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1.
Aerosol light scattering measurements as a function of relative humidity   总被引:1,自引:0,他引:1  
The hygroscopic nature of atmospheric fine aerosol was investigated at a rural site in the Great Smoky Mountains National Park during July and August 1995. Passing the sample aerosol through an inlet, which housed an array of Perma Pure diffusion dryers, controlled the sample aerosol's relative humidity (RH). After conditioning the aerosol sample in the inlet, the light scattering coefficient and the aerosol size distribution were simultaneously measured. During this study, the conditioned aerosol's humidity ranged between 5% < RH < 95%. Aerosol response curves were produced using the ratio bspw/bspd; where bspw is the scattering coefficient measured at some RH greater than 20% and bspd is the scattering coefficient of the "dry" aerosol. For this work, any sample RH values below 15% were considered dry. Results of this investigation showed that the light scattering ratio increased continuously and smoothly over the entire range of relative humidity. The magnitude of the ratio at a particular RH value, however, varied considerably in time, particularly for RH values greater than approximately 60%. Curves of the scattering coefficient ratios as a function of RH were generated for each day and compared to the average 12-hour chemical composition of the aerosol. This comparison showed that for any particular RH value the ratio was highest during time periods of high sulfate concentrations and lowest during time periods of high soil or high organic carbon concentrations.  相似文献   

2.
The goal of the Regional Haze Rule (RHR) is to return visibility in class I areas (CIAs) to natural levels, excluding weather-related events, by 2064. Whereas visibility, the seeing of scenic vistas, is a near instantaneous and sight-path-dependent phenomenon, reasonable progress toward the RHR goal is assessed by tracking the incremental changes in 5-yr average visibility. Visibility is assessed using a haze metric estimated from 24-hr average aerosol measurements that are made at one location representative of the CIA. It is assumed that, over the 5-yr average, the aerosol loadings and relative humidity along all of the site paths are the same and can be estimated from the 24-hr measurements. It is further assumed that any time a site path may be obscured by weather (e.g., clouds and precipitation), there are other site paths within the CIA that are not. Therefore, when calculating the haze metric, sampling days are not filtered for weather conditions. This assumption was tested by examining precipitation data from multiple monitors for four CIAs. It is shown that, in general, precipitation did not concurrently occur at all monitors for a CIA, and precipitation typically occurred 3-8 hr or less in a day. In a recent paper in this journal, Ryan asserts that the haze metric should include contributions from precipitation and conducted a quantitative assessment incorrectly based on the assumption that the Optec NGN-2 nephelometer measurements include the effects of precipitation. However, these instruments are programmed to shut down during rain events, and any data logged are in error. He further assumes that precipitation occurs as often on the haziest days as the clearest days and that precipitation light scattering (bprecip) is independent of geographic location and applied an average bprecip derived for Great Smoky Mountains to diverse locations including the Grand Canyon. Both of these assumptions are shown to be in error.  相似文献   

3.
Abstract

The goal of the Regional Haze Rule (RHR) is to return visibility in class I areas (CIAs) to natural levels, excluding weather-related events, by 2064. Whereas visibility, the seeing of scenic vistas, is a near instantaneous and sight-path-dependent phenomenon, reasonable progress toward the RHR goal is assessed by tracking the incremental changes in 5-yr average visibility. Visibility is assessed using a haze metric estimated from 24-hr average aerosol measurements that are made at one location representative of the CIA. It is assumed that, over the 5-yr average, the aerosol loadings and relative humidity along all of the site paths are the same and can be estimated from the 24-hr measurements. It is further assumed that any time a site path may be obscured by weather (e.g., clouds and precipitation), there are other site paths within the CIA that are not. Therefore, when calculating the haze metric, sampling days are not filtered for weather conditions. This assumption was tested by examining precipitation data from multiple monitors for four CIAs. It is shown that, in general, precipitation did not concurrently occur at all monitors for a CIA, and precipitation typically occurred 3-8 hr or less in a day. In a recent paper in this journal, Ryan asserts that the haze metric should include contributions from precipitation and conducted a quantitative assessment incorrectly based on the assumption that the Optec NGN-2 nephelometer measurements include the effects of precipitation. However, these instruments are programmed to shut down during rain events, and any data logged are in error. He further assumes that precipitation occurs as often on the haziest days as the clearest days and that precipitation light scattering (bprecip) is independent of geographic location and applied an average bprecip derived for Great Smoky Mountains to diverse locations including the Grand Canyon. Both of these assumptions are shown to be in error.  相似文献   

4.
The concentration of elements Na through Pb, select ions, and organic carbon from fine (<2.5 µm) particles has been monitored at Shenandoah and Great Smoky Mountains National Parks from 1988 through 1995. The data obtained from 1988 through 1994 show that significant changes in the concentrations of many aerosol constituents occur on a seasonal basis. Particulate sulfate and organic carbon are shown to exhibit substantially higher concentrations during the summer, while sulfur dioxide and nitrate concentrations are highest during the winter.

A method for estimating the degree of neutralization of particulate sulfate is given. This method uses routinely measured aerosol elemental compositions because ammonium ion, the primary neutralizing species for sulfate, is not measured on a routine basis. Application of this method to the selected data set shows that sulfate aerosol is most acidic during summer with an average molar Hs (moles of hydrogen associated with sulfur) to S (moles of sulfur) ratio of approximately 4. This suggests the average sulfate particle during the summer has a molar coon slightly more acidic than ammonium bisulfate (NH4HSO4) which has a molar hydrogen to sulfur ratio of 5. Winter Hs to S ratios, however, are approximately 8, suggesting the aerosol is on average fully neutralized ammonium sulfate [(NH4)2SO4].  相似文献   

5.
Ozone-sensitive and -tolerant individuals of cutleaf coneflower (Rudbeckia laciniata L.) were compared for their gas exchange characteristics and total non-structural carbohydrates at Purchase Knob, a high elevation site in Great Smoky Mountains National Park, USA. Photosynthesis and stomatal conductance decreased with increased foliar stipple. Sensitive plants had lower photosynthetic rates for all leaves, except the very youngest and oldest when compared to tolerant plants. Stomatal conductance decreased with increasing leaf age, but no ozone-sensitivity differences were found. Lower leaves had less starch than upper ones, while leaves on sensitive plants had less than those on tolerant plants. These results show that ambient levels of ozone in Great Smoky Mountains National Park can adversely affect gas exchange, water use efficiency and leaf starch content in sensitive coneflower plants. Persistence of sensitive genotypes in the Park may be due to physiological recovery in low ozone years.  相似文献   

6.
The hygroscopic properties of the organic fraction of aerosols are poorly understood. The ability of organic aerosols to absorb water as a function of relative humidity (RH) was examined using data collected during the 1999 Big Bend Regional Aerosol and Visibility Observational Study (BRAVO). (On average, organics accounted for 22% of fine particulate matter with an aerodynamic diameter less than 2.5 microm (PM2.5) mass). Hourly RH exceeded 80% only 3.5% of the time and averaged 44%. BRAVO aerosol chemical composition and dry particle size distributions were used to estimate PM2.5 light scattering (Bsp) at low and high ambient RH. Liquid water growth associated with inorganic species was sufficient to account for measured Bsp for RH between 70 and 95%.  相似文献   

7.
The ionic compositions of particulate matter with aerodynamic diameter < or = 2.5 microm (PM2.5) and size-resolved aerosol particles were measured in Big Bend National Park, Texas, during the 1999 Big Bend Regional Aerosol and Visibility Observational study. The ionic composition of PM2.5 aerosol was dominated by sulfate (SO4(2-)) and ammonium (NH4+). Daily average SO4(2-) and NH4+ concentrations were strongly correlated (R2 = 0.94). The molar ratio of NH4+ to SO4(2-) averaged 1.54, consistent with concurrent measurements of aerosol acidity. The aerosol was observed to be comprised of a submicron fine mode consisting primarily of ammoniated SO4(2-) and a coarse particle mode containing nitrate (NO3-). The NO3- appears to be primarily associated with sea salt particles where chloride has been replaced by NO3-, although formation of calcium nitrate (Ca(NO3)2) is important, too, on several days. Size-resolved aerosol composition results reveal that a size cut in particulate matter with aerodynamic diameter < or = 1 microm would have provided a much better separation of fine and coarse aerosol modes than the standard PM2.5 size cut utilized for the study. Although considerable nitric acid exists in the gas phase at Big Bend, the aerosol is sufficiently acidic and temperatures sufficiently high that even significant future reductions in PM2.5 SO4(2-) are unlikely to be offset by formation of particulate ammonium nitrate in summer or fall.  相似文献   

8.
Aerosol size distributions were measured during the summertime 1995 Southeastern Aerosol and Visibility Study (SEAVS) in Great Smoky Mountains National Park using an Active Scattering Aerosol Spectrometer (ASASP-X) optical particle counter. We present an overview of the experimental method, our data inversion technique, timelines of the size distribution parameters, and calculations of dry accumulation mode aerosol density and refractive index. Aerosol size distributions were recorded during daylight hours for aerosol in the size range 0.1 < Dp < 2.5 microns. The particle refractive index used for the data inversion was calculated with the partial molar refractive index approach using 12-hr measured aerosol chemical composition. Aerosol accumulation mode volume concentrations ranging from 1 to 26 micron 3 cm-3 were observed, with an average of 7 +/- 5 micron 3 cm-3. The study average dry accumulation mode geometric volume median diameter was 0.27 +/- 0.03 micron, and the mean geometric standard deviation was 1.45 +/- 0.06. Using an internally mixed aerosol model, and assuming chemical homogeneity across the measured particle distribution, an average accumulation mode dry sulfate ion mass scattering efficiency of 3.8 +/- 0.6 m2 g-1 was calculated.  相似文献   

9.
The recently completed Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study focused on particulate sulfate source attribution for a 4-month period from July through October 1999. A companion paper in this issue by Schichtel et al. describes the methods evaluation and results reconciliation of the BRAVO Study sulfate attribution approaches. This paper summarizes the BRAVO Study extinction budget assessment and interprets the attribution results in the context of annual and multiyear causes of haze by drawing on long-term aerosol monitoring data and regional transport climatology, as well as results from other investigations. Particulate sulfates, organic carbon, and coarse mass are responsible for most of the haze at Big Bend National Park, whereas fine particles composed of light-absorbing carbon, fine soils, and nitrates are relatively minor contributors. Spring and late summer through fall are the two periods of high-haze levels at Big Bend. Particulate sulfate and carbonaceous compounds contribute in a similar magnitude to the spring haze period, whereas sulfates are the primary cause of haze during the late summer and fall period. Atmospheric transport patterns to Big Bend vary throughout the year, resulting in a seasonal cycle of different upwind source regions contributing to its haze levels. Important sources and source regions for haze at Big Bend include biomass smoke from Mexico and Central America in the spring and African dust during the summer. Sources of sulfur dioxide (SO2) emissions in Mexico, Texas, and in the Eastern United States all contribute to Big Bend haze in varying amounts over different times of the year, with a higher contribution from Mexican sources in the spring and early summer, and a higher contribution from U.S. sources during late summer and fall. Some multiple-day haze episodes result from the influence of several source regions, whereas others are primarily because of emissions from a single source region.  相似文献   

10.
The Handix Scientific open-path cavity ringdown spectrometer (OPCRDS) was deployed during summer 2016 in Great Smoky Mountains National Park (GRSM). Extinction coefficients from the relatively new OPCRDS and from a more well-established extinction instrument agreed to within 7%. Aerosol hygroscopic growth (f(RH)) was calculated from the ratio of ambient extinction measured by the OPCRDS to dry extinction measured by a closed-path extinction monitor (Aerodyne’s cavity-attenuated phase shift particulate matter extinction monitor [CAPS PMex]). Derived hygroscopicity (relative humidity [RH] < 95%) from this campaign agreed with data from 1995 at the same site and time of year, which is noteworthy given the decreasing trend for organics and sulfate in the eastern United States. However, maximum f(RH) values in 1995 were less than half as large as those recorded in 2016—possibly due to nephelometer truncation losses in 1995. Two hygroscopicity parameterizations were investigated using high-time-resolution OPCRDS+CAPS PMex data, and the κext model was more accurate than the gamma model. Data from the two ambient optical instruments, the OPCRDS and the open-path nephelometer, generally agreed; however, significant discrepancies between ambient scattering and extinction were observed, apparently driven by a combination of hygroscopic growth effects, which tend to increase nephelometer truncation losses and decrease sensitivity to the wavelength difference between the two instruments as a function of particle size. There was not a statistically significant difference in the mean reconstructed extinction values obtained from the original and the revised IMPROVE (Interagency Monitoring of Protected Visual Environments) equations. On average, IMPROVE reconstructed extinction was ~25% lower than extinction measured by the OPCRDS, which suggests that the IMPROVE equations and 24-hr aerosol data are moderately successful in estimating current haze levels at GRSM. However, this conclusion is limited by the coarse temporal resolution and the low dynamic range of the IMPROVE reconstructed extinction.

Implications: Although light extinction, which is directly related to visibility, is not directly measured in U.S. National Parks, existing IMPROVE protocols can be used to accurately infer visibility for average humidity conditions, but during the large fraction of the year when humidity is above or below average, accuracy is reduced substantially. Furthermore, nephelometers, which are used to assess the accuracy of IMPROVE visibility estimates, may themselves be biased low when humidity is very high. Despite reductions in organic and sulfate particles since the 1990s, hygroscopicity, particles’ affinity for water, appears unchanged, although this conclusion is weakened by the previously mentioned nephelometer limitations.  相似文献   


11.
Abstract

The hygroscopic properties of the organic fraction of aerosols are poorly understood. The ability of organic aerosols to absorb water as a function of relative humidity (RH) was examined using data collected during the 1999 Big Bend Regional Aerosol and Visibility Observational Study (BRAVO). (On average, organics accounted for 22% of fine particulate matter with an aerodynamic diameter less than 2.5 µm (PM2.5) mass). Hourly RH exceeded 80% only 3.5% of the time and averaged 44%. BRAVO aerosol chemical composition and dry particle size distributions were used to estimate PM2.5 light scattering (Bsp) at low and high ambient RH. Liquid water growth associated with inorganic species was sufficient to account for measured Bsp for RH between 70 and 95%.  相似文献   

12.
Abstract

The U.S. Clean Air Act, amended in 1990, mandated the establishment of the Grand Canyon Visibility Transport Commission (GCVTC). The commission is required to submit a report to the U.S. Environmental Protection Agency addressing visibility issues in the region, including "the establishment of clean air corridors, in which additional restrictions on increases in emissions may be appropriate to protect visibility in affected Class I areas." This paper presents a methodology to identify candidate geographic areas for consideration for Clean Air Corridor (CAC) status for Colorado Plateau Class I areas. The methodology uses thousands of model determined trajectories over a five year period (1988 to 1992) to indicate the paths taken by air that arrives during clean air conditions at Class I areas. These clean air back-trajectories identify upwind areas where pollution emissions could jeopardize currently pristine visibility. Using this methodology, six candidate areas are identified, ranging in size from 75,000 to 506,000 square miles, and permitting varying levels of visibility protection for clean air days at Grand Canyon, Canyonlands, and Petrified Forest National Parks. Assuming effective emissions management of the CAC, the larger the CAC, the greater the visibility protection during clean air conditions.  相似文献   

13.
Improvements in measurement technology are permitting development of a more detailed scientific understanding of the cycling of mercury in the global atmospheric environment. Critical to advancing the state of knowledge is the acquisition of accurate measurement of speciated mercury (gaseous and particulate) at ground research stations in a variety of settings located around the globe. This paper describes one such research effort conducted at TVA's Look Rock air quality monitoring site in Tennessee—a mountain top site (813 m elevation) just west of the Great Smoky Mountains National Park. The Great Smoky Mountains National Park is the largest National Park in the eastern US and it receives environmental protection under a variety of US statutes. Gaseous and particle mercury species along with some additional trace gases were measured at Look Rock during two field studies totaling 84 days in the spring and summer of 2004. Average results for the entire sampling period are: gaseous elemental mercury Hg(0): 1.65 ng m−3, reactive gaseous mercury RGM: 0.005 ng m−3, particulate mercury Hg(p): 0.007 ng m−3. Literature review indicates that these levels are within the range found for other rural/remote sites in North America and worldwide. Reactive and particulate mercury comprised together less than 1%, on average, of total airborne mercury at Look Rock. When compared to the global background mercury literature, the Look Rock measurements demonstrate that the atmospheric mercury levels in the vicinity of the Great Smoky Mountains National Park are clearly dominated by the global atmospheric pool, not by local or regional sources.  相似文献   

14.
The risk of ozone injury to plants was assessed in support of the National Park Service's Vital Signs Monitoring Network program. The assessment examined bioindicator species, evaluated levels of ozone exposure, and investigated soil moisture conditions during periods of exposure for a 5-year period in each park. The assessment assigned each park a risk rating of high, moderate, or low. For the 244 parks for which assessments were conducted, the risk of foliar injury was high in 65 parks, moderate in 46 parks, and low in 131 parks. Among the well-known parks with a high risk of ozone injury are Gettysburg, Valley Forge, Delaware Water Gap, Cape Cod, Fire Island, Antietam, Harpers Ferry, Manassas, Wolf Trap Farm Park, Mammoth Cave, Shiloh, Sleeping Bear Dunes, Great Smoky Mountains, Joshua Tree, Sequoia and Kings Canyon, and Yosemite.  相似文献   

15.
The Big Bend Regional Aerosol and Visibility Observational (BRAVO) study was an intensive monitoring study from July through October 1999 followed by extensive assessments to determine the causes and sources of haze in Big Bend National Park, located in Southwestern Texas. Particulate sulfate compounds are the largest contributor of haze at Big Bend, and chemical transport models (CTMs) and receptor models were used to apportion the sulfate concentrations at Big Bend to North American source regions and the Carbón power plants, located 225 km southeast of Big Bend in Mexico. Initial source attribution methods had contributions that varied by a factor of > or =2. The evaluation and comparison of methods identified opposing biases between the CTMs and receptor models, indicating that the ensemble of results bounds the true source attribution results. The reconciliation of these differences led to the development of a hybrid receptor model merging the CTM results and air quality data, which allowed a nearly daily source apportionment of the sulfate at Big Bend during the BRAVO study. The best estimates from the reconciliation process resulted in sulfur dioxide (SO2) emissions from U.S. and Mexican sources contributing approximately 55% and 38%, respectively, of sulfate at Big Bend. The distribution among U.S. source regions was Texas, 16%; the Eastern United States, 30%; and the Western United States, 9%. The Carbón facilities contributed 19%, making them the largest single contributing facility. Sources in Mexico contributed to the sulfate at Big Bend on most days, whereas contributions from Texas and Eastern U.S. sources were episodic, with their largest contributions during Big Bend sulfate episodes. On the 20% of the days with the highest sulfate concentrations, U.S. and Mexican sources contributed approximately 71% and 26% of the sulfate, respectively. However, on the 20% of days with the lowest sulfate concentrations, Mexico contributed 48% compared with 40% for the United States.  相似文献   

16.
The southeastern aerosol and visibility study (SEAVS) was conducted in Great Smoky Mountains National Park in summer 1995 to investigate variations in ambient aerosol size distributions and their effect on visibility. In this paper, we compare dry aerosol size distribution parameters from a MOUDI impactor and two different optical particle counters (OPCs). Size distributions from the various instruments are expressed in a common measure of size, specifically, optical and aerodynamic diameters are converted to a dry, geometric diameter basis. Comparisons of the real part of particle refractive index obtained directly from light scattering measurements and inferred from aerosol composition measurements are also shown. Real refractive indices from direct measurements and those computed from measured fine aerosol chemical composition were generally within ±0.02. Maximum differences in estimated accumulation mode integrated volume concentrations from all instruments were within ∼22%. Accumulation mode integrated number concentrations and geometric standard deviations from the two OPCs agreed within ∼30% and ∼3%, respectively. Differences between MOUDI- and OPC-derived accumulation mode number concentrations and geometric standard deviations were ∼20% and ∼8%, respectively. The average geometric volume mean diameters derived from the three instruments agreed within 15% or less. The volume median diameters obtained by fitting the CSU number concentration data to a lognormal function were typically the smallest. We show that these discrepancies can be related to the differences and biases in the measurement and data analysis techniques.  相似文献   

17.
ABSTRACT

Aerosol water content was determined from relative humidity controlled optical particle counter (ASASP-X) size distribution measurements made during the Southeastern Aerosol and Visibility Study (SEAVS) in the Great Smoky Mountains National Park during summer 1995. Since the scattering response function of the ASASP-X is sensitive to particle refractive index, a technique for calibrating the ASASP-X for any real refractive index was developed. A new iterative process was employed to calculate water mass concentration and wet refractive index as functions of relative humidity. Experimental water mass concentrations were compared to theoretically predicted values assuming only ammonium sulfate compounds were hygroscopic. These comparisons agreed within experimental uncertainty. Estimates of particle hygroscopicity using a rural aerosol model of refractive index as a function of relative humidity demonstrated no significant differences from those made with daily varying refractive index estimates. Although aerosol size parameters were affected by the assumed chemical composition, forming ratios of these parameters nearly canceled these effects.  相似文献   

18.
Aerosol water content was determined from relative humidity controlled optical particle counter (ASASP-X) size distribution measurements made during the Southeastern Aerosol and Visibility Study (SEAVS) in the Great Smoky Mountains National Park during summer 1995. Since the scattering response function of the ASASP-X is sensitive to particle refractive index, a technique for calibrating the ASASP-X for any real refractive index was developed. A new iterative process was employed to calculate water mass concentration and wet refractive index as functions of relative humidity. Experimental water mass concentrations were compared to theoretically predicted values assuming only ammonium sulfate compounds were hygroscopic. These comparisons agreed within experimental uncertainty. Estimates of particle hygroscopicity using a rural aerosol model of refractive index as a function of relative humidity demonstrated no significant differences from those made with daily varying refractive index estimates. Although aerosol size parameters were affected by the assumed chemical composition, forming ratios of these parameters nearly canceled these effects.  相似文献   

19.
The Mohave Power Project (MPP) is an isolated 1580-MW coal-fired electric generating plant located in Laughlin, NV. Laughlin is a small desert gambling town situated in the lower Colorado River Valley near the junction of three states: Nevada, California, and Arizona. The location of the MPP is approximately 115 km southwest of the western end of the Grand Canyon National Park and about 240 km southwest from the Grand Canyon Village. This paper describes the summer transport patterns of the MPP emittants using illustrated examples from the Project MOHAVE (Measurements of Haze and Visual Effects) 1992 summer intensive study. The intensive study lasted 50 days from mid-July through August and encompassed the major meteorological patterns associated with southwestern U.S. summer meteorology. The MPP emittants were transported toward the Grand Canyon (north to the northeast) during more than 80% of the total hours. Airflow was from the south most of the time due to a combination of the semi-permanent thermal low, differential heating between the Gulf of California and lower Colorado River Valley, and upslope heating of the southern and western slopes of the nearby Colorado Plateau.  相似文献   

20.
The goals of this study were to document the development of ozone-induced foliar injury, on a leaf-by-leaf basis, and to develop ozone exposure relationships for leaf cohorts and individual tall milkweeds (Asclepias exaltata L.) in Great Smoky Mountains National Park. Plants were classified as either ozone-sensitive or insensitive based on the amount of foliar injury. Sensitive plants developed injury earlier in the season and to a greater extent than insensitive plants. Older leaf cohorts were more likely to belong to high injury classes by the end of each of the two growing seasons. In addition, leaf loss was more likely for older cohorts (2000) and lower leaf positions (2001) than younger cohorts and upper leaves, respectively. Most leaves abscised without prior ozone-like stippling or chlorosis. Failure to take this into account can result in underestimation of the effects of ozone on these plants.  相似文献   

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