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1.
Terry Deshler   《Atmospheric Research》2008,90(2-4):223-ICNAA07
Stratospheric aerosol, noted after large volcanic eruptions since at least the late 1800s, were first measured in the late 1950s, with the modern continuous record beginning in the 1970s. Stratospheric aerosol, both volcanic and non-volcanic are sulfuric acid droplets with radii (concentrations) on the order of 0.1–0.5 µm (0.5–0.005 cm− 3), increasing by factors of 2–4 (10–103) after large volcanic eruptions. The source of the sulfur for the aerosol is either through direct injection from sulfur-rich volcanic eruptions, or from tropical injection of tropospheric air containing OCS, SO2, and sulfate particles. The life cycle of non-volcanic stratospheric aerosol, consisting of photo-dissociation and oxidation of sulfur source gases, nucleation/condensation in the tropics, transport pole-ward and downward in the global planetary wave driven tropical pump, leads to a quasi steady state relative maximum in particle number concentration at around 20 km in the mid latitudes. Stratospheric aerosol have significant impacts on the Earth's radiation balance for several years following volcanic eruptions. Away from large eruptions, the direct radiation impact is small and well characterized; however, these particles also may play a role in the nucleation of near tropopause cirrus, and thus indirectly affect radiation. Stratospheric aerosol play a larger role in the chemical, particularly ozone, balance of the stratosphere. In the mid latitudes they interact with both nitrous oxides and chlorine reservoirs, thus indirectly affecting ozone. In the polar regions they provide condensation sites for polar stratospheric clouds which then provide the surfaces necessary to convert inactive to active chlorine leading to polar ozone loss. Until the mid 1990s the modern record has been dominated by three large sulfur-rich eruptions: Fuego (1974), El Chichón (1982) and Pinatubo (1991), thus definitive conclusions concerning the trend of non-volcanic stratospheric aerosol could only recently be made. Although anthropogenic emissions of SO2 have changed somewhat over the past 30 years, the measurements during volcanically quiescent periods indicate no long term trend in non-volcanic stratospheric aerosol.  相似文献   

2.
In the winter of 1994/95 the TRANSALL research aircraft performed several flights in the region of the Arctic vortex during the period of low stratospheric temperatures. The results of simultaneous measurements of HNO3 column amounts by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) and of aerosol backscatter profiles by the Ozone Lidar EXperiment (OLEX) are presented for two typical flight scenarios across the polar vortex boundary on December 17, 1994 and January 11/12, 1995. On December 17 and January 12, the column amounts of gaseous HNO3 decreased significantly in regions with low stratospheric temperatures. This decrease was correlated with the extent of the polar stratospheric clouds. Depolarisation measurements showed that type Ib PSCs were observed primarily, but equilibrium calculations for H2SO4/HNO3/H2O aerosols seem to underestimate the observed HNO3 sequestering.  相似文献   

3.
The first direct in situ measurements of the sulfuric acid contained in stratospheric aerosol particles were made using a novel balloon-based Ion Molecule Reaction Mass Spectrometer instrument (IMRMS) equipped with an aerosol vaporizer. The IMRMS method employed offers direct aerosol sulfuric acid measurements with high spatial resolution. The balloon flight took place on 23 October 1995 in middle latitudes (44°N) and reached a maximum altitude of 24 km. Measured molecular number densities of aerosol sulfuric acid decreased with increasing altitude from about 2.9 × 109 cm-3 at 15km altitude to about 2.4 × 108 cm-3 at 21 km. Corresponding mass mixing ratios are 2.5 and 0.6 ppbm, respectively. Calculated sulfuric acid mixing ratios from aerosol volumes inferred from aerosol size distribution measurements on the same balloon agree well with the IMRMS data using standard assumption aerosol composition.  相似文献   

4.
During a series of flights in the winters 1991/92 to 1994/95 total stratospheric NO2 was measured by means of the DOAS (Differential Optical Absorption Spectroscopy) technique on board a C160 (Transall) aircraft. In an area covering 60°W to 60°E, and 16°N to 86°N, the total stratospheric NO2 was observed to vary markedly with latitude and season (winter and spring). In the mid-winter Arctic vortex extremely low total stratospheric NO2 (< 3.1014/cm2) was always found, generally larger amounts of NO2 occurred outside the vortex in winter and towards the spring both inside and outside the vortex. This behaviour of stratospheric NO2 can be explained by the denoxification of the wintertime polar stratosphere. Ambient to the vortex in mid-winter however, sudden increases of total stratospheric NO2 by about a factor of 3 were observed. These sudden increases in stratospheric NO2 coincide with a change in the wavenumber 2 of the geopotential height at 60°N, which indicates that most likely the events are caused by planetary waves efficiently transporting air masses rich in NOx from lower to higher latitudes. The monitoring of stratospheric NO2, during latitudinal traverses ranging from the Arctic (80°N) to the Subtropics (18°N) in spring also unexpectedly showed a large variability in total stratospheric NO2 at mid-latitudes. Since photochemistry almost certainly can be excluded, it is proposed that the observed variability may be due to the planetary wave activity of the stratospheric surf zone, known to dynamically connect the tropical and the polar stratosphere.  相似文献   

5.
Zenith sky observations of O3, NO2, OClO and BrO are reported, which were performed at Kiruna (67.9°N, 21.1°E) within the SESAME winters 1993/1994 and 1994/95. For both winters large total amounts of OClO were observed inside the polar vortex at twilight, indicating the degree and the temporal variation of the halogen activation of the polar stratosphere. Occasionally OClO could also be observed outside the polar vortex, most likely due to export of halogen activated vortex air masses into the ambient stratosphere. BrO could also be detected in winter 1994/95, with the largest slant column amounts (5·1014/cm2) occuring in the polar vortex in mid-winter. Similar abundances of stratospheric BrO were observed at dusk and dawn, for both, air masses inside and outside the vortex. This observation is in reasonable agreement with previous studies on stratospheric BrO (observations and models) of Wahner et al. (1992), Arpag et al. (1994), Krug et al. (1996), and Lary et al. (1996a,b), but partly in disagreement with those of Solomon et al. (1989), Fish et al. (1995), and Sessler et al. (1996).  相似文献   

6.
Vertical column abundances of HCl, ClONO2, HF and HNO3 have been obtained from infrared solar absorption measurements made at Aberdeen, UK (57°N, 2°W) during the periods January 13 1994 - May 8 1994 and November 23 1994 - April 19 1995. The measurements reveal the partitioning of inorganic chlorine (Cly) inside and outside the polar vortex during these two winter and spring periods. Stratospheric temperatures within the northern polar vortex during 1993/94 were not cold throughout January and most of February. The measurements reported here suggest that following a brief period of chlorine activation in late February and early March, the active chlorine within the vortex recovered rapidly to form ClONO2 resulting in in-vortex ClONO2 columns of 7 × 1015 molecules cm-2. In contrast, measurements during January 1995 suggest extensive invortex activation with in-vortex HCl + ClONO2 as low as 3.6×1015 molecules cm-2. High day-to-day variability in the ClONO2 columns observed during February is evidence for the transport of ClONO2 rich air from high to mid latitudes during the late winter. The implications for mid latitude O3 loss are discussed. A preliminary comparison of the HCl, ClONO2, and HNO3 column data from winter 94/95 with a three-dimensional chemical transport model shows that the model generally reproduces well the day-to-day variability and absolute magnitude of the observed columns, especially for HNO3 outside of the vortex.  相似文献   

7.
Cascade impactor samples were collected over the Alaskan Arctic during the first three research flights of AGASP-II. These samples were analyzed using analytical electron microscopy to determine the morphology, mineralogy and elemental composition of individual particles. For analytical considerations, a typical impactor sample was run for approximately 20 min, thus giving excellent time resolution of discrete events.Samples collected during flights 201 and 202 consisted of stratospheric aerosol and lower-altitude haze samples. Stratospheric samples were characterized by moderate loadings of H2SO4 droplets with relatively few particles of other types. Samples collected in tropospheric haze layers generally exhibited light-to-moderate particle loadings. H2SO4 was again the most prevalent species, with crustal and anthropogenic particles also observed. One sample taken over south-central Alaska near the end of flight 203 showed high concentrations of solid crustal particles, with relatively little associated H2SO4. Giant particles larger than 5 m were occasionally observed in this aerosol. The composition of this material closely matches that of bulk ash from the Mt. Augustine volcano, which erupted 9–13 days before collection of this sample. This brings forth the possibility that pockets of ash-rich aerosol existed over parts of south and central Alska during the AGASP-II field mission. There is no evidence that these volcanic aerosols were present in the AGASP study area north of the Brooks Range.  相似文献   

8.
In‐situ aerosol measurements were performed in the northern hemispheric stratosphere up to altitudes of 21 km between 13 November 1996 and 14 January 1997, inside and outside of the polar vortex during the Airborne Polar Experiment (APE) field campaign. These are measurements of particle size distributions with a laser optical particle counter of the FSSP‐300 type operated during 9 flights on the Russian M‐55 high‐altitude research aircraft Geophysika. For specific flights, the FSSP‐300 measurements are compared with balloon‐borne data (launched from Kiruna, Sweden). It was found that the stratospheric aerosol content reached levels well below the background concentrations measured by the NASA operated ER‐2 in 1988/89 in the northern hemisphere. During the APE campaign, no PSC particle formation was observed at flight altitudes although the temperatures were below the NAT condensation point during one flight. The measured correlations between ozone and aerosol give an indication of the subsidence inside the 1996/97 polar vortex. Despite the lower aerosol content in the winter 1996/97 compared to the 1989 background, the heterogeneous reactivity of the aerosol (as calculated from the measured data with additional model input) is comparable. This is due to the dependency of the reactive uptake coefficients on the atmospheric water vapor content. Under the described assumptions the reaction rates on the background aerosol are significantly smaller than for competing gas phase chlorine activation, as can be expected for stratospheric background conditions especially inside the polar vortex.  相似文献   

9.
The paper discusses the potential effects on the ozone layer of gases released by the engines of proposed high altitude supersonic aircraft. The major problem arises from the emissions of nitrogen oxides which have the potential to destroy significant quantities of ozone in the stratosphere. The magnitude of the perturbation is highly dependent on the cruise altitude of the aircraft. Furthermore, the depletion of ozone is substantially reduced when heterogeneous conversion of nitrogen oxides into nitric acid on sulfate aerosol particles is taken into account in the calculation. The sensitivity of the aerosol load on stratospheric ozone is investigated. First, the model indicates that the aerosol load induced by the SO2 released by aircraft is increased by about 10–20% above the background aerosols at mid-high latitude of the Northern Hemisphere at 15 km for the NASA emission scenario A (the NASA emission scenarios are explained in Tables I to III). This increase in aerosol has small effects on stratospheric ozone. Second, when the aerosol load is increased following a volcanic eruption similar to the eruption of El Chichon (Mexico, April 1982), the ozone column in spring increases by as much as 9% in response to the injection of NO x from the aircraft with the NASA emission scenario A. Finally, the modeled suggests that significant ozone depletion could result from the formation of additional polar stratospheric clouds produced by the injection of H2O and HNO3 by the aircraft engines.  相似文献   

10.
平流层气溶胶的辐射强迫及其气候响应的水平二维分析   总被引:7,自引:0,他引:7  
利用比较先进的辐射模式计算了平流层气溶胶的辐射强迫,并对之进行了参数化。结果发现平流层气溶胶的辐射强迫的水平分布不仅与其本身的水平变化有关,而且与下垫面的反照率有很大的关系。利用近期开发的二维能量平衡模式模拟了皮纳图博火山气溶胶对地面平衡温度的影响,结果表明:皮纳图博火山至喷发后1年半左右降温达最大,至喷发后第5年降温已很小。  相似文献   

11.
蔡宏珂  郭静超  周任君 《大气科学》2011,35(6):1159-1168
本文采用卤素掩星试验(Halogen Occultation Experiment,HALOE)资料探讨了火山活动相对平静期平流层气溶胶与O3、H2O、HC1、NOx、CH4、HF等微量气体以及温度的关系.滞后相关分析显示气溶胶与微量气体和温度有显著关系,不同成分的相关性特征有所差异,中低纬度上空70~20 hPa高度...  相似文献   

12.
Polar stratospheric clouds (PSC) were observed with the multi-wavelength lidar of the MOANA project (Modelling and Observations of Aerosols in the Northern Atmosphere) during SESAME (Second European Stratospheric Arctic and Mid-latitude Experiment). The physical state, liquid or solid, of the cloud particles can be inferred from the lidar data. Using isentropic back-trajectories to obtain the thermal history of the sampled air masses, it is possible to reconcile most of the observations with current ideas on PSC formation and evolution. When the cloud particles were identified as liquid, changes in the size distribution of the droplets along the trajectory were calculated using a micro-physical box model. Backscatter ratios calculated from the size distributions are in broad agreement with the lidar data, giving confidence in current understanding of the evolution of ternary solution (H2SO4, HNO3 and H2O) droplets.Results from two soundings are shown which bear on the problem of the formation of solid particles. In the first, solid particles were detected. The air mass had cooled to the frost point 12 hours earlier. In the second no solid particles were detected although the air temperature was below the nitric acid trihydrate existence point, and had decreased by 12K in the previous 14 hours.  相似文献   

13.
As a component of the Canadian Arctic Haze Study, held coincident with the second Arctic Gas and Aerosol Sampling Program (AGASP II), vertical profiles of aerosol size distribution (0.17 m), light scattering parameters and cloud particle concentrations were obtained with an instrumented aircraft and ground-based lidar system during April 1986 at Alert. Northwest Territories. Average aerosol number concentrations range from about 200 cm–3 over the Arctic ice cap to about 100 cm–3 at 6 km. The aerosol size spectrum is virtually free of giant or coarse aerosol particles, and does not vary significantly with altitude. Most of the aerosol volume is concentrated in the 0.17–0.50 m size range, and the aerosol number concentration is found to be a good surrogate for the SO4 = concentration of the Arctic haze aerosol. Comparison of the aircraft and lidar data show that, when iced crystal scattering is excluded, the aerosol light scattering coefficient and the lidar backscattering coefficient are proportional to the Arctic haze aerosol concentration. Ratios of scattering to backscattering, scattering to aerosol number concentration, and backscattering to aerosol number concentration are 15.3 steradians, 1.1×10–13 m2, and 4.8×10–15 m2 sr–1, respectively. Aerosol scattering coefficients calculated from the measured size distributions using Mie scattering agree well with measured values. The calculations indicate the aerosol absorption optical depth over 6 km to range between 0.011 and 0.018. The presence of small numbers of ice crystals (10–20 crystals 1–1 measured) increased light scattering by over a factor of ten.  相似文献   

14.
The second Arctic Gas and Aerosol Sampling Program (AGASP-II) was conducted across the Alaskan and Canadian Arctic in April 1986, to study the in situ aerosol, and the chemical and optical properties of Arctic haze. The NOAA WP-3D aircraft, with special instrumentation added, made six flights during AGASP-II. Measurements of wind, pressure, temperature, ozone, water vapor, condensation nuclei (CN) concentration, and aerosol scattering extinction (bsp) were used to determine the location of significant haze layers. The measurements made on the first three flights, over the Arctic Ocean north of Barrow and over the Beaufort Sea north of Barter Island, Alaska are discussed in detail in this report of the first phase of AGASP II. In the Alaskan Arctic the WP-3D detected a large and persistent region of haze between 960 and 750 mb, in a thermally stable layer, on 2, 8, and 9 April 1986. At its most dense, the haze contained CN concentrations >10,000 cm–3 and bsp of 80×10–6 m–1 suggesting active SO2 to H2SO4 gas-to-particle conversion. Calculations based upon observed SO2 concentrations and ambient relative humidities suggest that 104–105 small H2SO4 droplets could have been produced in the haze layers. High concentrations of sub-micron H2SO4 droplets were collected in haze. Ozone concentrations were 5–10 ppb higher in the haze layers than in the surrounding troposphere. Outside the regions of haze, CN concentrations ranged from 100 to 400 cm–3 and bsp values were about (20–40)×10–6 m–1. Air mass trajectories were computed to depict the air flow upwind of regions in which haze was observed. In two cases the back trajectories and ground measurements suggested the source to be in central Europe.  相似文献   

15.
Use of an airborne quartz crystal microbalance cascade impactor instrument together with a correlation spectrometer has allowed the flux of particles and their size distribution to be determined at Mount Erebus. The plume contributes 21±3 metric tomnes/day of aerosol particles to the Antarctic upper troposphere. The aerosol particles consist of larger (5–25 m) particles of elemental sulfur and silica, a middle sized group of iron oxides and smaller particles (less than 1 m) of complex liquids. Unlike many volcanic plumes, the Erebus plume has only a small amount of sulfate particles. The concentrations of particles in the Erebus plumes was 70–370 m/m3. Limited sampling of the Antarctic atmosphere at 8 km altitude but hundreds of km away from Erebus obtained a few large particles of sulfur and silicates, suggesting a similarity with the Erebus plume. The fallout of these particles occurs slowly over a broad area of the Antarctic continent.  相似文献   

16.
Condensation nucleus (CN) concentrations have been measured at Mawson (67.6°S, 62.9°E) since mid 1981. Weekly median concentrations have an annual cycle with a maximum of around 300 to 400 cm-3 in summer and a minimum of a few tens of particles per cm-3 in winter. In this respect Mawson behaves very much like an Antarctic continental location. Preliminary measurements of the size distribution of CN particles taken over a nine month period suggest a seasonal change in typical particle radius from around 0.01 m in winter to around 0.04 m in summer. Diurnal variation in the CN concentration is generally very weak and does not show any systematic relation to the pronounced diurnal variation in wind-speed at Mawson.Department of Science, Antarctic Division  相似文献   

17.
利用2009年石家庄地区的4次机载PMS探测资料,对不同天气条件下大气气溶胶的数浓度、平均直径垂直分布和谱分布及一次晴天条件下的水平分布进行分析。结果表明:PCASP 探头探测的0.1-3.0 μm气溶胶粒子最大数浓度的量级为102-104 cm-3之间,平均值量级为102-103 cm-3之间,平均直径最大值介于0.225-0.717 μm,平均值介于0.148-0.167 μm。晴天条件下,气溶胶的数浓度随高度递减,直径随高度变化不大;逆温层底气溶胶明显积累,气溶胶浓度在大气边界层内明显高于其他层次;阴天轻雾情况下边界层内的气溶胶数浓度大于雨天和晴天,雨天气溶胶浓度最低;晴天气溶胶数浓度的水平分布不均匀;在云中气溶胶浓度明显下降,在云外气溶胶浓度较高。不同天气条件和晴天不同高度情况下,石家庄地区气溶胶谱型呈单峰分布,小于0.3 μm的细粒子对气溶胶的数浓度贡献最大,且随着高度的增加谱宽变窄。  相似文献   

18.
19.
A field study was conducted at a mountain-top site in northwestern Colorado. Supercooled cloud water, collected as a function of droplet size, was analyzed for anions, cations and trace elements. Enrichment factors (EF) of SO 4 2– , K+, Na+ and Cl relative to crustal and marine reference elements (Al and Na) were calculated to determine whether chemical fractionation of the aerosol occurs during cloud droplet formation. The largest EF's for all ions were found for droplets less than 10–15 µm diameter. Ratios of the small to large droplet mean EF's ranged from 1 to 2, for SO 4 2– relative to both Al and Na+, to 10 to 12 for Na+, Cl and K+, relative to Al. EF's of K+ and Cl in the bulk cloud water were in crustal and marine proportions, respectively. It was concluded that although bulk could chemistry may indicate a lack of enrichment of a species, this may not be true throughout the droplet size distribution. The higher enrichments in small droplets is likely a result of their formation on small aerosol particles whereas the large droplets form on the largest aerosol particles. This may suppress EF's in precipitation relative to the total aerosol.  相似文献   

20.
During a field measuring campaign at Kleiner Feldberg (Taunus) in 1990, microphysical characteristics of clouds have been measured by Forward Scattering Spectrometer Probes (FSSP). The aim was to study the influence of aerosol and meteorological factors on droplet size and number. The results are: More mass in the accumulation size range of the aerosol leads to more droplets in stratocumulus clouds and to higher soluble masses in droplets of stratus clouds. However, the aerosol distribution was coarser in the stratus clouds compared to the stratocumulus clouds. Within the first 200 m from cloud base, the droplets grow while their number decreases. The growth results in a stable size of about 14 µm diameter over a large distance from cloud base in many stratocumulus clouds. Two types of mixing processes were observed: processes with reductions in the number of droplets (inhomogeneous mixing) and with reductions in the size of the droplets (homogeneous mixing).  相似文献   

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