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1.
We calculated daily back-trajectories using the NOAA-HYSPLIT model to analyze 7 years of precipitation and PM2.5 data from three National Park sites in the Western US. Using a k-means clustering algorithm, the trajectories were segregated into six main transport patterns. At each site, we calculated trajectory clusters for 1, 5, and 10 days to represent short, medium and long-range flow patterns. Most clusters show marked seasonality. Faster flow patterns are more prevalent in winter, and slower/stagnant patterns are more prevalent in summer. The analyses between the 1, 5, and 10-day clusters revealed that the clusters of different duration show very different predictive power for rainfall and PM2.5. We found that the 1-day clusters are a better predictor for precipitation and PM2.5 concentrations, followed by the 5-day clusters. The 10-day clusters did a poorer job of differentiating precipitation and PM2.5. This is because the 10-day clusters show the greatest variability during the first day or two of transport.  相似文献   

2.
Each summer period extremely high ozone levels are registered at the rural background station of Lamas d'Olo, located in the Northeast of Portugal. In average, 30% of the total alert threshold registered in Portugal is detected at this site. The main purpose of this study is to characterize the atmospheric conditions that lead to the ozone-rich episodes at this site. Synoptic patterns anomalies and back trajectories cluster analysis were performed, for the period between 2004 and 2007, considering 76 days when ozone maximum hourly concentrations were above 200 μg m?3. The obtained atmospheric anomaly fields suggested that a positive temperature anomaly is visible above the Iberian Peninsula. A strong wind flow pattern from NE is observable in the North of Portugal and Galicia, in Spain. These two features may lead to an enhancement of the photochemical production and to the transport of pollutants from Spain to Portugal. In addition, the 3D mean back trajectories associated to the ozone episode days were analysed. A clustering method has been applied to the obtained back trajectories. Four main clusters of ozone-rich episodes were identified, with different frequencies of occurrence: north-westerly flows (11%); north-easterly flows (45%), southern flow (4%) and westerly flows (40%). Both analyses highlight the NE flow as a dominant pattern over the North of Portugal during summer. The analysis of the ozone concentrations for each selected cluster indicates that this northeast circulation pattern, together with the southern flow, are responsible for the highest ozone peak episodes. This also suggests that long-range transport of atmospheric pollutants is the main contributor to the ozone levels registered at Lamas d'Olo. This is also highlighted by the correlation of the ozone time-series with the meteorological parameters analysed in the frequency domain.  相似文献   

3.
Meteorological conditions associated with regional scale episodes of elevated atmospheric sulfur concentrations over the regions of Arizona and New Mexico, and North and South Dakota were studied. Episodes were defined as the period when the atmospheric concentration of fine sulfur (diameters less than 2.5 μm) at each station in the region exceeded one standard deviation above the station's annual geometric mean.For the Arizona and New Mexico region, the most extraordinary episode occurred during September 1979 when an anticyclonic circulation aloft covered the entire region, while a planetary boundary layer (PBL) convergence zone existed over western Arizona and southeastern California. Convergence of pollutants in the PBL along with slow transport and dispersion by the anticyclonic flow took place during the episode. A similar flow pattern was responsible for an August 1981 episode. Copper smelters in southern Arizona and New Mexico apparently were the major cause of these episodes. Southerly or southeasterly flow during September 1982 again transported sulfur from the smelter region, causing another episode.A statistical study of backward air parcel trajectories from Grand Canyon National Park showed that southern Arizona and New Mexico, as well as the San Joaquin Valley of California, were potential source regions of atmospheric sulfur at the Grand Canyon.Long-range transport of pollutants from states east and/or southeast of North and South Dakota was the major cause of episodes in this region. These episodes occurred when high pressure systems were located over southern Canada or the northeastern United States.A statistical study of backward air parcel trajectories from Theodore Roosevelt National Park (North Dakota) showed that long-range transport from states east and/or southeast of the park was primarily responsible for high concentrations of fine sulfur. No clean air parcels arrived at the park from states to the east.  相似文献   

4.
In order to contribute to current knowledge of ozone concentrations and transport across the Central Massif, a monitoring station was installed at 1780 m on the upper Spanish plateau about 55 km from the city of Madrid. Ozone concentrations and standard meteorological variables were measured in June and July 2002. A smoothed ozone hourly cycle was obtained with mean values of 120 and 110 microgm(-3) during day-time and night-time, respectively. The highest ozone concentrations were recorded in the SE-S-SW wind sectors, proving the influence of transport from the Madrid urban plume to the upper plateau. This assumption was also supported by the satisfactory correlation between ozone peaks obtained at the monitoring site and those recorded in a representative station on the foothill located on the lower plateau during episodic situations. To assess the contribution of long-range transport, backward air mass trajectories were computed each day of measurements at 820 hPa. The lowest ozone mean was linked to Atlantic Ocean air masses, and the highest to air masses from Central Europe.  相似文献   

5.
This paper evaluates the effects of long-range transport patterns of air masses to the regional PM profile in a megacity, Istanbul, Turkey. Five-day hourly backward trajectories were obtained by the HYSPLIT model for selected episodic events in 2008. Self Organizing Maps (SOM), a very powerful classification tool, was used to cluster these trajectories. In total, eight cluster groups were obtained. All of the clusters were evaluated with respect to inhalable particulate matter (PM10) concentrations observed in Istanbul for the arrival times of the trajectories. Istanbul is generally under the effect of trajectories in three clusters (1, 2 and 4) (52% of all pre-selected episodic events), which have higher mean concentration values than the mean value of all the samples. These clusters typically make significant PM contributions to Istanbul's air quality. PM loadings of the trajectories in these clusters were attributed to massive anthropogenic activity over all of Europe and southwestern air flow most likely carrying PM10 atmospheric particles originating from the Saharan Desert and other global dust generation regions located in the northern part of Africa.  相似文献   

6.
Continuous measurements of particle number (PN), particle mass (PM10), and gaseous pollutants [carbon monoxide (CO), nitric oxide (NO), oxides of nitrogen (NOx), and ozone (O3)] were performed at five urban sites in the Los Angeles Basin to support the University of Southern California Children's Health Study in 2002. The degree of correlation between hourly PN and concentrations of CO, NO, and nitrogen dioxide (NO2) at each site over the entire year was generally low to moderate (r values in the range of 0.1-0.5), with a few notable exceptions. In general, associations between PN and O3 were either negative or insignificant. Similar analyses of seasonal data resulted in levels of correlation with large variation, ranging from 0.0 to 0.94 depending on site and season. Summertime data showed a generally higher correlation between the 24-hr average PN concentrations and CO, NO, and NO2 than corresponding hourly concentrations. Hourly correlations between PN and both CO and NO were strengthened during morning rush-hour periods, indicating a common vehicular source. Comparing hourly particle number concentrations between sites also showed low to moderate spatial correlations, with most correlation coefficients below 0.4. Given the low to moderate associations found in this study, gaseous co-pollutants should not be used as surrogates to assess human exposure to airborne particle number concentrations.  相似文献   

7.
During April 1996–June 1997 size-segregated atmospheric aerosol particles were collected at an urban and a rural site in the Helsinki area by utilising virtual impactors (VI) and Berner low-pressure impactors (BLPI). In addition, VI samples were collected at a semi-urban site during October 1996–May 1997. The average PM2.3 (fine particle) concentrations at the urban and rural sites were 11.8 and 8.4 μg/m3, and the PM2.3−15 (coarse particle) concentrations were 12.8 and about 5 μg/m3, respectively. The difference in fine particle mass concentrations suggests that on average, more than one third of the fine mass at the urban site is of local origin. Evaporation of fine particle nitrate from the VI Teflon filters during sampling varied similarly at the three sites, the average evaporation being about 50–60%.The average fine particle concentrations of the chemical components (25 elements and 13 ions) appeared to be fairly similar at the three sites for most components, which suggests that despite the long-range transport, the local emissions of these components were relatively evenly distributed in the Helsinki area. Exceptions were the average fine particles Ba, Fe, Sb and V concentrations that were clearly highest at the urban site pointing to traffic (Ba, Fe, Sb) and to combustion of heavy fuel oil (V) as the likely local sources. The average coarse particle concentrations for most components were highest at the urban site and lowest at the rural site.Average chemical composition of fine particles was fairly similar at the urban and rural sites: non-analysed fraction (mainly carbonaceous material and water) 43% and 37%, sulphate 21% and 25%, crustal matter 12% and 13%, nitrate 12% and 11%, ammonium 9% and 10% and sea-salt 2.5% and 3.2%, respectively. At the semi-urban site also, the average fine particle composition was similar. At the urban site, the year round average composition of coarse particles was dominated by crustal matter (59%) and the non-analysed components (28%, mainly carbonaceous material and water), while the other contributions were much lower: sea-salt 7%, nitrate 4% and sulphate 2%. At the rural site, the coarse samples were collected in spring and summer and the percentage was clearly lower for crustal matter (37%) and sea-salt (3%) but higher for the not-analysed fraction (51%). At the semi-urban site, the average composition of coarse particles was nearly identical to that at the urban site.Correlations between the chemical components were calculated separately for fine and coarse particles. In urban fine particles sulphate, ammonium, Tl, oxalate and PM2.3 mass correlated with each other and originated mainly from long-range transport. The sea-salt ions Na+, Cl and Mg2+ formed another group and still another group was formed by the organic anions oxalate, malonate, succinate, glutarate and methane sulphonate. Ni and V correlated strongly pointing to combustion of heavy fuel oil as the likely source. In addition, some groups with lower correlations were detected. At the rural and semi-urban sites, the correlating components were rather similar to those at the urban site, although differences were also observed.  相似文献   

8.
Meteorological trajectory analysis, MAP3S precipitation chemistry data, and hourly precipitation data at Whiteface Mountain (WFM) were used to determine the source direction of sulfate deposited in precipitation for 1978. A sensitivity study was done on source direction from different trajectory models, using different transport layers, and different precipitation information to determine the time deposition occurred. Results obtained from the different precipitation information indicate that precipitation data in 6-h increments or less are essential to correctly identify the trajectories associated with the wet deposition. Bias resulted when trajectories were not only associated with wet deposition. The direction of source regions, defined by 30° sectors, was much less dependent on the trajectory model or transport layer. Results suggest that over one-third of the wet sulfate deposition at WFM in 1978 arrived from the west-southwest, passing through the eastern Great Lakes region.  相似文献   

9.
A trajectory statistics method has been used to examine the causes of variability and seasonality of sulphur dioxide, particulate sulphate and non-sea-salt sulphate in precipitation measured at a French rural site. This methodology has permitted to define the likely contributing sources for two seasons, a warm and a cold, that show different patterns. The general results suggest the impact of the long-range transport of SO2 and SO2 secondary species from high anthropogenic sources. The increase of photochemical activity during the warm period, the seasonal large-scale wind movements responsible for precipitation and the removal processes during atmospheric transport may also significantly influence sulphur concentrations at Morvan.  相似文献   

10.
The impact of various atmospheric transport directions on ambient fine particle (PM2.5) concentrations at several sites in southeastern Canada was estimated (for May-September) using back-trajectory analysis. Three-day back trajectories (four per day) were paired with 6-hr average PM2.5 mass concentrations measured using tapered element oscillating microbalances (TEOM). PM2.5 concentrations at rural locations in the region were affected by nonlocal sources originating in both Canada and the United States. Comparison of sites revealed that, on average, the local contribution to total PM2.5 in the greater Toronto area (GTA) is approximately 30-35%. At each location, average PM2.5 concentrations under south/southwesterly flow conditions were 2-4 times higher than under the corresponding northerly flow conditions. The chemical composition of both urban and rural PM2.5 was determined during two separate 2-week spring/summer measurement campaigns. Components identified included SO4(2-) NO3-, NH4+, black carbon and organic carbon (OC), and trace elements. Higher particle mass at the urban Toronto site was composed of a higher proportion of all components. However, black carbon, NO3-, NaCl, and trace elements were found to be the most enriched over the rural/regional background levels.  相似文献   

11.
Kim KH  Kim MY  Hong SM  Youn YH  Hwang SJ 《Chemosphere》2005,59(7):929-937
The concentrations of three different size fractions of particulate matter (PM) including PM2.5, PM10, and TSP were determined continuously at hourly intervals from four different sites in Seoul, Korea during the spring of 2001. To learn the effects of wind speed change on PM fractionation, the entire data sets were initially sorted into three particle fractions such as: fine (F: PM2.5), coarse (C: PM10-PM2.5), and giant (G: TSP-PM10). The inter-fraction relationships of PM were then explored by linear regression analysis of the data divided into four wind speed regimes. The results of this analysis, when examined in terms of either relative dominance between different PM fractions (i.e., in terms of their slope values) or strength of correlations, indicate the existence of diverse inter-fraction patterns. Most importantly, the physical influence of wind speed is seen to be reflected most efficiently between fine and coarse particle fractions, as the relative contribution of coarse fraction to the mass concentration of total particles (e.g., PM10) changes proportionally with changes in wind speed. However, such systematic patterns decrease noticeably between fine and giant fractions, as they can be affected more sensitively by such factors as the nature of their sources or the surrounding environmental conditions. The results of our comparative analysis thus confirm that wind speed is a useful barometer to distinguish and predict the behavior of different particle fractions in relation to each other.  相似文献   

12.
The relationships are considered between monthly and quarterly means of the fine particle sulfur (S) concentrations and wind flow direction, period of day and season of the year. The measurements used are those obtained at selected urban and at rural monitoring stations in the St Louis area during the Regional Air Pollution Study in 1975, 1976 and 1977. Higher mean fine particle S concentrations are observed with wind flows from the E compared to the W and from the NE and SE quadrants compared to the NW quadrant. Substantially higher fine particle S concentrations are obtained with wind flows from the E compared to the W even when conditions are selected so that the values of temperature, solar radiation intensity and wind speed are within the same restricted ranges. A consistent increase in the fine particle S concentrations occurs through the late morning and afternoon with decrease in the evening and especially in the early morning during spring and summer months with wind flows from the E.The contributions are estimated for local scale and regional scale processes to the observed fine particle S concentrations. Local scale processes include those involving atmospheric formation and primary emissions each contribute 0.6−1.0 and 0.6 μg m−3 of the fine particle S. Regional scale processes account for the greater part of the observed concentrations especially when the wind flows are from the SE or SW. Regional scale episodes involving passage of warm high pressure systems to the E of St Louis with accumulation of precursors made especially significant contributions to formation of fine particle S.The atmospheric gas phase and liquid phase chemical reactions contributing to the formation of fine particle S are discussed. Emphasis is placed on the effects of chemistry on the seasonal variations in concentrations of fine particle S.  相似文献   

13.
Polycyclic aromatic hydrocarbons (PAH) were measured in air samples at a remote air monitoring site established in the Yukon Territory, Canada as part of a global project (International Polar Year; IPY) to study the potential for atmospheric long-range transport of anthropogenic pollutants to the Arctic. Gas- and particle-phase PAH were collected in polyurethane foam plugs and on glass fibre filters respectively from August 2007 to October 2009. PAH concentrations were found to be highest in the winter months and lowest in summer. The gas/particle partitioning coefficients of 3–5 ringed PAH were computed and seasonal averages were compared. In the summer time, lower molecular mass PAH exhibited relatively higher partitioning into the particle-phase. This particle-phase partitioning led to the shallowest slopes being recorded during summer for the log–log correlation plots between the PAH partition coefficients and their sub-cooled vapour pressures. Air mass back trajectories suggest that local impacts may be more important during the summer time which is marked by increased camping activities at camping sites in the proximity of the sampling station. In conclusion, both summer and wintertime variations in PAH concentrations and gas/particle partitioning are considered to be source- and phototransformation-dependent rather than dependent on temperature-driven shifts in equilibrium partitioning.  相似文献   

14.
During January and February 1984, a field project was conducted near North Bay, Ontario, Canada. The principal objective was to characterize the chemical and microphysical properties of the air masses, clouds and precipitation in this region of NE North America during the winter season. Two extensively instrumented aircraft with some newly designed cloudwater and snow collectors were used, as well as a surface station continuously monitoring pollutant concentrations and a precipitation event sampling network. Pollutant concentrations at the surface were found to vary with the airmass back trajectory with the highest concentrations observed for trajectories from the S and SW and the lowest from the N. Vertical profiles of aerosol particle (0.2−2 μm diameter) and NOx concentrations show similar trends with maxima of 1200 cm−3 and 7 ppb, respectively near ground level with air mass trajectories from the S, in comparison to values of 250 cm−3 and 1 ppb obtained with trajectories from the N. Cloudwater, aircraft precipitation and ground precipitation samples had a daily median pH of 3.6,4.6 and 4.2, respectively with the cloudwater having the highest sulphate and nitrate concentrations. The nitrate/sulphate equivalent concentration ratios in the cloudwater, aircraft precipitation and ground precipitation samples were 0.7,0.6 and 1.4, respectively. The data suggest that precipitation scavenging of nitric acid below cloud base is an important process during the winter season.  相似文献   

15.
The measurements during episodic periods in the St. Louis area in 1975 and 1976 of fine particle sulfur, fine particle mass and ozone are related. Such episodes are concentrated into time periods in the late spring and summer months. During such episodes, particle sulfur is the major constituent of the fine particle mass. The sum of the non-sulfur species in the fine particle mass do not show similar episodic patterns as the fine particle sulfur.Elevated concentrations of fine particle sulfur and of ozone usually occur together within the same episodic time periods. However, the day to day variations in fine particle sulfur and of ozone do differ somewhat within these time periods.Both fine particle sulfur and ozone show the influence of regional scale and local scale atmospheric photochemical processes on their formation during episodic time periods. Regional scale boundary layer processes frequently appear to contribute more to fine particle sulfur concentrations than to ozone formation. Local scale primary emissions also contribute to the ambient fine particle sulfur concentrations at core urban locations.  相似文献   

16.
Measurements of size-resolved particle number concentrations during the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) field campaign were made at the Gosan super-site, South Korea. In East Asia, dust and precipitation phenomena play a crucial role in atmospheric environment and climate studies because they are major sources and sinks of atmospheric aerosols, especially in the springtime. Total Ozone Mapping Spectrometer (TOMS) Aerosol Index and backward trajectories are analyzed to investigate the spatial and temporal evolution of dust storms. The size distributions between dust and non-dust periods and times with and without precipitation are compared. In order to understand the temporal evolution of the aerosol size distribution during dust and precipitation events, a simple aerosol dynamics model is employed. The model predicted and observed size distributions are compared with the measured data. The results show that the coarse mode particle number concentrations increase by a factor of 10–16 during dust events. During precipitation, however, particles in the coarse mode are scavenged by impaction mechanism. It is found that the larger particles are more efficiently scavenged. The degree of scavenged particle varies depending on the rainfall rate, raindrop size distribution and aerosol size distribution.  相似文献   

17.
Air quality monitoring was conducted at a rural site with a tower in the middle of California's San Joaquin Valley (SJV) and at elevated sites in the foothills and mountains surrounding the SJV for the California Regional PM10/ PM2.5 Air Quality Study. Measurements at the surface and n a tower at 90 m were collected in Angiola, CA, from December 2000 through February 2001 and included hourly black carbon (BC), particle counts from optical particle counters, nitric oxide, ozone, temperature, relative humidity, wind speed, and direction. Boundary site measurements were made primarily using 24-hr integrated particulate matter (PM) samples. These measurements were used to understand the vertical variations of PM and PM precursors, the effect of stratification in the winter on concentrations and chemistry aloft and at the surface, and the impact of aloft-versus-surface transport on PM concentrations. Vertical variations of concentrations differed among individual species. The stratification may be important to atmospheric chemistry processes, particularly nighttime nitrate formation aloft, because NO2 appeared to be oxidized by ozone in the stratified aloft layer. Additionally, increases in accumulation-mode particle concentrations in the aloft layer during a fine PM (PM2.5) episode corresponded with increases in aloft nitrate, demonstrating the likelihood of an aloft nighttime nitrate formation mechanism. Evidence of local transport at the surface and regional transport aloft was found; transport processes also varied among the species. The distribution of BC appeared to be regional, and BC was often uniformly mixed vertically. Overall, the combination of time-resolved tower and surface measurements provided important insight into PM stratification, formation, and transport.  相似文献   

18.
Five intensive field measurements were carried out at two background sites in Korea; Kosan and Kangwha during spring, fall, and winters of 1996 and 1997 to investigate the characteristics of long-range transport of air pollutants in northeastern Asia. Fine particles (PM2.5) were collected by low-volume samplers and the concentrations of major ions, organic and elemental carbons, and nitric acid were quantified. The concentrations of anthropogenic species in PM2.5 measured at both sites were generally higher than those at other background areas, Nagano, Japan and San Nicolas Is., USA due to continental outflow of air pollutants, but lower than those at an urban background site, Qingdao, China. The major components of PM2.5 were sulfate, organic carbon (OC), and ammonium for Kosan and sulfate, OC, ammonium, and nitrate for Kangwha. The major fractions of sulfate at both sites are non-sea-salts (nss) sulfate. Based on the relationship among major anthropogenic species, analysis of the nss sulfate to total nitrate molar ratios, and backward air parcel trajectories, it was found that fine particles measured at both sites during the measurement periods are mainly coming from China. At Kosan, the concentrations of anthropogenic species were higher when air parcels were coming from southern China than when air parcels were from northern China. At Kangwha, however, the differences of the concentrations were not statistically significant since most air parcels were from northern China and local effects are prominent.  相似文献   

19.
This paper presents measurements of daily sampling of fine particulate matter (PM2.5) and its major chemical components at three urban and one rural locations in North Carolina during 2002. At both urban and rural sites, the major insoluble component of PM2.5 is organic matter, and the major soluble components are sulfate (SO4(2-)), ammonium (NH4(+)), and nitrate (NO3(-)). NH4(+) is neutralized mainly by SO4(2-) rather than by NO3(-), except in winter when SO4(2-) concentration is relatively low, whereas NO3(-) concentration is high. The equivalent ratio of NH4(+) to the sum of SO4(2-) and NO3(-) is < 1, suggesting that SO4(2-) and NO3(-) are not completely neutralized by NH4(+). At both rural and urban sites, SO4(2-) concentration displays a maximum in summer and a minimum in winter, whereas NO3(-) displays an opposite seasonal trend. Mass ratio of NO3(-) to SO4(2-) is consistently < 1 at all sites, suggesting that stationary source emissions may play an important role in PM2.5 formation in those areas. Organic carbon and elemental carbon are well correlated at three urban sites although they are poorly correlated at the agriculture site. Other than the daily samples, hourly samples were measured at one urban site. PM2.5 mass concentrations display a peak in early morning, and a second peak in late afternoon. Back trajectory analysis shows that air masses with lower PM2.5 mass content mainly originate from the marine environment or from a continental environment but with a strong subsidence from the upper troposphere. Air masses with high PM2.5 mass concentrations are largely from continental sources. Our study of fine particulate matter and its chemical composition in North Carolina provides crucial information that may be used to determine the efficacy of the new National Ambient Air Quality Standard (NAAQS) for PM fine. Moreover, the gas-to-particle conversion processes provide improved prediction of long-range transport of pollutants and air quality.  相似文献   

20.
Detailed hourly precipitation data are required for long-range modeling of dispersion and wet deposition of particulate matter and water-soluble pollutants using the CALPUFF model. In sparsely populated areas such as the north central United States, ground-based precipitation measurement stations may be too widely spaced to offer a complete and accurate spatial representation of hourly precipitation within a modeling domain. The availability of remotely sensed precipitation data by satellite and the National Weather Service array of next-generation radars (NEXRAD) deployed nationally provide an opportunity to improve on the paucity of data for these areas. Before adopting a new method of precipitation estimation in a modeling protocol, it should be compared with the ground-based precipitation measurements, which are currently relied upon for modeling purposes. This paper presents a statistical comparison between hourly precipitation measurements for the years 2006 through 2008 at 25 ground-based stations in the north central United States and radar-based precipitation measurements available from the National Center for Environmental Predictions (NCEP) as Stage IV data at the nearest grid cell to each selected precipitation station. It was found that the statistical agreement between the two methods depends strongly on whether the ground-based hourly precipitation is measured to within 0.1 in/hr or to within 0.01 in/hr. The results of the statistical comparison indicate that it would be more accurate to use gridded Stage IV precipitation data in a gridded dispersion model for a long-range simulation, than to rely on precipitation data interpolated between widely scattered rain gauges.

Implications:

The current reliance on ground-based rain gauges for precipitation events and hourly data for modeling of dispersion and wet deposition of particulate matter and water-soluble pollutants results in potentially large discontinuity in data coverage and the need to extrapolate data between monitoring stations. The use of radar-based precipitation data, which is available for the entire continental United States and nearby areas, would resolve these data gaps and provide a complete and accurate spatial representation of hourly precipitation within a large modeling domain.  相似文献   


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