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1.
Arctic haze observed during polar flights from Anchorage, Alaska, to Thule, Greenland, and Thule to Bodo, Norway, during March 1983, was widespread over the entire Arctic region flown. The distribution of this haze exhibited strong horizontal and vertical variability resulting from the synopticmeteorological situations encountered: e.g. the presence of fronts and haze transport zones. Condensation nuclei concentrations of about 500 cm−3 and aerosol scattering extinction values of about 4 × 10−5m−1 were typical for Arctic haze layers. Intrusions of stratospheric air into the Arctic troposphere through tropopause folds were observed twice, suggesting that these events might occur quite frequently in the springtime Arctic atmosphere.  相似文献   

2.
Measurements are reported of the cloud condensation nucleus spectrum of Arctic haze from which it has been possible to deduce that a large fraction of the cloud active nuclei are soluble salts. On the basis of these findings, maximum supersaturation during the formation of Arctic stratiform clouds is expected to be around a third of a percent (for updrafts of 10 cm s−1). Soluble nuclei down to 3–4 × 10−6 radius would be nucleated under these conditions. These inferences suggest that clouds forming in polluted Arctic air may contain relatively small (i.e. 10–30 cm−3) cloud droplet concentrations.  相似文献   

3.
Number distribution data for 0.1–45 μm diameter aerosol were obtained using optical counting and sizing probes flown over the Alaskan Arctic during the second Arctic Gas and Aerosol Sampling Program (AGASP-II), flights 201–203. Due to noise present in the lowest size channels of the optical probes, estimates of the H2SO4 component of Arctic haze were not attempted. Large particle (> 0.5 μm diameter) results are presented here. Large particle number and volume concentration were determined along with estimated mass, which was generally </ 0.1μg m−3. Lognormal fitting to > 0.3 μg m−3 mass loading sizedistributed aerosol data produced a means for comparing volume geometric median diameters (VGMD) for these higher-mass time intervals. These VGMDs showed that solid crustal particles previously observed during AGASP-II had VGMDs in the 1.2–1.6 μm range and that the shape of these fitted lognormal distributions was essentially constant. This result suggests very-long-range transport from a distant crustal source and, in conjunction with aerosol physical and chemical characterization data, argues against the presence of the Mt. Augustine eruptive particles during AGASP-II Alaskan Arctic sampling.  相似文献   

4.
Ten aircraft-collected cascade impactor samples from the North American Arctic were analyzed using analytical electron microscopy. Morphological, mineralogical and elemental information were obtained from individual particles, as well as compositional data and size distribution estimates of the bulk aerosol. Categorization of carbonaceous material into organic-type and combustion-type carbon particles was performed in this study. This was accomplished through the use of a new ultra-thin window X-ray spectrometer, which can directly detect carbon X-rays emitted from particles, and through interpretation of morphological and electron diffraction data. Verification of graphite as a specific carbon mineral phase present in Arctic soot particles was performed in this manner.Several classes of particles were present in most of the aerosol samples and size fractions. These included liquid H2SO4 droplets, which were always present in the highest numbers, and crustal-type and composite SO4−2 particles. A small fraction (0–30%) of a random sampling of SO2−4particles from all impactor stages were found to contain detectable nitrogen, suggesting that partial neutralization by NH3 may have occurred in this minority of the SO2−4 droplets. Particles rich in non-combustion carbon and thought to be composed of organic material were also observed in most samples. Haze samples collected off the coast of Alert, NWT, show moderate loadings of H2SO4 droplets. Judging from these loadings and those from higher-altitude samples, ambient aerosol particle concentrations must have been considerably higher in the haze. The extent to which local activity at Alert has influenced these haze samples is not known, although a major contribution is not expected. Stratospheric samples did not contain several classes of particles thought to have major anthropogenic source inputs to the Arctic, such as black carbon and coal-fired combustion spheres. The lightest particle loadings in any samples were collected in the upper troposphere near the tropopause, where condensation nuclei counts during sampling fell to as low as 10 cm−3.  相似文献   

5.
Measurements of carbonaceous aerosol, aerosol light absorption and aerosol light scattering were made at two rural sites in southwestern Pennsylvania during August 1983. Aerosol light absorption ranged from 5.2 × 10−6 m−1 to 6.4 × 10−5 m−1 (average: 1.9 × 10−5 m−1) and accounted for about 13% of the aerosol total light extinction. Elemental carbon, averaging 1.3 μg m−3 at the two sites (and comprising some 36 % of the aerosol carbon), accounted for effectively all (> 95 %) of the aerosol light absorption.  相似文献   

6.
Atmospheric aerosols in subarctic central Alaska were studied for two winter seasons. Both optical absorptivity and excess (non-marine) sulfate undergo seasonal variation similar to that reported in Arctic locations (maximum in late spring and minimum in summer), but the magnitudes are a factor of two smaller than in the Arctic. The meridional variation in aerosol blackness and sulfur content (cleaner air to the south) is contrary to the trend in the Scandinavian Arctic and is interpreted to indicate the existence of pollution sources generally north and west, outside of Alaska's borders.Aerosol size varies with air temperature. Submicrometer aerosol mass and geometric mean diameter (GMD) increase as temperature decreases. Aerosols in all air masses studied were rich in volatile particles. The volatility suggests the presence of aqueous solutions of H2SO4. On the basis of (a) the relativity high aerosol volatility, and (b) the opposite trends between mean diameters and air temperature, it is conjectured that condensation of H2SO4 vapor may be an important mechanism for aerosol evolution in the winter (dark) polar troposphere.  相似文献   

7.
During autumn, 2006, variation in the frequency of aerosol nucleation events, as inferred from nanoparticle growth events, and associated hygroscopicity were investigated as a function of air mass transport history at a mixed deciduous forest in central Virginia, U.S. Above-canopy size distributions of aerosols between 0.012 and 0.700 μm diameter, size-resolved particle hygroscopicity at eight dry diameters between 0.012 and 0.400 μm, and cloud condensation nuclei (CCN) activity were characterized. Air mass back trajectories were clustered to identify source regions. Growth events were most frequent in fast-moving air masses (mean = 9 m s?1) that originated over the north central U.S. Under these flow regimes, mean values for preexisting sub-μm aerosol number concentrations (4700 cm?3), corresponding surface area (142 μm2 cm?3), air temperature (6.2 °C), and relative humidity (RH, 49.4%) were relatively low compared to other regimes. Under stagnant flow conditions (mean = 3 m s?1), mean number concentrations were higher (>6000 cm?3) and size fractions <0.1 μm diameter exhibited enhanced hygroscopicity compared to other source regions. These results indicate that precursors emitted into relatively clean, cold, and dry air transported over the southeastern U.S. reacted to form condensable intermediates that subsequently produced new aerosols via nucleation and growth. This pathway was an important source for CCN. During events in October, nanoparticles were produced in greater numbers and grew more rapidly compared to November and December.  相似文献   

8.
Aerosol data consisting of condensation nuclei (CN) counts, black carbon (BC) mass, aerosol light scattering (SC), and aerosol optical depth (AOD) measured at Barrow, Alaska from 1977 to 1994 have been analyzed by three-way positive matrix factorization (PMF3) by pooling all of the different data into one large three-way array. The PMF3 analysis identified four factors that indicate four different combinations of aerosol sources active throughout the year in Alaska. Two of the factors (F1, F2) represent Arctic haze. The first Arctic haze have factor F1 is dominant in January–February while the second factor F2 is dominant in March–April. They appear to be material that is generally ascribed to long-range transported anthropogenic particles. A lower ratio of condensation nuclei to scattering coefficient loadings is obtained for F2 indicating larger particles. Factor F3 is related to condensation nuclei. It has an annual cycle with two maxima, March and July–August indicating some involvement of marine biogenic sources. The fourth factor F4 represents the contribution to the stratospheric aerosol from the eruptions of El Chichon and Mt. Pinatubo. No significant long-term trend for F1 was detected while F2 shows a negative trend over the period from 1982 to 1994 but not over the whole measurement period. A positive trend of F3 over the whole period has been observed. This trend may be related to increased biogenic sulfur production caused by reductions in the sea-ice cover in the Arctic and/or an air temperature increase in the vicinity of Barrow. Potential source contribution function (PSCF) analysis showed that in winter and spring during 1989 to 1993 regions in Eurasia and North America are the sources of particles measured at barrow. In contrast to this, large areas in the North Pacific Ocean and the Arctic Ocean was contributed to observed high concentrations of CN in the summer season. Three-way positive matrix factorization was an effective method to extract time-series information contained in the measured quantities. PSCF was useful for the identification possible source areas and the potential pathways for the Barrow aerosol. The effects of long-distance transport, photochemical aerosol production, emissions from biogenic activities in the ocean, volcanic eruptions on the aerosol measurements made at Barrow were extracted using this combined methodology.  相似文献   

9.
A review of the physical characteristics of sulfur-containing aerosols, with respect to size distribution of the physical distributions, sulfur distributions, distribution modal characteristics, nuclei formation rates, aerosol growth characteristics, and in situ measurement, has been made.Physical size distributions can be characterized well by a trimodal model consisting of three additive lognormal distributions.When atmospheric physical aerosol size distributions are characterized by the trimodal model, the following typical modal parameters are observed:1. Nuclei mode – geometric mean size by volume, DGVn, from 0.015 to 0.04 μm. σgn=1.6, nucler mode volumes from 0.0005 over the remote oceans to 9 μm3 cm−3 on an urban freeway.2. Accumulation mode – geometric mean size by volume, DGVa, from 0.15 to 0.5 μm, σga=1.6–2.2 and mode volume concentrations from 1 for very clean marine or continental backgrounds to as high as 300 μm3 cm−3 under very polluted conditions in urban areas.3. Coarse particle mode – geometric mean size by volume, DGVc, from 5 to 30 μm, σgn=2–3, and mode volume concentrations from 2 to 1000 μm3 cm−3.It has also been concluded that the fine particles (Dp<2 μm) are essentially independent in formation, transformation and removal from the coarse particles (Dp>2 μm).Modal characterization of impactor-measured sulfate size distributions from the literature shows that the sulfate is nearly all in the accumulation mode and has the same size distribution as the physical accumulation mode distribution.Average sulfate aerodynamic geometric mean dia. was found to be 0.48±0.1 μm (0.37±0.1 μm vol. dia.) and σg=2.00±0.29. Concentrations range from a low of about 0.04 μg m−3 over the remote oceans to over 8 μg m−3 under polluted conditions over the continents.Review of the data on nucleation in smog chambers and in the atmosphere suggests that when SO2, is present, SO2-to-aerosol conversion dominates the Aitken nuclei count and, indirectly, through coagulation and condensation, the accumulation mode size and concentration. There are indications that nucleation is ubiquitous in the atmosphere, ranging from values as low as 2 cm−3 h−1 over the clean remote oceans to a high of 6×106 cm−3 h−1 in a power plant plume under sunny conditions.There is considerable theoretical and experimental evidence that even if most of the mass for the condensational growth of the accumulation mode comes from hydrocarbon conversion, sulfur conversion provides most of the nuclei.  相似文献   

10.
A detailed study of resuspension of 1.85 μm MMAD silica particles from five horizontal layers within a small scale spruce canopy was carried out in a wind tunnel in which saplings were exposed to a constant free stream wind speed of 5 m s−1. This provided quantitative estimates of the potential for a tree canopy contaminated with an aerosol deposit to provide (i) an airborne inhalation hazard within the forest environment and (ii) a secondary source of airborne contamination after an initial deposition event. Resuspension occurred with a flux of 1.05×10−7 g m−2 s−1 from spruce saplings initially contaminated at a level of 4.1×10−2 g m−2. An average resuspension rate (Λ) of 4.88×10−7 s−1 was obtained for the canopy as a whole. Values of Λ were significantly different (ANOVA, p<0.001) between canopy layers and Λ was markedly greater at the top of the canopy than lower down although there was a slight increase in Λ at the base of the canopy. The resuspended silica particles deposited onto the soil surface at an average rate of about 5.3×10−8 μg cm−2 s−1. It is concluded that resuspension under wind velocities similar to that used in the reported experiments is likely to pose a relatively small inhalation hazard to humans and a relatively minor source of secondary contamination of adjacent areas. Furthermore, resuspension rates are likely to diminish rapidly with time. The results are discussed in relation to the growing interest in the tree planting schemes in urban areas to reduce the impacts of air pollution.  相似文献   

11.
The aim of this work is to quantify the sensitivity of shortwave radiative fluxes to changes in the vertical distribution of aerosol absorption, taken into account through the aerosol Single Scattering Albedo (SSA). The case study represents a real atmospheric situation with a desert dust layer (DDL) in the mid troposphere over an urban Boundary Layer (BL) observed at Rome on 20 June 2007. A moderately high aerosol optical depth (AOD), 0.292 at 550 nm, and low Ångström exponent of 0.30 were measured. The observed case was reconstructed with a radiative transfer model, in which the SSA of the boundary layer aerosols was varied from that of a highly absorbing aerosol type (urban) to a highly scattering one (clear marine). The SSA of the DDL is determined keeping fixed the measured SSA of the whole atmospheric column. The simulations show notable changes in the surface and top of the atmosphere (TOA) diffuse fluxes depending on the boundary layer aerosol properties. The aerosol radiative forcing (ARF) at the surface changes by 6–19 W m?2, depending on the solar zenith angle, when urban or clean marine particles are included in the boundary layer. The ARF differences observed at TOA are between 1 and 5 W m?2 when urban and clean marine aerosol types in the BL are respectively used, showing a smaller dependency on the solar zenith angle than at the surface.  相似文献   

12.
Airborne particles of diameter > 0.4 μm reaching Dye 3, Greenland during April–May 1983 were highly variable in size and concentration from day to day. Five-day backward air mass trajectories suggest the importance of long-range transport from more northerly latitudes on days with high concentrations; particle sizes were larger on these days. Lower concentrations and smaller particle sizes were associated with transport from the south. It is inferred that Dye 3 may receive material emitted from Eurasian sources and transported over the Pole, similar to inferences for more northern Arctic sites.Elemental analysis of individual particles showed an abundance of crustal material, with many particles also containing sulfur. Bulk chemical analyses of airborne particles and fresh snow, collected during three snowstorms where ice nucleation dominated, provided data which were used to estimate mass-basis scavenging ratios. Average scavenging ratios were in the range ~1000–2000 for the crustal elements Al, Fe, K, Mg, Mn, and Na. Similar values were observed for Cd, Cu and NO3. The corresponding ratios for Pb and SO42− averaged less than 200. These ratios were used with precipitation rate data to estimate wet deposition velocities in the order of ~2 cm s−1 for the first nine species, and ~0.2 cm s−1 for Pb and SO42−. Comparing fresh and older surface snow concentrations gave an average dry deposition velocity of roughly 0.2 cm s−1 for the crustal elements, with the small fraction of large particles (~5–10 μm) dominating deposition; much smaller values were associated with the remaining species. When used with other data in the literature, the results of this study suggest that total deposition velocities of Pb and SO42− may be as small as 0.05 cm s−1 in relatively dry regions of the Arctic.  相似文献   

13.
From December to April, the Arctic air mass is polluted by man-made mid-latitudinal emissions from fossil fuel combustion, smelting and industrial processes. In the rest of the year, pollution levels are much lower. This is the outcome of less efficient pollutant removal processes and better south (S) to north (N) transport during winter. In winter, the Arctic air mass covers much of Eurasia and N. America. Meteorological flow fields and the distribution of anthropogenic SO2 emissions in the northern hemisphere favor northern Eurasia as the main source of visibility reducing haze. Observations of SO42− concentrations in the atmosphere throughout the Arctic yield, depending on location and year, a January–April mean of 1.5–3.9 μg m−3 in the Norwegian Arctic to 1.2–2.2 μg m−3 in the N. American Arctic. An estimate of the mean vertical profile of fine particle aerosol mass during March and April shows that, on average, pollution is concentrated in the lower 5 km of the atmosphere. Not only are anthropogenic particles present in the Arctic atmosphere but also gases such as SO2, perfluorocarbons and pesticides. The acidic nature and seasonal variation of Arctic pollution is reflected in precipitation, the snowpack and glacier snow in the Arctic. A pH of 4.9–5.2 in winter and ~ 5.6 in summer is expected in the absence of calcareous wind blown soil. Glacial records indicate that Arctic air pollution has undergone a marked increase since the mid 1950s paralleling a marked increase in SO2 and NOx emissions in Europe. Effects of Arctic pollution include a reduction in visibility and perturbation of the solar radiation budget in April–June. Potential effects are the acidification and toxification of sensitive ecosystems.  相似文献   

14.
The effect of black carbon (BC) on climate forcing is potentially important, but its estimates have large uncertainties due to a lack of sufficient observational data. The BC mass concentration in the southeastern US was measured at a regionally representative site, Mount Gibbes (35.78°N, 82.29°W, 2006 m MSL). The air mass origin was determined using 48-h back trajectories obtained from the hybrid single-particle Lagrangian integrated trajectory model. The highest average concentration is seen in polluted continental air masses and the lowest in marine air masses. During the winter, the overall average BC value was 74.1 ng m−3, whereas the overall summer mean BC value is higher by a factor of 3. The main reason for the seasonal difference may be enhanced thermal convection during summer, which increases transport of air pollutants from the planetary boundary layer of the surrounding urban area to this rural site. In the spring of 1998, abnormally high BC concentrations from the continental sector were measured. These concentrations were originating from a biomass burning plume in Mexico. This was confirmed by the observations of the Earth probe total ozone mapping spectrometer. The BC average concentrations of air masses transported from the polluted continental sector during summer are low on Sunday to Tuesday with a minimum value of 256 ng m−3 occurring on Monday, and high on Wednesday to Friday with a maximum value of 379 ng m−3 occurring on Friday. The net aerosol radiative forcing (scattering effects plus absorption effects) per unit vertical depth at 2006 m MSL is calculated to be −1.38×10−3 W m−3 for the southeastern US. The magnitude of direct radiative forcing by aerosol scattering is reduced by 15±7% due to the BC absorption.  相似文献   

15.
In an effort to reduce uncertainties in the quantification of aerosol direct radiative forcing (ADRF) in the southeastern United States (US), a field column experiment was conducted to measure aerosol radiative properties and effects at Mt. Mitchell, North Carolina, and at an adjacent valley site. The experimental period was from June 1995 to mid-December 1995. The aerosol optical properties (single scattering albedo and asymmetry factor) needed to compute ADRF were obtained on the basis of a procedure involving a Mie code and a radiative transfer code in conjunction with the retrieved aerosol size distribution, aerosol optical depth, and diffuse-to-direct solar irradiance ratio. The regional values of ADRF at the surface and top of atmosphere (TOA), and atmospheric aerosol absorption are derived using the obtained aerosol optical properties as inputs to the column radiation model (CRM) of the community climate model (CCM3). The cloud-free instantaneous TOA ADRFs for highly polluted (HP), marine (M) and continental (C) air masses range from 20.3 to −24.8, 1.3 to −10.4, and 1.9 to −13.4 W m−2, respectively. The mean cloud-free 24-h ADRFs at the TOA (at the surface) for HP, M, and C air masses are estimated to be −8±4 (−33±16), −7±4 (−13±8), and −0.14±0.05 (−8±3) W m−2, respectively. On the assumption that the fractional coverage of clouds is 0.61, the annual mean ADRFs at the TOA and the surface are −2±1, and −7±2 W m−2, respectively. This also implies that aerosols currently heat the atmosphere over the southeastern US by 5±3 W m−2 on annual timescales due to the aerosol absorption in the troposphere.  相似文献   

16.
Size distribution of particle number concentrations in the geometric equivalent diameter range 0.01–2.5 μm were determined in three communities, Zerbst, Bitterfeld and Hettstedt of the state of Sachsen-Anhalt in Eastern Germany, in the first half of 1993 and 1999. A Mobile Aerosol Spectrometer (MAS) consisting of a differential mobility particle spectrometer (DMPS) and a laser aerosol spectrometer (LAS-X) were used for size-selective particle number concentration measurements from which mass concentrations were derived based on an apparent mean density of the ambient aerosol of the closely situated city of Erfurt.The total number concentration was governed by ultra-fine particles (<0.1 μm) (81% in 1993 and 90% in 1999) and 0.1–0.5 μm size fraction dominates total mass concentration (approximately 80%). While the mass concentration of fine particles (PM2.5) decreased from 39 to 19 μg m−3, the geometric means of total number concentration showed constant concentration (13.3×103 cm−3 in 1993 and 13.3×103 cm−3 in 1999, p=0.975) and the geometric means of number concentration of ultra-fine particles (UP) between 10 and 30 nm increased from 5.9×103 to 8.2×103 cm−3 from 1993 to 1999 (p=0.016). The temporal changes of number and mass concentrations in the three communities are similar. The clear shift to smaller particle sizes within this six years period was caused by changes of the most prominent sources, traffic and domestic heating, since formerly dominating industries in Bitterfeld and Hettstedt had vanished grossly.  相似文献   

17.
Experiments were performed to compare the capability of u.v. light, γ-radiation and simultaneous u.v. and γ-radiation to produce aerosol particles in a mixture of SO2, NO2 and synthetic air at different humidities. In the presence of u.v. radiation, γ-radiation was found to enhance the particle production at dose rates as low as 10−4 μGy s−1 at 0% r.h., and 2 × 10−2 μGy s−1 at 75% r.h. γ-radiation alone did not produce aerosol particles at the same dose rates. The possible processes underlying this synergistic effect are discussed.  相似文献   

18.
Large quantities of atmospheric aerosols with compositions SO4 =, NO3 ? and NH4 + have been detected in highly industrialized areas. The major portions of aerosol products are the results of energyrelated fuel combustion. Both microphysical and macrophysical processes are considered in investigating the time dependent evolution of the saturation spectra of condensation nuclei associated with both polluted and clean atmospheres during the time periods of advection fog formation. The results show that the condensation nuclei associated with a polluted atmosphere provide more favorable conditions than condensation nuclei associated with a clean atmosphere to produce dense advection fog, and that attaining a certain degree of supersaturation is not necessarily required for the formation of advection fog with condensation nuclei associated with a polluted atmosphere for monodisperse distribution.  相似文献   

19.
The synoptic conditions over the Alaskan Arctic during the Arctic Gas and Aerosol Sampling Program (AGASP) of March 1983 are described. Air mass characteristics are pictured in terms of meteorological parameters, condensation nuclei, ozone and CO2 concentrations, aerosol size and number distributions, and aerosol scattering coefficients, as measured at the Barrow Geophysical Monitoring for Climatic Change (GMCC) baseline station and by aircraft Latitude-altitude cross sections of meteorological and aerosol parameters indicated both strong vertical and horizontal variability within the Arctic air mass. Aerosol concentrations aloft were usually higher than those measured at the ground and peak-to-peak variations are greater aloft than at the surface, showing that the stable Arctic boundary layer reduces mixing from aloft to the surface. Thus, surface measurements cannot be extrapolated to higher levels in a straightforward manner. Horizontal variability in the haze, as determined by the aircraft, was found to be abrupt and was not generally due to the presence of strong meteorological fronts. During 9–19 March 1983, at least four different air mass types were present in the Barrow region, each of which was characterized by distinct meteorological, aerosol and trace gas characteristics.  相似文献   

20.
In a pilot study the concentration levels of man-made mineral fibres in homes were investigated during a thermal insulation procedure in which glass or rock fibres were blown into the cavity wall. The concentration in the rooms during the insulation procedure varied between 5 × 10−3 and 25 × 10−3 lightmicroscopically detectable fibres cm−3, with peaks up to 65 × 10−3 fibres cm−3. The next day the concentration had been decreased to 10−3-10 × 10−3 fibres cm−3. The concentration of the electronmicroscopically detectable fibres during the insulation varied between 50 × 10−3 and 400 × 10−3 fibres cm−3. The next day the concentration in some houses was still above the level usually found in the ambient air in The Netherlands. It is likely that good ventilation during the next day would bring the indoor concentration to the outdoor level.  相似文献   

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