Numerical Investigation of the Effects of Boundary-Layer Evolution on the Predictions of Ozone and the Efficacy of Emission Control Options in the Northeastern United States

This paper examines the effects of two different planetary boundary-layer (PBL) parameterization schemes – Blackadar and Gayno–Seaman – on the predicted ozone (O₃) concentration fields using the MM5 (Version 3.3) meteorological model and the MODELS-3 photochemical model. The meteorological fields obtained from the two boundary-layer schemes have been used to drive the photochemical model to simulate O₃ concentrations in the northeastern United States for a three-day O₃ episodic period. In addition to large differences in the predicted O₃ levels at individual grid cells, the simulated daily maximum 1-h O₃ concentrations appear at different regions of the modeling domain in these simulations, due to the differences in the vertical exchange formulations in these two PBL schemes. Using process analysis, we compared the differences between the different simulations in terms of the relative importance of chemical and physical processes to O₃ formation and destruction over the diurnal cycle. Finally, examination of the photochemical model's response to reductions in emissions reveals that the choice of equally valid boundary-layer parameterizations can significantly influence the efficacy of emission control strategies.     

A Large-Eddy Simulation Study of the Convective Boundary Layer over Philadelphia during the 1999 Summer NE-OPS Campaign

This study presents a large-eddy simulation (LES) study of the convective boundary layer on August 1, 1999 over Philadelphia, PA during a summer ozone episode. The study is an evaluation of the Colorado State University's Regional Atmospheric Modeling System Version 4.3 (RAMS4.3) with the LES option using Northeast Oxidant and Particulate Study (NE-OPS) data. Simulations were performed with different imposed sensible heat fluxes at the ground surface. The model was initialized with the atmospheric sounding data collected at Philadelphia at 1230 UTC and model integrations continued till 2130 UTC. The resulting mean profiles of temperature and humidity obtained from the LES model were compared with atmospheric soundings, tethered balloon and aircraft data collected during the NE-OPS 1999 field campaign. Also the model-derived vertical profiles of virtual temperature were compared with NE-OPS Radio Acoustic Sounder System (RASS) data while the humidity profiles were compared with NE-OPS lidar data. The comparison of the radiosonde data with the LES model predictions suggests that the growth of the mixing layer is reasonably well simulated by the model. Overall, the agreement of temperature predictions of the LES model with the radiosonde observations is good. The model appears to underestimate humidity values for the case of higher imposed sensible heat flux. However, the humidity values in the mixing layer agree quite well with radiosonde observations for the case of lower imposed sensible heat flux. The model-predicted temperature and humidity profiles are in reasonable agreement with the tethered balloon data except for some small overestimation of temperature at lower layers and some underestimation of humidity values. However, the humidity profiles as simulated by the model agree quite well with the tethered balloon data for the case of lower imposed sensible heat flux. The model-predicted virtual temperature profile is also in better agreement with RASS data for the case of lower imposed sensible heat flux. The model-predicted temperature profile further agrees quite well with aircraft data for the case of lower imposed heat flux. However, the relative humidity values predicted by the model are lower compared with the aircraft data. The model-predicted humidity profiles are only in partial agreement with the lidar data. The results of this study suggest that the explicitly resolved energetic eddies seem to provide the correct forcing necessary to produce good agreement with observations for the case of an imposed sensible heat flux of 0.1 K m s^–1 at the surface.     

Determination of levoglucosan in atmospheric fine particulate matter

A microanalytical method suitable for the quantitative determination of the sugar anhydride levoglucosan in low-volume samples of atmospheric fine particulate matter (PM) has been developed and validated. The method incorporates two sugar anhydrides as quality control standards. The recovery standard sedoheptulosan (2,7-anhydro-beta-D-altro-heptulopyranose) in 20 microL solvent is added onto samples of the atmospheric fine PM and aged for 1 hr before ultrasonic extraction with ethylacetate/ triethylamine. The extract is reduced in volume, an internal standard is added (1,5-anhydro-D-mannitol), and a portion of the extract is derivatized with 10% by volume N-trimethylsilylimidazole. The derivatized extract is analyzed by gas chromatography/mass spectrometry (GC/MS). The recovery of levoglucosan using this procedure was 69 +/- 6% from five filters amended with 2 microg levoglucosan, and the reproducibility of the assay is 9%. The limit of detection is approximately 0.1 microg/mL, which is equivalent to approximately 3.5 ng/m3 for a 10 L/min sampler or approximately 8.7 ng/m3 for a 4 L/min personal sampler (assuming 24-hr integrated samples). We demonstrated that levoglucosan concentrations in collocated samples (expressed as ng/m3) were identical irrespective of whether samples were collected by PM with aerodynamic diameter < or = 2.5 microm or PM with aerodynamic diameter < or = 10 microm impactors. It was also demonstrated that X-ray fluorescence analysis of samples of atmospheric PM, before levoglucosan determinations, did not alter the levels of levoglucosan.     

Modelling trends in woody vegetation structure in semi-arid Australia as determined from aerial photography

Accounting of carbon stocks in woody vegetation for greenhouse purposes requires definition of medium term trends with accurate error assessment. Tree and shrub cover was sampled through time at randomly located sites over a large area of central Queensland, Australia using aerial photography from 1945 to 1999. Calibration models developed from field data for the same land types as those represented within the study area allowed for the extrapolation of overstorey and understorey cover, basal area and biomass values and these were modelled as trends over the latter half of the 20th century. These structural attributes have declined over the region because of land clearing with values for biomass changing from a mean of 58.0(+/-1.2)t/ha in 1953 to 41.1(+/-1.0)t/ha in 1991. The biomass of Acacia on clay and Eucalypt on texture contrast soils land types has declined most dramatically. Within uncleared vegetation there was an overall trend of increase from 56.1(+/-1.2)t/ha in 1951 to 67.6(+/-1.3)t/ha in 1995. The increase in structural attributes within uncleared vegetation was most pronounced for the Eucalypt on texture contrast soils and Eucalypt on clay land types. It was demonstrated that the sites sampled were representative of their land types and that spatial bias of the photography, undetected tree-killing, sampling error, inherent variability of structural attributes and measurement error should not have impacted greatly on bias or precision of trend estimates for well-sampled land types. Certainly the errors are not likely to be substantial for trends averaged over all land types and they provide an accurate assessment of the magnitude and direction of change. The technique presented here would appear to be a robust means of accounting for the above-ground woody component of woodlands and open forests and will also contribute to a broader understanding of savanna dynamics.     

Nitrogen dynamics among cropland and riparian buffers: soil-landscape influences

Nitrate (NO3-) leaching to ground water poses water quality concerns in some settings. Riparian buffers have been advocated to reduce excess ground water NO3- concentrations. We characterized inorganic N in soil solution and shallow ground water for 16 paired cropland-riparian plots from 2003 to 2005. The sites were located at two private dairy farms in Central New York on silt and gravelly silt loam soils (Aeric Endoaqualfs, Fluvaquentic Endoaquepts, Fluvaquentic Eutrudepts, Glossaquic Hapludalfs, and Glossic Hapludalfs). It was hypothesized that cropland N inputs and soil-landscape variability would jointly affect NO3- leaching and transformations in ground water. Results showed that well and moderately well drained fields had consistently higher ground water NO3- compared to more imperfectly drained fields receiving comparable N inputs. Average 50-cm depth soil solution NO3- and ground water dissolved oxygen (DO) explained 64% of average cropland ground water NO3- variability. Cropland ground water with an average DO of <3 mg L(-1) tended to have <4 mg L(-1) of NO3- with a water table depth (WTD) of 相似文献   

Evaluation of aerial photography for predicting trends in structural attributes of Australian woodland including comparison with ground-based monitoring data

The accurate assessment of trends in the woody structure of savannas has important implications for greenhouse accounting and land-use industries such as pastoralism. Two recent assessments of live woody biomass change from north-east Australian eucalypt woodland between the 1980s and 1990s present divergent results. The first estimate is derived from a network of permanent monitoring plots and the second from woody cover assessments from aerial photography. The differences between the studies are reviewed and include sample density, spatial scale and design. Further analyses targeting potential biases in the indirect aerial photography technique are conducted including a comparison of basal area estimates derived from 28 permanent monitoring sites with basal area estimates derived by the aerial photography technique. It is concluded that the effect of photo-scale; or the failure to include appropriate back-transformation of biomass estimates in the aerial photography study are not likely to have contributed significantly to the discrepancy. However, temporal changes in the structure of woodlands, for example, woodlands maturing from many smaller trees to fewer larger trees or seasonal changes, which affect the relationship between cover and basal area could impact on the detection of trends using the aerial photography technique. It is also possible that issues concerning photo-quality may bias assessments through time, and that the limited sample of the permanent monitoring network may inadequately represent change at regional scales.     

The Akoya pearl oyster shell as an archival monitor of lead exposure

The Akoya pearl oyster (Pinctada imbricata) was experimentally exposed to (a) constant levels of lead (Pb) at 180 microg L(-1) for nine weeks, or (b) two short term (pulse) exposures of Pb at 180 microg L(-1) (three weeks each) with an intervening depuration period (three weeks), to assess its utility as an (i) accumulative monitor of Pb contamination and an (ii) archival monitor for discriminating constant versus pulsed Pb exposure events. P. imbricata showed similar reductions in growth (based on shell morphology and wet weight) and Pb accumulation patterns for whole tissue and shell in response to both Pb exposure regimes. Thus the whole oyster was deemed an inappropriate accumulative monitor for assessing short-term temporal variation of Pb exposure and effect. However, using secondary ion mass spectrometry, Pb was shown to accumulate in the successively deposited nacreous layers of the shell of P. imbricata, documenting the exposure history of constant versus pulsed Pb events. Patterns of Pb deposition not only reflected the frequency of Pb exposure events but also their relative durations. Thus, the shell of P. imbricata may be employed as a suitable biological archive of Pb exposure.     

Air quality measurements for the aerosol research and inhalation epidemiology study

Measurements of pollutant gases, airborne particulate matter mass and composition, and meteorology have been made at a core site near downtown Atlanta, GA, since August 1998 in support of the Aerosol Research and Inhalation Epidemiology Study (ARIES). This site is one of eight in the Southeastern Aerosol Research and Characterization network. The measurement objective is to provide a long-term, multivariate dataset suitable for investigating statistical associations of respiratory and cardiovascular disease with airborne particulate matter composition, meteorology, and copollutant gases through epidemiologic modeling. Measurements are expected to continue through 2010. Ancillary multiyear measurements at additional sites in the Atlanta metropolitan area and in short-term exposure assessments have been used to estimate the exposure/measurement error associated with using data from a central site to approximate human exposures for the entire area. To date, 13-, 25-, and 53-month air quality datasets have been used in epidemiologic analyses.     

Effects of instrument precision and spatial variability on the assessment of the temporal variation of ambient air pollution in Atlanta, Georgia

Data from the U.S. Environmental Protection Agency Air Quality System, the Southeastern Aerosol Research and Characterization database, and the Assessment of Spatial Aerosol Composition in Atlanta database for 1999 through 2002 have been used to characterize error associated with instrument precision and spatial variability on the assessment of the temporal variation of ambient air pollution in Atlanta, GA. These data are being used in time series epidemiologic studies in which associations of acute respiratory and cardiovascular health outcomes and daily ambient air pollutant levels are assessed. Modified semivariograms are used to quantify the effects of instrument precision and spatial variability on the assessment of daily metrics of ambient gaseous pollutants (SO2, CO, NOx, and O3) and fine particulate matter ([PM2.5] PM2.5 mass, sulfate, nitrate, ammonium, elemental carbon [EC], and organic carbon [OC]). Variation because of instrument imprecision represented 7-40% of the temporal variation in the daily pollutant measures and was largest for the PM2.5 EC and OC. Spatial variability was greatest for primary pollutants (SO2, CO, NOx, and EC). Population-weighted variation in daily ambient air pollutant levels because of both instrument imprecision and spatial variability ranged from 20% of the temporal variation for O3 to 70% of the temporal variation for SO2 and EC. Wind     

An assessment of persistent organic pollutants in Scottish coastal and offshore marine environments

Concentrations of persistent organic pollutants (POPs), including polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) were determined in sediment and biota (fish liver) from around Scotland. The concentrations were investigated using assessment criteria developed by OSPAR and ICES. Organic contaminant concentrations, PAHs, PCBs and PBDEs in sediment, and PCBs and PBDEs in fish liver, were significantly higher in the Clyde compared to all other sea areas. This is mainly due to historic industrial inputs. Highest PCB and PAH concentrations were found in the strata furthest up the Clyde estuary, with concentrations of POPs in these strata being at levels such that there is an unacceptable risk of chronic effects occurring in marine species. Furthermore, for PAHs in Clyde sediment there was a significant negative gradient going from north to south towards the open sea. PAH and PCB concentrations in sediment and biota in all other Scottish sea areas (except for PCBs in sediment from East Scotland) were unlikely to give rise to pollution effects, being below relevant assessment criteria. Although no assessment criteria are available for PBDEs, the concentrations observed in Scottish sediments were low with all congeners below the limit of detection (LoD; 0.03 μg kg(-1) dry weight) in 140 out of a total of 307 samples analysed. Where PBDEs were detected, the dominant congeners were BDE47 and BDE99. PBDEs were detected in fish livers, although concentrations were less than 150 μg kg(-1) lipid weight in all sea areas except the Clyde where concentrations ranged between 8.9 and 2202 μg kg(-1) lipid weight. Few trends were detected in contaminant concentrations in biota or sediment at any Scottish site with more than five years data. Downward trends were detected in PAHs in sediment from the Clyde, Irish Sea and Minches and Malin Sea and PCBs in fish liver from the Moray Firth. Rules were developed for the aggregation of the contaminant data across a sea area. An overall assessment for each sea area was then assigned, looking at the frequency of sites or strata within each sea area that were above or below the relevant assessment criteria. Overall the status of the various sea areas, with respect to the assessed POPs, can be considered to be acceptable in that they were below concentrations likely to result in chronic effects for all sea areas except the Clyde.