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1.
Causes for the unusually high and seasonally anomalous ozone concentrations at Summit, Greenland were investigated. Surface data from continuous monitoring, ozone sonde data, tethered balloon vertical profiling data, correlation of ozone with the radionuclide tracers 7Be and 210Pb, and synoptic transport analysis were used to identify processes that contribute to sources and sinks of ozone at Summit. Northern Hemisphere (NH) lower free troposphere ozone mixing ratios in the polar regions are ∼20 ppbv higher than in Antarctica. Ozone at Summit, which is at 3212 m above sea level, reflects its altitude location in the lower free troposphere. Transport events that bring high ozone and dry air, likely from lower stratospheric/higher tropospheric origin, were observed ∼40% of time during June 2000. Comparison of ozone enhancements with radionuclide tracer records shows a year-round correlation of ozone with the stratospheric tracer 7Be. Summit lacks the episodic, sunrise ozone depletion events, which were found to reduce the annual, median ozone at NH coastal sites by up to ∼3 ppbv. Synoptic trajectory analyses indicated that, under selected conditions, Summit encounters polluted continental air with increased ozone from central and western Europe. Low ozone surface deposition fluxes over long distances upwind of Summit reduce ozone deposition losses in comparison to other NH sites, particularly during the summer months. Surface-layer photochemical ozone production does not appear to have a noticeable influence on Summit's ozone levels.  相似文献   

2.
During a one-year period, from November 1998 upto October 1999, the atmospheric activity concentrations of the short-lived (222Rn)-progeny (218Po, 214Pb, 214Po) were measured every 4 h in the open air, using α-spectrometry. The concentration data of short-lived radon progeny together with meteorological variables (relative humidity, air temperature, and wind speed) were used for a comprehensive regression analysis of daily time variation of radioactivity in the air. The seasonal concentration pattern of all short-lived radon progeny shows the same trend for diurnal variation with higher values at night and early morning hours compared with lower values at noon and in afternoon. The activity concentrations were observed to be higher during the winter months (November–January) than in other seasons. The mean activity concentrations of 218Po, 214Pb and 214Po within the whole year were found to be 6.7±0.8, 4.9±0.5 and 4.4±0.3 Bq m−3, respectively.Also, within that time period, approximately 120 samples were analysed to determine the concentrations of the long-lived radon decay product 210Pb and the cosmogenic radionuclide 7Be using a single-filter technique. The course of 210Pb air concentration is characterized by higher values in autumn/winter season and lower values in spring/summer season. The seasonal concentration pattern of 7Be reaches regular maximum values in the spring to early summer months. The annual average concentration values of 210Pb and 7Be have been found to be 0.37±0.06 and 2.0±0.09 mBq m−3, respectively. A mean aerosol mass concentration of 36.6±6.2 μg m−3 was also determined during the measurements of the long-lived radionuclides. The majority of attached 210Pb and 7Be were observed at lower aerosol mass concentrations while small fractions of attached activities were found to be associated with the higher mass concentrations.  相似文献   

3.
Sonic anemometer turbulence measurements were made at Summit, Greenland during summer 2004 and spring 2005. These measurements allow for the characterization of the variability of the atmospheric boundary layer at this site by describing seasonal and diurnal changes in sensible heat flux and boundary layer stability as well as providing estimates of mixing layer height. Diurnal sensible heat fluxes at Summit ranged from −18 to −2 W m−2 in the spring and from −7 to +10 W m−2 in the summer. Sustained stable surface layer conditions and low wind speeds occured during the spring but not during the summer months. Unstable conditions were not observed at Summit until late April. Diurnal cycles of convective conditions during the daytime (0700–1700 h local time) were observed throughout July and August. Boundary layer heights, which were estimated for neutral to stable conditions, averaged 156 m for the spring 2005 observations. Comparisons of the boundary layer characteristics of Summit with those from South Pole, Antarctica, provide possible explanations for the significant differences in snowpack and surface-layer chemistry between the two sites.  相似文献   

4.
Direct measurements of radionuclide tracers are useful tools for correcting proxy fluxes that are subject to post depositional changes. An analytical methodology was designed for the measurement of 210Pb and 7Be in rainwater. Atmospheric inputs of the radionuclides to Cumbria (UK) were recorded. Rainwater fluxes were then compared with measurements from soil cores. The annual deposition from April 1997 to March 1998 of 210Pb and 7Be was 165 ± 8 Bq m-2 and 3912 ± 120 Bq m-2, respectively, compared to an indirect 210Pb flux of 148 ± 7 Bq m-2 yr-1 calculated from soil core records.  相似文献   

5.
High-volume PM2.5 samples were collected at Summit, Greenland for approximately six months from late May through December of 2006. Filters were composited and analyzed for source tracer compounds. The individual organic compounds measured at Summit are orders of magnitude smaller than concentrations measured at other sites, including locations representative of remote oceanic, and remote and urban continental aerosol. The measured tracers were used to quantify the contribution of biomass burning (0.6–0.9 ng C m?3), vegetative detritus (0.3–0.9 ng C m?3), and fossil fuel combustion (0.1–0.8 ng C m?3) sources, 4% of OC total, to atmospheric organic carbon concentrations at the remote location of Summit, Greenland. The unapportioned organic carbon (96%) during the early summer period correlates well with the fraction of water soluble organic carbon, indicating secondary organic aerosol as a large source of organic carbon, supported by the active photochemistry occurring at Summit. To the author's knowledge, this paper represents the first source apportionment results for the polar free troposphere.  相似文献   

6.
The atmospheric transport of 210Pb and 7Be is simulated by the Laboratoire de Météorologie Dynamique general circulation model, LMDz, driven by ECMWF reanalyses. Daily averaged concentrations collected at three surface stations are compared with numerical results for a 1 year (2004) global simulation. The model, with a resolution of 3.75°×2.5° and 19 levels, succeeds in reproducing daily variations of 210Pb and 7Be concentrations. Figures of merit in time (FMT), quantifying the overlapping of the predicted and observed time series over each month, range from 55% to 70%. Sensitivity studies as well as the analysis of numerical signals allow determining the main physical atmospheric processes characterizing the stations on a daily basis. Concentrations of 210Pb at the three stations are particularly sensitive to scavenging in convective updrafts.  相似文献   

7.
Leaves of linden (Tilia tomentosa L. and Tilia cordata Mill.) and horse chestnut (Aesculus hippocastanum L.) were analysed as biomonitors of radionuclides in urban air. Samples of soils, leaves and aerosols were collected in Belgrade, Serbia. Activities of 137Cs, 40K, 210Pb and 7Be in the samples were measured on an HPGe detector by standard gamma spectrometry. “Soil-to-leaves” transfer factors were calculated. Student’s t test and linear Pearson correlation coefficients were used for statistical analysis. Differences in local conditions at the sampling sites were not significant, and the mechanisms of the radionuclides’ accumulation in both plant species are similar. Ceasium-137 was detected in some of the leaf samples only. Transfer factors for 137Cs and 40K were (0.03–0.08) and 1.3, respectively. The concentrations of 210Pb and 7Be in leaves were higher in autumn than in spring, and there were some similarities in their seasonal patterns in leaves and in air. Weak to medium correlation was obtained for the 210Pb and 7Be activities in leaves and aerosols. Large positive correlation was obtained for the 210Pb activities in linden leaves and the mean activity in aerosols for the preceding months. Different primary modes of radionuclides accumulation in leaves were observed. Since large positive correlation was obtained for the 210Pb activity in linden leaves and the mean in aerosols for the preceding months, mature linden leaves could be used as biomonitors of recent 210Pb activity in air.  相似文献   

8.
The 7Be activity concentrations measured from 1996 to 1998 at four high-altitude stations, Jungfraujoch—Switzerland, Zugspitze—Germany, Sonnblick—Austria and Mt. Cimone—Italy, were analyzed in combination with a set of, meteorological and atmospheric parameters such as the tropopause height, relative and specific humidity and also in conjunction with 3D back-trajectories in order to investigate the climatological features of 7Be. A frequency distribution analysis on 7Be activity concentrations revealed the existence of two concentration classes around 1.5 and 6 mBq m−3 and a transition class between the two modes of the distribution at 3–4 mBq m−3. Cross-correlation analysis performed between 7Be and a number of meteorological and atmospheric parameters at the first three stations showed a strong negative correlation with relative humidity (−0.56, −0.51, −0.41) indicating the importance of wet scavenging as a controlling mechanism. Also, the positive correlation with the height of 3-days back-trajectories and tropopause height (+0.49/+0.43, +0.59/+0.36, +0.44/+0.38) shows that downward transport from the upper or middle to lower troposphere within anticyclonic conditions plays also an important role. Trajectory statistics showed that low 7Be concentrations typically originate from lower-altitude subtropical ocean areas, while high concentrations arrive from the north and high altitudes, as is characteristic for stratospheric intrusions. Although the 7Be activity concentrations are highly episodic, the monthly means indicate an annual cycle with a late-summer maximum at all stations. The correlation coefficients calculated for monthly means of the 7Be and atmospheric data suggest that the main predictor controlling the seasonality of the 7Be concentrations is tropopause height (+0.76, +0.56, +0.60), reflecting more vertical transport from upper tropospheric levels into the lower troposphere during the warm season than during the cold season.  相似文献   

9.
The 7Be activity concentrations measured from 1996 to 1998 at four high-altitude stations, Jungfraujoch—Switzerland, Zugspitze—Germany, Sonnblick—Austria and Mt. Cimone—Italy, were analyzed in combination with a set of, meteorological and atmospheric parameters such as the tropopause height, relative and specific humidity and also in conjunction with 3D back-trajectories in order to investigate the climatological features of 7Be. A frequency distribution analysis on 7Be activity concentrations revealed the existence of two concentration classes around 1.5 and 6 mBq m−3 and a transition class between the two modes of the distribution at 3–4 mBq m−3. Cross-correlation analysis performed between 7Be and a number of meteorological and atmospheric parameters at the first three stations showed a strong negative correlation with relative humidity (−0.56, −0.51, −0.41) indicating the importance of wet scavenging as a controlling mechanism. Also, the positive correlation with the height of 3-days back-trajectories and tropopause height (+0.49/+0.43, +0.59/+0.36, +0.44/+0.38) shows that downward transport from the upper or middle to lower troposphere within anticyclonic conditions plays also an important role. Trajectory statistics showed that low 7Be concentrations typically originate from lower-altitude subtropical ocean areas, while high concentrations arrive from the north and high altitudes, as is characteristic for stratospheric intrusions. Although the 7Be activity concentrations are highly episodic, the monthly means indicate an annual cycle with a late-summer maximum at all stations. The correlation coefficients calculated for monthly means of the 7Be and atmospheric data suggest that the main predictor controlling the seasonality of the 7Be concentrations is tropopause height (+0.76, +0.56, +0.60), reflecting more vertical transport from upper tropospheric levels into the lower troposphere during the warm season than during the cold season.  相似文献   

10.
Ultra-fine particle number concentrations were measured over Siberia during two large-scale airborne measurement campaigns in April and September 2006. During both campaigns, an aircraft flew between Novosibirsk and Yakutsk, collecting every 200 km vertical profiles up to 7 km. This dataset was completed by 5 years of monthly profiles above Novosibirsk. Particle number concentration was measured in the size ranges 3–70 and 70–200 nm, along with other tracers. Free troposphere (FT) particle concentrations (N3–200) varied between 60 and 460 cm?3, inferior to boundary layer concentrations (100–7000 cm?3). In April, high concentrations of ~500 cm?3 were observed in a polluted air mass recently uplifted at 5–6 km altitude over eastern Siberia, with no sign of significant new particle formation. In September, particle concentrations decreased with altitude, but with a steeper gradient in N70–200 compared to N3–70, the latter accounting for 90% of the total particle concentration in the free troposphere at 6–7 km altitude. Because ultra-fine particles presumably have short lifetimes, these observed particles could have been formed in situ in the clean Siberian atmosphere. Two cases of possible nucleation with high concentration and N3–70/N70–200 ratios are reported for the September campaign, in the upper troposphere and in cloud outflow in the mid-troposphere. In the seasonal analysis, a FT N3–70 maximum is found in July–August between 6 and 7 km altitude, with N3–70 accounting for ~90% of N3–200 supporting the hypothesis of in situ formation in the FT. A secondary FT maximum of N3–70 was identified later in autumn. In the boundary layer, seasonally maximum N3–70 concentrations were found over Novosibirsk in May and September, but not in summer, possibly due to scavenging by precipitations and a large condensational sink from biomass burning aerosols. Our dataset has a limited size resolution and no speciation capability; more investigation is thus required to understand the conditions leading to in situ nucleation processes in the Siberian air shed.  相似文献   

11.
Mixing in the planetary boundary layer (PBL) affects vertical distributions of air tracers in the lower troposphere. An accurate representation of PBL mixing is critical for chemical-transport models (CTMs) for applications sensitive to simulations of the vertical profiles of tracers. The full mixing assumption in the widely used global CTM GEOS-Chem has recently been supplemented with a non-local PBL scheme. This study analyzes the impact of the non-local scheme on model representation of PBL mixing, consequences for simulations of vertical profiles of air tracers and surface air pollution, and implications for model applications to the interpretation of data retrieved from satellite remote sensing. The non-local scheme significantly improves simulations of the vertical distributions for NO2 and O3, as evaluated using aircraft measurements in summer 2004. It also reduces model biases over the U.S. by more than 10 ppb for surface ozone concentrations at night and by 2–5 ppb for peak ozone in the afternoon, as evaluated using ground observations. The application to inverse modeling of anthropogenic NOx emissions for East China using satellite retrievals of NO2 from OMI and GOME-2 suggests that the full mixing assumption results in 3–14% differences in top–down emission budgets as compared to the non-local scheme. The top–down estimate combining the non-local scheme and the Lin et al. inverse modeling approach suggests a magnitude of 6.6 TgN yr?1 for emissions of NOx over East China in July 2008 and 8.0 TgN yr?1 for January 2009, with the magnitude and seasonality in good agreement with bottom–up estimates.  相似文献   

12.
Abstract

Natural radionuclides have been proposed as a means of assessing the transport of ozone (O3) and aerosols in the troposphere. Beryllium-7 (7Be) is produced in the upper troposphere and lower stratosphere by the interaction of cosmogenic particles with atmospheric nitrogen and oxygen. 7Be has a 53.29-day half-life (478 keV γ) and is known to attach to fine particles in the atmosphere once it is formed. It has been suggested that O3 from aloft can be transported into rural and urban regions during stratospheric–tropospheric folding events leading to increased background levels of O3 at the surface. 7Be can be used as a tracer of upper atmospheric air parcels and the O3 associated with them. Aerosol samples with a 2.5-µm cutoff were collected during 12-hr cycles (day/night) for a 30-day period at Deer Park, TX, near Houston, in August– September of 2000, and at Waddell, AZ, near Phoenix, in June–July of 2001. A comparison of 7Be levels with 12-hr O3 averages and maxima shows little correlation. Comparison of nighttime and daytime O3 levels indicate that during the day, when mixing is anticipated to be higher, the correlation of 7Be with O3 in Houston is approximately twice that observed at night. This is consistent with mixing and with the anticipated loss of O3 by reaction with nitric oxide (NO) and dry deposition. At best, 30% of the O3 variance can be explained by the correlation with 7Be for Houston, less than that for Phoenix where no significant correlation was seen. This result is consistent with the intercept values obtained for 7Be correlations with either O3 24-hr averages or O3 12-hr maxima and is also in the range of the low O3 levels (25 ppb) observed at Deer Park during a tropical storm event where the O3 is attributable primarily to background air masses. That is, maximum background O3 level contributions from stratospheric sources aloft are estimated to be in the range of 15–30 ppb in the Houston, TX, and Phoenix, AZ, area, and levels above these are because of local tropospheric photochemical production.  相似文献   

13.
The first measurements of peroxy (HO2+RO2) and hydroxyl (OH) radicals above the arctic snowpack were collected during the summer 2003 campaign at Summit, Greenland. The median measured number densities for peroxy and hydroxyl radicals were 2.2×108 mol cm−3 and 6.4×106 mol cm−3, respectively. The observed peroxy radical values are in excellent agreement (R2=0.83, M/O=1.06) with highly constrained model predictions. However, calculated hydroxyl number densities are consistently more than a factor of 2 lower than the observed values. These results indicate that our current understanding of radical sources and sinks is in accord with our observations in this environment but that there may be a mechanism that is perturbing the (HO2+RO2)/OH ratio. This observed ratio was also found to depend on meteorological conditions especially during periods of high winds accompanied by blowing snow. Backward transport model simulations indicate that these periods of high winds were characterized by rapid transport (1–2 days) of marine boundary layer air to Summit. These data suggest that the boundary layer photochemistry at Summit may be periodically impacted by halogens.  相似文献   

14.
The seasonal variation of the 210Po/210Pb activity ratio in aerosols, as a function of particle size, have been studied at Kamo, on the west coast of Japan from July 1995 to June 1996. It was shown that 70% of 210Po and 77% of 210Pb activities were measured in aerosols with a diameter smaller than 0.7 μm. On the other hand, the abundances of 210Po and 210Pb in aerosols with a diameter larger than 10.9 μm were 3 and 1%, respectively. In general, the maxima of the 210Po/210Pb ratio were observed in aerosols of 5.4–10.9 μm, but the maxima in January and April 1996 appeared in the largest and the smallest size fractions, respectively. The results suggest that the size distribution of the 210Po/210Pb activity ratio may be modified by changes in the nature and intensity of aerosol sources.  相似文献   

15.
Strok M  Smodiš B 《Chemosphere》2011,82(7):970-976
210Po and 210Pb activity concentrations in fish from the Slovenian part of Adriatic Sea, in the vicinity of a former uranium mine at ?irovski vrh and from the Slovenian market were determined. In addition, 210Po and 210Pb activity concentrations in squid from the Slovenian market and in mussels from the Slovenian part of the Adriatic Sea were also determined. Fish, squid and mussel consumption in Slovenia was assessed from the data available from Eurostat and Food and Agriculture Organisation (FAO) and the data used for the corresponding dose calculation. Fish species with the highest activity concentrations were grilled to assess possible loss of 210Po during the food preparation process. Samples were freeze dried and radiochemical separation of 210Po and 210Pb was performed. Measurements of 210Po were performed by alpha spectrometry and 210Pb by a low background gas-flow proportional counter. 210Po activity concentrations in fish, squid and mussels were from 0.039 to 35.0 Bq kg−1 fresh weight and 210Pb activity concentrations were from 0.08 to 3.03 Bq kg−1 fresh weight. Grilling of fish resulted in no significant loss of 210Po at 90 °C. The assessed combined annual effective ingestion dose due to 210Po and 210Pb for fish, squid and mussels consumed in Slovenia is 47.6 μSv year−1.  相似文献   

16.
A background of ozone (O3), principally of stratospheric origin, is present in the lower free troposphere. Typical mean O3 levels of 50 ppb, 40 ppb, and 30 ppb are encountered here in spring, summer, and fall, respectively. Maximum hourly O3 concentrations which are twice these mean values can be expected. Ozone from the free troposphere is routinely brought down to ground level under turbulent atmospheric conditions. Deep and rapid Intrusions of stratospheric air into the lower troposphere are associated with low-pressure troughs and occur regularly. In the mid troposphere, O3 levels as high as 300 ppb are found within these intrusions. Observational data showing these intrusions, containing high O3 concentrations, to directly reach ground level are currently lacking. Over the United States, an intrusion was present aloft on 8 9% of the days in 1978. The frequency, however, is somewhat reduced in summer and a northward movement is evident. During 1978, no intrusion occurred south of 30°N between June and August and none south of 40 °N in August.

The hypothesis that low levels of stratospheric O3 produce disproportionately large amounts of O3 in the polluted atmosphere cannot be supported from currently known chemistry but should be studied further. The experimental technique involving a 7Be/O3 ratio to estimate the daily stratospheric component of ground level O3 is unverified and considered to be inadequate for air quality applications. Estimates resulting from such a technique are considered uncertain by a factor of more than three. Specially designed aircraft studies provide the best means to determine quantitatively the impact of stratospheric O3 on ground level air quality.  相似文献   

17.
Study of the vertical concentration profile and of the deposition of cosmogenic radionuclides provides information on the vertical transport in the stratosphere and troposphere and the processes of scavenging of aerosol particles by precipitation. Information on the distribution of atmospheric aerosols is important for the understanding of the physical processes relating to the studies in weather climate, air pollution, and aerosol physics. In this work the one-dimensional steady-state model of vertical concentration profile was established and the values of turbulent diffusion coefficient and scavenging coefficient determined by model using experimental data of the 7Be monthly average atmospheric activity concentrations and monthly deposition fluxes in Bratislava are presented. The temporal variations of the vertical distribution profiles of 7Be for each month are also calculated.  相似文献   

18.
Results of 2 years monitoring of 210Po and 210Pb activity concentrations in soft tissue of the species Mytilus galloprovincialis from Croatian part of the Adriatic coast are presented. The samples were collected at thirteen coastal stations (some of which are also a part of the Mediterranean Mussel Watch Project) in spring and autumn of 2010 and 2011. The collected mussels were ranging between 4 cm and 6 cm in shell length. After sample pre-treatment lead and polonium were radiochemically separated on Sr resin. 210Po was determined by alpha-particle spectrometry and 210Pb was determined, via 210Bi, by a low-level gas proportional counter. The results of 210Po activity concentrations were found to vary between (104 ± 11) and (1421 ± 81) Bq kg−1 dry weight while 210Pb activity concentrations were much lower and in range (8.2 ± 5.3)–(94.1 ± 29.8) Bq kg−1 dry weight. Higher 210Po and 210Pb activity concentrations were determined in spring period. The inter-site differences seen in their activity concentrations can be due to natural background levels of sites. The 210Po/210Pb activity concentration ratios in all cases exceeded unity for all mussel samples and ranged between 4.0 and 47.9.  相似文献   

19.
In the Aguere Valley (in the oceanic boundary layer at Tenerife, 28°N, 16°W, 580 m a.s.l.) the ozone levels were monitored for ambient air quality assessment. Although precursors are emitted in this area, the strong correlation between ozone levels and wind velocity indicates that ozone is transported into the valley from the ocean. The inland ozone supply along the valley is induced by an orographic channelling effect of the northern oceanic air masses. The highest ozone concentrations are mostly recorded during the nocturnal stage under the influence of fresh oceanic air masses, and during high wind speed events. The seasonal cycle is characterised by elevated ozone mixing ratios in the spring (nighttime levels >45 ppbv) and low mixing ratios in the summer (nighttime levels in the range 20–35 ppbv). Back-trajectory analysis shows that the ozone monitored in the Aguere Valley is associated with long-range transport processes. High ozone events in the spring are associated with transport from upper tropospheric levels, both over the North Atlantic-high latitudes (>45°N) and Europe. This downward transport was observed in the western edge of upper tropospheric cyclones, which suggests that the upper tropospheric/low stratospheric ozone sources play a significant role. In summer, ozone is mainly transported from the North Atlantic-high latitudes (>45°N) and from mid- to low-tropospheric levels. In autumn and winter, the high ozone concentrations are transported from sources located a few km above the North Atlantic-high latitudes (>45°N) and over Europe. The Central-North Atlantic (<45°N) and North Africa are not significant sources of ozone. The high spring and lower summer ozone events in the Aguere Valley agree with other North Atlantic ozone observation in the oceanic boundary layer. However, this behaviour contrasts with the high ozone events frequently recorded at Izaña BAPMoN station (located in the free troposphere in Tenerife) during the summer, which have been attributed in the literature to downward transport from upper levels. An intensification of the inversion layer that separates the oceanic boundary layer of the free troposphere during the summer in Canary Islands is interpreted as the cause of this different behaviour between ozone in the Aguere Valley and Izaña BAPMoN station.  相似文献   

20.
The root uptake of lead (Pb) by trees and the transfer of Pb by leaf litter deposition to the forest floor were investigated through a pot experiment with Norway spruce. Natural Pb and radio isotopic lead (210Pb) were determined in needles and twigs and in the pot soil spiked with 210Pb. Calculations of the specific activity in plant material and in the supporting pot soil showed that less than 2% of the Pb content of needles and twigs originates from root uptake and approximately 98% are deposited from the atmosphere. Atmospheric Pb has declined by a factor of 7 from 1980 to 2007 but is still a major pathway of Pb to vegetation and topsoils. The conclusion from the experiment is that the internal circulation of Pb through root uptake, translocation and litterfall, gives an insignificant input of Pb to the forest floor compared to atmospheric deposition.  相似文献   

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