Large-Scale Weather Influences on Community Air Pollution Potential in the United States

This paper describes the large-scale weather features that typically are associated with relatively rapid and slow atmospheric dispersion. Specific examples for some well-known air pollution incidents are illustrated and discussed. Particular attention is paid to the features of quasi-stagnating anticyclones, the typical weather system associated with persistent and extensive areas of sluggish dispersion. On the large scale, the basic quantitative parameters of dispersion over urban areas are the mixing height and the wind speed averaged through that height. These parameters are defined and discussed. Mean morning and afternoon mixing heights and wind speeds are presented for four locations across the United States, illustrating their diurnal, seasonal, and spatial variations. Also for these four locations, data are given on the climatological occurrence of periods during which critical values of the basic parameters were not exceeded. The spatial distributions of mixing heights and average wind speeds during a well-documented air pollution episode are presented.     

Prediction of overall persistence and long-range transport potential with multimedia fate models: robustness and sensitivity of results

The hazard indicators persistence (P) and long-range transport potential (LRTP) are used in chemicals assessment to characterize chemicals with regard to the temporal and spatial extent of their environmental exposure. They are often calculated based on the results of multimedia fate models. The environmental and substance-specific input parameters of such models are subject to a range of methodological uncertainties and also influenced by natural variability. We employed probabilistic uncertainty analysis to quantify variance in P and LRTP predictions for chemicals with different partitioning and transport behavior. Variance found in the results is so large that it prevents a clear distinction between chemicals. Additionally, only small improvements are observed when evaluating the results relative to a benchmark chemical. This can be explained by the dominance of substance-specific parameters and the only small direct influence of environmental parameters on P and LRTP as model outcomes. The findings underline the importance of learning how environmental conditions cause variability in substance behavior for improved substance ranking and classification.     

Vertical transport of ozone and CO during super cyclones in the Bay of Bengal as detected by Tropospheric Emission Spectrometer

Vertical profiles of carbon monoxide (CO) and ozone retrieved from Tropospheric Emission Spectrometer have been analyzed during two super cyclone systems Mala and Sidr. Super cyclones Mala and Sidr traversed the Bay of Bengal (BOB) region on April 24–29, 2006 and November 12–16, 2007 respectively. The CO and ozone plume is observed as a strong enhancement of these pollutants in the upper troposphere over the BOB, indicating deep convective transport. Longitude–height cross-section of these pollutants shows vertical transport to the upper troposphere. CO mixing ratio ~90 ppb is observed near the 146-mb level during the cyclone Mala and near 316 mb during the cyclone Sidr. Ozone mixing ratio ~60–100 ppb is observed near the 316-mb level during both the cyclones. Analysis of National Centers for Environmental Prediction (NCEP) reanalysis vertical winds (omega) confirms vertical transport in the BOB.     

Modeling short-term variability of semivolatile organic chemicals in air at a local scale: an integrated modeling approach

Monitoring campaigns from different locations have recently shown how air concentrations of persistent semivolatile contaminants such as polychlorinated biphenyls (PCBs) often exhibit short-term (less than 24 h) variations. The observed patterns have been ascribed to different factors, such as temperature-mediated air-surface exchange and variability of planetary boundary layer (PBL) height and dynamics. Here, we present a new modeling approach developed in order to investigate the short-term variability in air concentrations of organic pollutants at a local scale. A new dynamic multimedia box model is supplied by a meteorological preprocessor (AERMET) with hourly values of air compartment height and wind speed. The resulting model is tested against an existing dataset of PCB air concentrations measured in Zurich, Switzerland. Results show the importance of such modeling approach in elucidating the short- and long-term behavior of semivolatile contaminants in the air/soil system.     

Atmospheric fate of non-volatile and ionizable compounds

A modified version of the Multimedia Activity Model for Ionics MAMI, including two-layered atmosphere, air-water interface partitioning, intermittent rainfall and variable cloud coverage was developed to simulate the atmospheric fate of ten low volatility or ionizable organic chemicals. Probabilistic simulations describing the uncertainty of substance and environmental input properties were run to evaluate the impact of atmospheric parameters, ionization and air-water (or air-ice) interface enrichment.The rate of degradation and the concentration of OH radicals, the duration of dry and wet periods, and the parameters describing air-water partitioning (K_AW and temperature) and ionization (pK_a and pH) are the key parameters determining the potential for long range transport. Wet deposition is an important removal process, but its efficiency is limited, primarily by the duration of the dry period between precipitation events.Given the underlying model assumptions, the presence of clouds contributes to the higher persistence in the troposphere because of the capacity of cloud water to accumulate and transport non-volatile (e.g. 2,4-D) and surface-active chemicals (e.g. PFOA). This limits the efficiency of wet deposition from the troposphere enhancing long-range transport.     

Behavior of particulate matter during high concentration episodes in Seoul

The behavior of particulate matter (PM) during high-concentration episodes was investigated using monitoring data from Guui station, a comprehensive air monitoring station in Seoul, Korea, from January 2008 to March 2010. Five non-Asian dust (ND) episodes and two Asian dust (AD) episodes of high PM concentrations were selected for the study. During the ND episode, primary air pollutants accumulated due to low wind speeds, and PM_2.5 increased along with most other air pollutants. Particles larger than PM_2.5 were also high since these particles were generated by vehicular traffic rather than wind erosion. During strong AD episodes, PM_10–2.5 primarily increased and gaseous primary air pollutants decreased under high wind speeds. However, even during the AD episode, PM_2.5 and gaseous primary air pollutants increased when the effects of AD were weak and wind speeds were low. This study corroborates that accumulation of air pollutants due to a drop in surface wind speed plays an important role in short-term high-concentration occurrences. However, low wind speeds could not be directly linked to local emissions because a significant portion of accumulated air pollutants resulted from long-range transport.     

Vertical distributions of aerosols under different weather conditions: Analysis of in-situ aircraft measurements in Beijing,China

In this study, aerosol vertical distributions of 17 in-situ aircraft measurements during 2005 and 2006 springs are analyzed. The 17 flights are carefully selected to exclude dust events, and the analyses are focused on the vertical distributions of aerosol particles associated with anthropogenic activities. The results show that the vertical distributions of aerosol particles are strongly affected by weather and meteorological conditions, and 3 different types of aerosol vertical distributions corresponding to different weather systems are defined in this study. The measurement with a flat vertical gradient and low surface aerosol concentrations is defined as type-1; a gradual decrease of aerosols with altitudes and modest surface aerosol concentrations is defined as type-2; a sharp vertical gradient (aerosols being strongly depressed in the PBL) with high surface aerosol concentrations is defined as type-3. The weather conditions corresponding to the 3 different aerosol types are high pressure, between two high pressures, and low pressure systems (frontal inversions), respectively. The vertical mixing and horizontal transport for the 3 different vertical distributions are analyzed. Under the type-1 condition, the vertical mixing and horizontal transport were rapid, leading to strong dilution of aerosols in both vertical and horizontal directions. As a result, the aerosol concentrations in PBL (planetary boundary layer) were very low, and the vertical distribution was flat. Under the type-2 condition, the vertical mixing was strong and there was no strong barrier at the PBL height. The horizontal transport (wind flux) was modest. As a result, the aerosol concentrations were gradually reduced with altitude, with modest surface aerosol concentrations. Under the type-3 condition, there was a cold front near the region. As a result, a frontal inversion associated with weak vertical mixing appeared at the top of the inversion layer, forming a very strong barrier to prevent aerosol particles being exchanged from the PBL height to the free troposphere. As a result, the aerosol particles were strongly depressed in the PBL height, producing high surface aerosol concentrations. The measured vertical aerosol distributions have important implications for studying the effects of aerosols on photochemistry. The J[O₃] values are reduced by 11%, 48%, and 50%, under the type-1, type-2, and type-3 conditions, respectively. This result reveals that atmospheric oxidant capacity (OH concentrations) is modestly reduced under the type-1 condition, but is significantly reduced under the type-2 and type-3 conditions. This result also suggests that the effect of aerosol particles on surface solar flux is an integrated column effect, and detailed vertical distributions of aerosol particles are very important for assessing the impacts of aerosol on photochemistry.     

Identification of substances with potential for long-range transport as possible substances of very high concern

According to the European legislation, REACH, organic compounds are considered as substances of very high concern (SVHC) if they are persistent, bioaccumulative and toxic (PBT). A substance's long-range transport potential (LRTP) may also pose a risk to remote regions. This is, however, not yet explicitly included. For identification of compounds, which are not PBT according to REACH criteria, but show LRTP, we investigated 22,438 compounds from the Canadian Domestic Substance List (CDSL). The CDSL was searched for organic, neutral compounds. Substance properties were estimated with EPI Suite v4.00. Next, the substance list was edited in two ways: (1) The half-life criterion in air for LRTP as defined in the Stockholm Convention was applied. (2) For all compounds, indicators for persistence and LRTP were calculated with the multimedia model ELPOS v2.2. Applying the half-life criterion, we identified 594 substances, which are prone to LRT but are not PBT (non-PBT-L substances). In contrast, investigations with ELPOS lead to a shorter list of 188 substances, which are non-PBT-L substances. Finally, the list was compared with potential Arctic contaminants identified in previous literature. Our results show that there is a large number of organic chemicals which would not be considered as SVHC since they are not, at the same time, persistent, bioaccumulative and toxic according to REACH criteria. Nevertheless, they show LRTP according to different screening approaches and thus a potential hazard to remote regions.     

Evaluation of weather conditions for methyl bromide ambient air monitoring in Monterey, Santa Cruz, and Kern Counties in the year 2000

Weather condition is one of the most important factors affecting spatial and temporal distributions of air pollutants, especially for short-term air dispersion. Abnormal weather conditions might lead to higher or lower ambient air concentrations than they would be under normal weather conditions. Therefore, testing for normality of weather conditions during the air monitoring period is an essential step for evaluating ambient air monitoring results. In this paper, a distance method was used to select a most representative weather station from the available candidates. An array of meteorological elements were identified that affect air dispersion and transportation. A statistical method was used to determine whether the weather conditions during the air monitoring period were significantly different from that of previous years. Using methyl bromide ambient air monitoring as a case study, this paper documents the methods, procedures, and results of weather analysis for Monterey, Santa Cruz, and Kern Counties during ambient air monitoring periods for methyl bromide in the year 2000. With a few exceptions, the meteorological elements and atmospheric stability factors, such as wind speeds, wind directions, and stability classes, during the monitoring period were in the normal range. Although there were higher frequencies of stable atmospheric conditions in Monterey/Santa Cruz Counties than in Kern County, weather conditions during the monitoring period were not significantly different from normal local weather conditions of previous years. Consequently, the subchronic air concentrations observed during the ambient air monitoring periods for methyl bromide in the year 2000 was taken under typical weather conditions of those areas at that time of the year.     

Seasonal variation of the structure of the atmospheric boundary layer over a Suburban area

The long-term observational data of wind and temperature obtained from a 213-m instrumented tower in a suburban area were analyzed to investigate the seasonal variation of the structure of the atmospheric boundary layer.It was found from the daily variations of wind and temperature and the seasonal variation of the power spectrum of wind that in the summer the atmospheric boundary layer below 200 m is well mixed by convective turbulence, but in the winter the inversion layer near the ground suppresses the turbulent mixing, and the diurnal variation caused by turbulent mixing is confined to below 50–100 m height.Power spectra of wind speed were computed for different seasons of the year. In the summer season there is no significant variation of the shape of the spectrum with height. However, in winter the spectrum varies with height. The spectrum also varies annually and the characteristic of the long period (a few days) spectral peak of wind is related closely to the synoptic weather situation, and this suggests the possibility of a spectrum climatology.     

On the use of the synoptic vertical wind component in a transport trajectory model

The study of the transport of polluted air masses has acquired great importance in the last years and as a consequence computed air mass trajectories are now currently associated with the analysis of atmospheric samples. Schematically, we can say that the pollution emitted in the boundary layer is partly transported within the boundary layer itself and partly within the free troposphere. By the latter route pollution can travel long distances. The main problem is now how to simulate the transport of pollutants when such a statification of the air is considered. Different techniques have been used to model the long-range transport of air masses (geostrophic, isobaric, isentropic trajectories…), but, presently, none can give a complete and satisfying response to the problem. The purpose of this study is to explore the use of the analyzed vertical wind component as a tool to compute air mass trajectories in five case studies. This parameter, resulting from the mass balance, is available from the data set of the European Center of Meteorological Weather Forecasts (ECMWF, Reading, U.K.). We shall discuss in which cases the computed trajectory is sensitive to this parameter. Our study suggests that this parameter should be used to compute air mass transport within the free troposphere.     

Monitoring of ozone in a marine environment in Tenerife (Canary Islands)

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.     

Polycyclic aromatic hydrocarbon and nitroarene concentrations in ambient air during a wintertime high-NOx episode in the Los Angeles basin

The ambient concentrations of polycyclic aromatic hydrocarbons (PAH) (including biphenyl) and nitroarenes were measured during a wintertime, high-NO_x episode at a location in Southern California. Daytime and night-time ambient air samples were collected using Hi-vol filters, polyurethane foam (PUF) plugs and Tenax-GC solid adsorbent. 2-Nitrofluoranthene was the most abundant particle-associated nitroarene, but higher concentrations of 1- and 2-nitronaphthalene, methylnitronaphthalenes and 3-nitrobiphenyl were observed on the PUF plugs. Our data show that the ambient concentrations of the more volatile PAH and nitroarenes can be far greater than those of the less volatile species, and suggest that the most abundant nitroarenes in ambient air arise from atmospheric transformations of PAH emitted from combustion sources.     

Effects of the density of meteorological observations on the diagnostic wind fields and the performance of photochemical modeling in the greater Seoul area

The high ozone episode in the greater Seoul area (GSA) for the period of 27 July–1 August 1997 was modeled by the California Institute of Technology (CIT) three-dimensional photochemical model. During the period, ozone concentrations around 140 ppb were observed for 2 days. Two sets of diagnostic wind fields were constructed by using observations from the weather stations operated by the Korea Meteorological Administration. One set of wind fields utilized only observations from the surface weather stations (SWS) and the other set also utilized observations from the automatic weather stations (AWS) that were more densely distributed than the SWS. The results showed that utilizing observations from the AWS could represent fine variations in the wind field such as those caused by topography. A better wind field gave a more reasonable spatial distribution of ozone concentrations. The model performance of ozone prediction was also improved to some extent, but only marginally acceptable owing to large day-to-day variations. Overshoots of primary pollutants particularly for NO₂ were observed as pollutants were accumulated where low wind speeds were maintained. More precise information on diurnal and daily variations in emissions was warranted in order to better model the photochemical phenomena over the GSA.     

Indicators for persistence and long-range transport potential as derived from multicompartment chemistry-transport modelling

Total environmental and compartmental residence times as a measure for persistence as well as indicators for long-range transport potential (LRTP) have been derived from global geo-referenced modelling and LRTP is characterized in two geographic directions for the first time. A dynamic multicompartment chemistry-transport model (MCTM) was used to study the fate of the insecticides DDT and alpha-hexachlorocyclohexane (alpha-HCH) during the first 2 years upon entry. The indicators for LRTP were defined such as to address the tendencies of substance distributions to migrate ('plume displacement', PD) and to spread into remote areas ('spatial spreading', SS). The indicators deliver values as function of time upon entry. With the aim to address the effect of location of entry on environmental fate, scenarios of emission from the territories of seven countries were studied. It was found that the effect of location of entry on the spatial scale of countries (400-4000 km) is significant for the compartmental distribution and the inter-compartmental mass exchange fluxes (e.g., number of atmospheric cycles, 'hops'). Location of entry introduces uncertainties in the order of a factor of 5 for the total environmental residence time, tau(overall), and a factor of 5-20 for PD and SS. For the 2nd year upon entry into the environment, tau(overall)=317-1527 days are predicted for DDT and 101-463 days for alpha-HCH. The influence of location of entry does affect the substance ranking, i.e. we cannot simply state that DDT is more persistent than alpha-HCH, but for one scenario studied, application in China, the opposite is predicted. Precipitation patterns proved to be significant, besides other climate parameters, for atmospheric residence time. Integration of the location of entry in chemicals risk assessments is therefore recommended. In general, persistence and some indicators for LRTP, pertinent to their definition, refer to the fate of a large fraction, e.g., 63% (=1-1/e) or 90%, but not the total substance burden. The choice of this fraction may have the consequence of a normative step which defines the spatial and temporal extensions of a related chemicals risk assessment and may affect substance ranking.     

Long-range transport and global fractionation of POPs: insights from multimedia modeling studies

The long-range transport of persistent organic pollutants (POPs) is investigated with two multimedia box models of the global system. ChemRange is a purely evaluative, one-dimensional steady-state (level III) model; CliMoChem is a two-dimensional model with different temperatures, land/water ratios and vegetation types in different latitudinal zones. Model results are presented for three case studies: (i) the effect of atmospheric aerosol particles on the long-range transport of POPs, (ii) the effect of oceanic deposition on the long-range transport of different PCB congeners, (iii) the global fractionation of different PCB congeners. The model results for these case studies show: (i) the low atmospheric half-lives estimated for several organochlorine pesticides are likely to be inconsistent with the observed long-range transport of these compounds; (ii) export to the deep sea reduces the potential for long-range transport of highly hydrophobic compounds (but does not remove these chemicals from the biosphere); (iii) there are different meanings of the term global fractionation that refer to different aspects of the fractionation process and need to be distinguished. The case-study results further indicate that the influences of varying environmental conditions on the physicochemical properties and the degradation rate constants of POPs need to be determined.     

Transport and dispersion during wintertime particulate matter episodes in the San Joaquin Valley, California

Data analysis and modeling were performed to characterize the spatial and temporal variability of wintertime transport and dispersion processes and the impact of these processes on particulate matter (PM) concentrations in the California San Joaquin Valley (SJV). Radar wind profiler (RWP) and radio acoustic sounding system (RASS) data collected from 18 sites throughout Central California were used to estimate hourly mixing heights for a 3-month period and to create case studies of high-resolution diagnostic wind fields, which were used for trajectory and dispersion analyses. Data analyses show that PM episodes were characterized by an upper-level ridge of high pressure that generally produced light winds through the entire depth of the atmospheric boundary layer and low mixing heights compared with nonepisode days. Peak daytime mixing heights during episodes were -400 m above ground level (agl) compared with -800 m agl during nonepisodes. These episode/nonepisode differences were observed throughout the SJV. Dispersion modeling indicates that the range of influence of primary PM emitted in major population centers within the SJV ranged from -15 to 50 km. Trajectory analyses revealed that little intrabasin pollutant transport occurred among major population centers in the SJV; however, interbasin transport from the northern SJV and Sacramento regions into the San Francisco Bay Area (SFBA) was often observed. In addition, this analysis demonstrates the usefulness of integrating RWP/RASS measurements into data analyses and modeling to improve the understanding of meteorological processes that impact pollution, such as aloft transport and boundary layer evolution.     

Intercomparison of nocturnal mixing height estimate methods for urban air pollution modelling

One of the most important meteorological input parameters for three-dimensional photochemical air pollution models is the mixing height h, which has a strong influence on the shape and intensity of the vertical diffusivity K_z and, as a consequence, on ground-level air concentrations of primary and secondary pollutants. A number of indirect algorithms for the estimate of h in nocturnal, stable conditions, when the mixing is dominated by mechanical turbulence, are reviewed and compared with mixing heights derived from wind (SODAR) and temperature (RASS) profiles measured in the Milan urban area during spring and summer 1996. Mixing heights derived from temperature soundings correlate positively with those derived from wind soundings only when a stable layer is superimposed to a quasi-adiabatic layer, while the correlation is very weak in the presence of a ground-based inversion. In general, indirect algorithms perform very poorly if compared with RASS-based estimates, and reasonably well if compared with SODAR-based estimates. Among the others, Benkley and Schulman (1979, Journal of Applied Meteorology 18, 772–780) method, which makes use of wind speed observed at 10 m height, and Nieuwstadt (1984, Boundary-Layer Meteorology 30, 31–55), which makes use of friction velocity and Monin–Obukhov length, give the best results.     

Long-range transport potential of semivolatile organic chemicals in coupled air-water systems

Ongoing deliberations on the regulation of semivolatile organic chemicals require the assessment of chemical transport in atmospheric and marine systems. The characteristic travel distance was proposed as a measure for the transport potential in air and water. However, the existing definition treats the transport processes separately. It is shown that combined transport in coupled air-ocean systems can accelerate the overall transport into remote regions. Concentration ratios in air and water change with distance from sources depending on the initial concentration ratio and on the difference between the transport velocities. A measure is suggested facilitating the chemical screening with respect to transport potentials in such air-ocean systems. A case study for alpha and gamma-hexachlorocyclohexane shows that the suggested measure qualitatively reveals the transport potentials of these chemicals and exemplifies possible concentration patterns.     

Numerical study of atmospheric dispersion of a substance released from an industrial complex in the southern coast of Korea

Diurnal variations of wind field and pollutant dispersion in a complex terrain with a shoreline were investigated under the insolation conditions of summer and winter. The area is located in the south of the Korean Peninsula and includes a large petrochemical industrial complex. The Regional Atmospheric Modeling System (RAMS) was used in the simulation study. Initially, horizontally homogeneous wind fields were assumed on the basis of sounding data at the nearby upper-air station for days with morning wind speeds below 2 m s⁻¹. On these days, the sea breeze prevailed in summer while the land breeze lasted for a few hours in the morning; the effect of synoptic winds was strong in winter with some inclusion of wind variations owing to the interaction between sea and land. The predicted wind direction at the location of the weather station captured an important change of the sea/land breeze of the observed one. In the morning, both in summer and winter, complicated wind fields with low wind speeds resulted in high pollutant concentrations almost all over the area. On the other hand, in the afternoon, the wind field was rather uniform and the terrain effects were not significant even in the mountainous area with the development of a mixing layer.