specific natural products (e.g. phytosterols, terpenes, etc.) are identified as molecular markers.Aerosols from rural and remote areas in the western United States, South America, Nigeria and Australia have been analyzed and all contained predominantly plant waxes. The loadings of hydrocarbons ranged approximately from 10–1400 ng/m³ of air, of fatty acids from 10–450 ng/m³ and of fatty alcohols from 10–1650 ng/m³. These higher molecular weight lipids primarily from flora comprise a major component of the organic carbon in rural and remote aerosols. They are thus important indicators for regional biogenic sources in the global cycling of organic carbon.Presented in part at the International Symposium on Biosphere-Atmosphere Exchange, Mainz, E.R. Germany, March 16–22, 1986, for Part IV see Simoneit et al. (1988) Atmos. Environ. 22, 983–1004.     

Water-Soluble dicarboxylic acids, ketoacids and dicarbonyls in the atmospheric aerosols over the southern ocean and western pacific ocean

Water-soluble dicarboxylic acids (DCAs), ketoacids, and α-dicarbonyls in the marine aerosol samples collected over the Southern Ocean and western Pacific Ocean were determined. Oxalic acid was the most abundant species, followed by malonic acid and then succinic acid. It is suggested that aerosol concentrations of the organics over the Southern Ocean in this work represent their global background levels. Over the Southern Ocean, total concentrations of DCAs ranged from 2.9 to 7.2 ng m⁻³ (average: 4.5 ng m⁻³), ketoacids from 0.14 to 0.40 ng m⁻³ (av.: 0.28 ng m⁻³), and dicarbonyls from 0.06 to 0.29 ng m⁻³ (av.: 0.11 ng m⁻³). Over the western Pacific, total concentrations of DCAs ranged from 1.7 to 170 ng m⁻³ (av.: 60 ng m⁻³), ketoacids from 0.08 to 5.3 ng m⁻³ (av.: 1.8 ng m⁻³), and dicarbonyls from 0.03 to 4.6 ng m⁻³ (av.: 0.95 ng m⁻³). DCAs over the western Pacific have constituted a large fraction of organic aerosols with a mean DCAs-C/TC (total carbon) of 7.0% (range: 0.59–14%). Such a high value was in contrast to the low DCAs-C/TC (av.: 1.8%; range: 0.89–4.0%) for the Southern Ocean aerosols. Based on the relative abundances and latitudinal distributions of these organics, we propose that long-range atmospheric transport is more important over the western Pacific Ocean, in contrast, in situ photochemical production is more significant over the Southern Ocean although absolute concentrations of the organics are much lower.     

A method for determining thermophysical properties of organic material in aqueous solutions: Succinic acid

A method for determining evaporation rates and thermodynamic properties of aqueous solution droplets is introduced. The method combines evaporation rate measurements using modified TDMA technique with data evaluation using an accurate evaporation model. The first set of data has been collected and evaluated for succinic acid aqueous solution droplets.Evaporation rates of succinic acid solution droplets have been measured using a TDMA system at controlled relative humidity (65%) and temperature (298 K). A temperature-dependent expression for the saturation vapour pressure of pure liquid phase succinic acid at atmospheric temperatures has been derived by analysing the evaporation rate data with a numerical model. The obtained saturation vapour pressure of liquid phase succinic acid is ln(p) = 118.41 − 16204.8/T − 12.452ln(T). The vapour pressure is in unit of Pascal and the temperature in Kelvin. A linear expression for the enthalpy of vaporization for liquid state succinic acid is also presented.According to the results presented in the following, a literature expression for the vapour pressure of liquid phase succinic acid defined for temperatures higher than 461 K [Yaws, C.L., 2003. Yaws' Handbook of Thermodynamic and Physical Properties of Chemical Compounds, Knovel] can be extrapolated to atmospheric temperatures with very good accuracy. The results also suggest that at 298 K the mass accommodation coefficient of succinic acid is unity or very close to unity.