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1.
Electrical charges on aerosol particles and droplets modify the droplet–particle collision efficiencies involved in scavenging, and the droplet–droplet and particle–particle collision efficiencies involved in coalescence of droplets and particles, even in only weakly electrified clouds and aerosol layers. This work places electrically enhanced scavenging, and the electrical inhibition of scavenging in the context of the microphysics of weakly electrified clouds.Collision efficiencies are calculated by numerical integration to obtain particle trajectories, that are determined by the complex interplay of electrical, gravitational and phoretic forces together with inertia. These modify the trajectory of a particle as it is carried by flow around the falling droplet. Conversely, the flow around the particle also modifies the trajectory of the droplet. The flows are specified analytically, using a hybrid of the Proudman–Pearson stream function for that region close to the droplet or particle, where it is accurate, merging into the exact Oseen stream function for larger distances, where that becomes accurate. The effect of the flow around the particle on the motion of the droplet was simulated using Langmuir's superposition technique on the hybrid stream functions. The treatment of inertia in the present calculations allows an extension of the scope of our previous work by a factor of 10 larger in particle size (103 in mass). The coverage is extended to a wide range of atmospheric conditions and particle densities.The pressures and temperatures used in the models ranged from a representation of the lower troposphere at  1 km altitude (900 hPa, 10 °C) to that of the middle stratosphere at  30 km altitude (12 hPa, − 47 °C). The particles considered range from 0.1 μm to 10 μm radius; the droplet radii range from 4 μm to 50 μm; particle densities range from 300 kg m− 3 to 2500 kg m− 3; particle charges range from 2e to 100e with droplet charges of like sign of 100e; and relative humidities range from 10% to 100%.For the larger particles (radii greater than about 3 μm) interacting with the larger droplets (radii greater than about 15 μm) the effects of inertia increase with particle density and dominate at the larger densities. For particles with radii in the range 1–3 μm the ‘Greenfield Gap’ of very low collision efficiencies was found, and was determined to be due to the effects of the gravitational force causing a reduction of collisions of particles with the front of the droplet, and the effect of inertia overcoming the tendency for the weight to produce a collision in the slow velocity region in the rear. When the electrical or phoretic forces are sufficiently large the Greenfield Gap is closed.When the particles have radii < 3 μm inertial effects no longer dominate the collisions, although inertia modifies the weight effects for particles with radii down to about 0.5 μm. For charged aerosol particles with radii smaller than about 0.1 μm interacting with droplets or background aerosol particles smaller than a radius of about 15 μm, the long range electrical repulsive force is effective in opposing the phoretic forces and keeping the particle out of range of the short range attractive image force. Thus ‘electroscavenging’ gives way to ‘electroprotection’ against the scavenging or coagulation processes otherwise caused by Browninan diffusion or phoretic forces.In an atmosphere of temperature 10 °C and pressure 900 hPa the net phoretic force reduces to zero and becomes repulsive for particles with radii above about 2 μm (depending on particle conductivity). This enhances the development of the Greenfield Gap. However, the value of this radius (at which the net phoretic force is zero) increases strongly with decreasing temperature and pressure (increasing altitude) as expected from theory, and is about 5 μm in the middle troposphere and more than 10 μm in the stratosphere. Thus a net attractive phoretic force on particles extends into the 1–3 μm radius range in the upper troposphere; however, the weight and inertial effects can ensure the presence of the Greenfield Gap in that range for 2000 kg m− 3 particles up to the middle stratosphere.  相似文献   

2.
Airborne observations during August 1985 over Greenland and the North American Arctic revealed that dense, discrete haze layers were common above 850 mb. No such hazes were found near the surface in areas remote from local sources of particles. The haze layers aloft were characterized by large light-scattering coefficients due to dry particles (maximum value 1.24 × 10–4m–1) and relatively high total particle concentrations (maximum value 3100 cm–3). Sulfate was the dominant ionic component of the aerosol (0.06 – 1.9 g m–3); carbon soot was also present. Evidence for relatively fresh aerosols, accompanied by NO2 and O3 depletion, was found near, but not within, the haze layers. The hazes probably derived from anthropogenic sources and/or biomass burning at midlatitudes.It is hypothesized that the scavenging of particles by stratus clouds plays an important role in reducing the frequency and intensity of hazes at the surface in the Arctic in summer. Since the detection of haze layers aloft through measurements of column-integrated parameters from the surface (e.g., by lidar) cannot be carried out reliably when clouds are present, such measurements have likely underestimated the occurrence of haze layers in the Arctic, particularly in summer.  相似文献   

3.
Summary Using scattering coefficient profiles of the Pinatubo aerosols derived from the observation of skylight polarization and lidar backscattering ratio in Beijing, the radiative effect of Pinatubo aerosols in middle latitudes is assessed by a delta-four-stream radiative transfer model. It is shown that the Pinatubo aerosols significantly change the radiation field. Due to the presence of the volcanic aerosols, the downward short wave flux at the surface decreases with a maximum of 8 W/m2 while the upward short wave flux at the top of the atmosphere increases with a maximum of 6.5 W/m2. The volcanic aerosols are injected into the region bounded below by the tropopause and up by the 25 km level. The upward and downward radiative fluxes are changed in opposite directions at those two boundaries. Downward short wave fluxes below the tropopause are 7–9 W/m2 less than background values and downward long wave fluxes below the tropopause are 2 W/m2 more than background values. Upward short wave fluxes above 25 km level is 5–7 W/m2 more and upward fluxes above there are about 3 W/m2 less.The effects of the Pinatubo aerosols on heating rates are also significant. The maximum increase in the short wave heating rate can be as large as 0.2 K/day at 22 km. The increase in the long wave heating rate is less with a maximum amplitude of about 0.15 K/day. The maximum increase of the total heating rate is about 0.35 K/day, which is comparable with the heating rate caused by the ozone 9.6 µm band in this region.Results of this study are compared with studies of Lacis et al. (1992) and Russell et al. (1993) as well as ERBE measurements. The results generally agree well. Causes for the differences are analyzed.Based on the numerical study, it is also found that the LOWTRAN fresh volcanic model is not representative for the Pinatubo aerosols.With 9 Figures  相似文献   

4.
Mass size distribution of the crustal elements (Al, Ca, Fe, Mg, Si, Ti), anthropogenic elements (Zn, Mn, Cr, Cu, K, P, Pb) and sea elements (Na, Cl) were obtained from measurements carried out with an inertial cascade impactor in Sfax. A fitting procedure by data inversion was applied to those data. This procedure yields accurate size distributions of aerosols in the diameter range 0.1–25 μm in two different sites. In a coastal industrial site, the mass distribution of the aerosol showed a bimodal structure; and in urban area, the lower particle mode cannot be observed. The elemental dry deposition flux was calculated as a function of particle size. The element flux size distribution increased rapidly with particle size. The modelling results indicate that the majority of the crustal and anthropogenic elements flux (>90%) was due to particles larger than 3 μm in diameter.  相似文献   

5.
The change of the chemical composition of the near-ground level atmospheric aerosol was studied during two summer episodes by a Lagrangian type of experimental approach. Bulk and single-particle chemical analyses of ions and elements in the particulate phase were deployed. N(-III) and N(V) components were also measured in the gas-phase. The measurements were completed by particle size distributions.Secondary inorganic aerosols (SIA) and fine particles of ≈0.2–0.4 μm size were still elevated 50 km downwind of the city. The direct comparison of transport over the city in contrast to transport over the surrounding areas showed that SIA was formed from emission from the city within less than 3 h. Relative increases, i.e., enrichment during transport were observed for primary and secondary aerosol components. The degree of mixing on the individual particle level increased significantly during transport in the area. In particular, newly emitted carbonaceous particles became internally mixed within hours with pre-existing sulphate particles. Mostly due to secondary aerosol formation the average particle size (mass median diameter) of major constituents of the aerosol was significantly decreased while being transported over 13 h. Given recent insights which link fine particles number and mass concentrations with health risks, the results suggest that rural populations in areas which frequently are located within an urban plume might run an elevated health risk relative to populations in areas not affected by urban plumes.  相似文献   

6.
Measurements of the small-, intermediate-, and large-ion concentrations and the air–earth current density along with simultaneous measurements of the concentration and size distribution of aerosol particles in the size ranges 4.4–163 nm and 0.5–20 μm diameter are reported for a drifting snow period after the occurrence of a blizzard at a coastal station, Maitri, Antarctica. Ion concentrations of all categories and the air–earth current simultaneously decrease by approximately an order of magnitude as the wind speed increases from 5 to 10 ms− 1. The rate of decrease is the highest for large ions, lowest for small ions and in-between the two for intermediate ions. Total aerosol number concentration decreases in the 4.4–163 nm size range but increases in the 0.5–20 μm size range with wind speed. The size distribution of the nanometer particles shows a dominant maximum at ~ 30 nm diameter throughout the period of observations and the height of the maximum decreases with wind speed. However, larger particles show a maximum at ~ 0.7 μm diameter but the height of the maximum increases with increasing wind speed. The results are explained in terms of scavenging of atmospheric ions and aerosols by the drifting snow particles.  相似文献   

7.
The diffusion aerosol spectrometer for the measurements of particle size spectra and concentration levels is described. It includes three principal parts: (i) a block of diffusion batteries for measuring the particles, whose size does not exceed 0.15 μm, (ii) the particle amplifier for growing the particles passing through the diffusion batteries up to optically distinguishable sizes and (iii) the laser aerosol spectrometer, which counts the amplified particles and may also serve for independent measurements of particle size spectra within submicron size range. The tandem including: diffusion batteries+laser aerosol spectrometer allows for detecting particles of radius >3 nm at maximal concentration up to 2×104 particles/cm3. The tandem is managed either by PC or manually. The instrument is designed for studying aerosols in the atmosphere and for ecological measurements.  相似文献   

8.
During three of the flights with the NOAA P3 Orion over the Arctic icecap in April 1986, the atmospheric concentration of PAN (peroxyacetyl nitrate) was measured. Due to major experimental problems, the uncertainty in the data is large (+/–50%), but, nevertheless, some important trends can be resolved. More than 600 (+/–300) ppt(v) of PAN was present in a moderately dense arctic haze layer, confirming conclusions reached from surface observations at Alert, N.W.T., Canada, that PAN is a major odd nitrogen species in Arctic polluted air masses. In relatively clean air off Barrow, Alaska, PAN levels were well below 100 (+/–50) ppt(v), increasing with altitude, in agreement with theoretical predictions concerning the occurrence of PAN in clean air. PAN mixing ratios in the upper troposphere or lower stratosphere were variable (from ca. 30 (+/–15) ppt(v) on April 13 up to 140 (+/–70) ppt(v) on April 8), suggesting involvement in the tropospheric-stratospheric exchange of odd nitrogen. To place the PAN data in a broader context, measurements of other NOy compounds as well as integrated SOx data are also reported.  相似文献   

9.
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.  相似文献   

10.
A closure study of sub-micrometer aerosol particle hygroscopic behaviour   总被引：2，自引：0，他引：2  
The hygroscopic properties of sub-micrometer aerosol particles were studied in connection with a ground-based cloud experiment at Great Dun Fell, in northern England in 1995. Hygroscopic diameter growth factors were measured with a Tandem Differential Mobility Analyser (TDMA) for dry particle diameters between 35 and 265 nm at one of the sites upwind of the orographic cloud. An external mixture consisting of three groups of particles, each with different hygroscopic properties, was observed. These particle groups were denoted less-hygroscopic, more-hygroscopic and sea spray particles and had average diameter growth factors of 1.11–1.15, 1.38–1.69 and 2.08–2.21 respectively when taken from a dry state to a relative humidity of 90%. Average growth factors increased with dry particle size. A bimodal hygroscopic behaviour was observed for 74–87% of the cases depending on particle size. Parallel measurements of dry sub-micrometer particle number size distributions were performed with a Differential Mobility Particle Sizer (DMPS). The inorganic ion aerosol composition was determined by means of ion chromatography analysis of samples collected with Berner-type low pressure cascade impactors at ambient conditions. The number of ions collected on each impactor stage was predicted from the size distribution and hygroscopic growth data by means of a model of hygroscopic behaviour assuming that only the inorganic substances interacted with the ambient water vapour. The predicted ion number concentration was compared with the actual number of all positive and negative ions collected on the various impactor stages. For the impactor stage which collected particles with aerodynamic diameters between 0.17–0.53 μm at ambient relative humidity, and for which all pertinent data was available for the hygroscopic closure study, the predicted ion concentrations agreed with the measured values within the combined measurement and model uncertainties for all cases but one. For this impactor sampling occasion, the predicted ion concentration was significantly higher than the measured. The air mass in which this sample was taken had undergone extensive photochemical activity which had probably produced hygroscopically active material other than inorganic ions, such as organic oxygenated substances.  相似文献   

11.
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   

12.
In this work, the charging state of atmospheric nanoparticles was estimated through simultaneous measurements of aerosol size distribution and air ions mobility distribution with the aim to elucidate the formation mechanisms of atmospheric aerosols. The measurements were performed as a part of the QUEST 2 campaign at a boreal forest station in Finland. The overlapping part of the measurement ranges of the particle size spectrometers and air ion mobility spectrometers in the mass diameter interval of 2.6–40 nm was used to assess the percentage of charged particles (charging probability). This parameter was obtained as the slope of the linear regression line on the scatterplot of the measured concentrations of total (neutral + charged) and charged particles for the same diameter interval. Charging probabilities as a function of particle diameter were calculated for different days and were compared with the steady state charging probabilities of the particles in the bipolar ion atmosphere. For the smallest particles detectable by the particle size spectrometers (2.6–5 nm), the high percentages of negatively charged particles were found during the nanometer particle concentration bursts. These values considerably exceeded the values for the steady charging state and it was concluded that negative cluster ions preferably act as condensation nuclei. This effect was found to be the highest in the case of comparatively weak nucleation bursts of nanoparticles, when the rate of the homogeneous nucleation and the concentration of freshly nucleated particles were low. The nucleation burst days were classified according to the concentration of the generated smallest detectable new particles (weak and strong bursts). Approximately the same classification was obtained based on the charge asymmetry on particles with respect to the charge sign (polarity). The probabilities of negative and positive charge on the particles with the diameter of 5–20 nm were found to be nearly equal and they approximately agree with the values corresponding to the steady state charge distribution for negative particles known from lab experiments. It means that the steady charging state was reached during the growing time of particles up to 5 nm. The natural charging state of particles with a diameter between 2.5 and 4.5 nm was estimated by means of a special DMPS setup. Results were found to be in good correlation with the data by the particle size spectrometers and air ion mobility spectrometers.  相似文献   

13.
Large volcanic eruptions, in addition to the well-known effect of producing global cooling for a year or two, have been observed to produce shorterterm responses in the climate system involving non-linear dynamical processes. In this study, we use the ECHAM2 general circulation model forced with stratospheric aerosols to test some of these ideas. Run in a perpetual-January mode, with tropical stratospheric heating from the volcanic aerosols typical of the 1982 El Chichón eruption or the 1991 Pinatubo eruption, we find a dynamical response with an increased polar night jet in the Northern Hemisphere (NH) and stronger zonal winds which extend down into the troposphere. The Azores High shifts northward with increased tropospheric westerlies at 60°N and increased easterlies at 30°N. Surface temperatures are higher both in northern Eurasia and North America, in agreement with observations for the NH winters of 1982–83 and 1991–92 as well as the winters following the other 10 largest volcanic eruptions since 1883.This paper was presented at the Second International Conference on Modelling of Global Climate Variability, held in Hamburg 7–11 September 1992 under the auspices of the Max Planck Institute for Meteorology. Guest Editor for these papers is L. Dümenil  相似文献   

14.
The potential resources on the ion-stimulated syntheses effects of aerosol particles of lower troposphere in test sites in the arctic, mountain, arid and forest areas as the function of irradiation time and gas-precursor concentration were experimentally and theoretically evaluated. The dust-free outdoor air was irradiated with an ionization current of 10− 6 A by α-rays from isotope 239Pu. The total output of radiolytic aerosols (RA) with a diameter of 3–1000 nm was found to be 0.05–0.1 molecules per 1 eV of absorbed radiation, while the physical upper limit is 0.25–0.4 molecules/eV. In an interval of exposition time from 6 to 800 s (adsorbed energy is 3 · 1012–1014 eV/cm3) the RA mass concentration at different sites was increased from 1–10 to 50–500 μg/m3. According to the liquid chromatography data the major RA material is the H2O/HNO3 solution with acid concentration  25%. The used physical model presents new aerosols as a product from small and intermediate ion association through formation of neutral clusters and describes adequately some of the peculiarities in field experiment data. Introducing SO2, NH3, and also hydrochloric, nitric and sulphuric acid vapours with concentration 0.1–1 mg/m3 in the irradiated air stimulated an increase of mass aerosol concentration by a factor of 8–30. The mean size also decreased by a factor of 3–5. These facts allowed us to expect that the chemical composition of radiolytic aerosols generated in outdoor air would noticeably differ after addition of the gas-precursors.  相似文献   

15.
Thirty-six aerosol filter samples collected in tropospheric Arctic haze layers, in the stratosphere, and in the marine boundary layer during the 1983 Arctic Gas and Aerosol Sampling Program were analyzed for trace elements using instrumental neutron activation analysis. Average crustal dust concentrations were 540 ng/m3 and 330 ng/m3 for samples collected in Arctic haze over the North American and Norwegian Arctic, respectively. An average marine salt concentration of 120 ng/m3 was obtained for haze samples collected above the marine boundary layer on both sides of the Arctic.Meteorological and wind trajectory information were used to identify specific haze transport pathways, which brought relatively unmixed aerosol from the central Soviet Union into the AGASP sampling areas. Results from individual filters collected within these transport zones are discussed, with emphasis on certain trace metal ratos which have been proposed by other researchers as discriminators of aerosols from different source regions. Our aircraft-collected data are compared with previously-collected ground-based measurements, and show reasonably good agreement for most tracer elements and ratios. Specifically, we have determined the As/Sb ratio tracer, named by other researchers as the most effective elemental discriminator of aerosol from the central Soviet Union, to be approximately 5–6. This relatively high tracer value is consistent with previous ground-based findings. A significantly lower V/Sb ratio was observed throughout this study, possibly indicating a change in the source signature.  相似文献   

16.
Aerosol particles were collected on filters for studies of their ability to nucleate ice during the second Arctic Gas and Aerosol Sampling Program (AGASP-II) in April, 1986. The ice nuclei (IN) samples were collected from an aircraft at altitudes ranging from the surface to the vicinity of the tropopause in Arctic locations over Alaska, northern Canada and Greenland. Samples of other components of the aerosol were collected and measurements were made of other properties of the aerosol coincident in time with the IN samples. The IN filters were exposed to water saturation in a dynamic developing chamber at –15° C and –25° C. Ice crystals grew on the IN and were counted on the filters at discrete time intervals during the exposure period to determine the rate of ice nucleation and the final concentration of (IN). Results show that Arctic haze aerosol, identified by pollutant signatures, had lower IN concentrations, a lower IN to total aerosol fraction and slower ice nucleation rates than aerosol which had a chemical signature more indicative of the remote unpolluted troposphere. These observations suggest that the Arctic haze aerosol does not efficiently form ice in the arctic troposphere. This may be a factor contributing to the long-range transport of Arctic haze.  相似文献   

17.
During the second Arctic Gas and Aerosol Sampling Program conducted in April 1986, we performed measurements of the optically absorbing carbonaceous component of the ambient aerosol from the NOAA WP-3D aircraft operating between sea level and 10 km altitude. We collected the aerosol of filters that were exposed for several hours; we also operated the aethalometer to measure the concentration of aerosol black carbon in real time. The filter analyses represent averages over the altitude range and time span during which the filter was collecting. The real-time results were sorted by altitude to calculate vertical profiles of black carbon concentration. Values typically ranged from 300 to 500 ng m–3 at lower altitudes, decreasing gradually to 25 to 100 ng m–3 at 8–10 km. Strong stratification at lower altitudes was frequently observed. The magnitude of these concentrations suggests that the sources are distant regions of considerable fuel consumption. The presence of this material in the tropospheric column and its probable deposition to the high-albedo surface may result in perturbations of the solar radiation balance. The concentrations measured at the highest altitudes may mean that particulate carbon and accompanying emissions for which it is a tracer are mixing into the stratosphere.  相似文献   

18.
The climate changes that occured following the volcanic eruption of Mount Pinatubo in the Phillippines on 15 June 1991 have been simulated using the ARPEGE atmosphere general circulation model （AGCM）. The model was forced by a reconstructed spatial-time distribution of stratospheric aerosols intended for use in long climate simulations. Four statistical ensembles of the AGCM simulations with and without volcanic aerosols over a period of 5 years following the eruption have been made, and the calculated fields have been compared to available observations. The model is able to reproduce some of the observed features after the eruption, such as the winter warming pattern that was observed over the Northern Hemisphere （NH） during the following winters. This pattern was caused by an enhanced Equator-to-pole temperature gradient in the stratosphere that developed due to aerosol heating of the tropics. This in turn led to a strengthening of the polar vortex, which tends to modulate the planetary wave field in such a way that an anomalously positive Arctic Oscillation pattern is produced in the troposphere and at the surface, favouring warm conditions over the NH. During the summer, the model produced a more uniform cooling over the NH.  相似文献   

19.
Using the chemical composition of snow and ice of a central Greenland ice core, we have investigated changes in atmospheric HNO3 chemistry following the large volcanic eruptions of Laki (1783), Tambora (1815) and Katmai (1912). The concentration of several cations and anions, including SO 4 2– and NO 3 – , were measured using ion chromatography. We found that following those eruptions, the ratio of the concentration of NO 3 – deposited during winter to that deposited during summer was significantly higher than during nonvolcanic periods. Although we cannot rule out that this pattern originates from snow pack effects, we propose that increased concentrations of volcanic H2SO4 particles in the stratosphere may have favored condensation and removal of HNO3 from the stratosphere during Arctic winter. In addition, this pattern might have been enhanced by slower formation of HNO3 during summer, caused by direct consumption of OH through oxidation of volcanic SO2.  相似文献   

20.
Simultaneous measurements of the three rare isotopes Deuterium (D), Tritium (T), and Oxygen-18 (18O) in water vapour were made for the first time in the vicinity of the northern hemisphere tropopause. In contrast to expectation, high D/H and 18O/16O ratios, but relatively low T/H ratios, were found within the lowermost stratosphere. Since water vapour in the low-latitude upper troposphere shows a similar isotopic signature, we conclude that in the mid-latitudes considerable amounts of tropospheric water vapour are injected into the lowermost stratosphere, probably resulting in a hydration of the lower stratosphere. In addition, T can serve as tracer for precipitation of water containing stratospheric aerosol particles, because the T/H ratio in stratospheric water vapour is orders of magnitude higher than in the upper troposphere. Thus, even a small contribution of water of stratospheric origin should be detectable in the tropopause region. In our measurements performed in the Arctic we did not find isotopic evidence for sedimentation of PSC particles down to the tropopause. This may be caused by the low spatial and temporal coverage of our observations; however, it may also be due to the much weaker wintertime dehydration of the Arctic vortex compared to the Antarctic.  相似文献   

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