Kristen M. Foley

Attribution of the United States "warming hole": aerosol indirect effect and precipitable water vapor.

Aerosols can influence the climate indirectly by acting as cloud condensation nuclei and/or ice nuclei, thereby modifying cloud optical properties. In contrast to the widespread global warming, the central and south central United States display a noteworthy overall cooling trend during the 20th century, with an especially striking cooling trend in summertime daily maximum temperature (Tmax) (termed the U.S. “warming hole”). Here we used observations of temperature, shortwave cloud forcing (SWCF), longwave cloud forcing (LWCF), aerosol optical depth and precipitable water vapor as well as global coupled climate models to explore the attribution of the “warming hole”. We find that the observed cooling trend in summer Tmax can be attributed mainly to SWCF due to aerosols with offset from the greenhouse effect of precipitable water vapor. A global coupled climate model reveals that the observed “warming hole” can be produced only when the aerosol fields are simulated with a reasonable degree of accuracy as this is necessary for accurate simulation of SWCF over the region. These results provide compelling evidence of the role of the aerosol indirect effect in cooling regional climate on the Earth. Our results reaffirm that LWCF can warm both winter Tmax and Tmin.

Description and evaluation of the Community Multiscale Air Quality (CMAQ) modeling system version 5.1

The Community Multiscale Air Quality (CMAQ) model is a comprehensive multipollutant air quality modeling system developed and maintained by the US Environmental Protection Agency’s (EPA) Office of Research and Development (ORD). Recently, version 5.1 of the CMAQ model (v5.1) was released to the public, incorporating a large number of science updates and extended capabilities over the previous release version of the model (v5.0.2). These updates include the following: improvements in the meteorological calculations in both CMAQ and the Weather Research and Forecast (WRF) model used to provide meteorological fields to CMAQ, updates to the gas and aerosol chemistry, revisions to the calculations of clouds and photolysis, and improvements to the dry and wet deposition in the model. Sensitivity simulations isolating several of the major updates to the modeling system show that changes to the meteorological calculations result in enhanced afternoon and early evening mixing in the model, periods when the model historically underestimates mixing. This enhanced mixing results in higher ozone (O3) mixing ratios on average due to reduced NO titration, and lower fine particulate matter (PM2.5) concentrations due to greater dilution of primary pollutants (e.g., elemental and organic carbon). Updates to the clouds and photolysis calculations greatly improve consistency between the WRF and CMAQ models and result in generally higher O3 mixing ratios, primarily due to reduced cloudiness and attenuation of photolysis in the model. Updates to the aerosol chemistry result in higher secondary organic aerosol (SOA) concentrations in the summer, thereby reducing summertime PM2.5 bias (PM2.5 is typically underestimated by CMAQ in the summer), while updates to the gas chemistry result in slightly higher O3 and PM2.5 on average in January and July. Overall, the seasonal variation in simulated PM2.5 generally improves in CMAQv5.1 (when considering all model updates), as simulated PM2.5 concentrations decrease in the winter (when PM2.5 is generally overestimated by CMAQ) and increase in the summer (when PM2.5 is generally underestimated by CMAQ). Ozone mixing ratios are higher on average with v5.1 vs. v5.0.2, resulting in higher O3 mean bias, as O3 tends to be overestimated by CMAQ throughout most of the year (especially at locations where the observed O3 is low); however, O3 correlation is largely improved with v5.1. Sensitivity simulations for several hypothetical emission reduction scenarios show that v5.1 tends to be slightly more responsive to reductions in NOx (NO + NO2), VOC and SOx (SO2 + SO4) emissions than v5.0.2, representing an improvement as previous studies have shown CMAQ to underestimate the observed reduction in O3 due to large, widespread reductions in observed emissions.

A Comparison of Statistical Techniques for Combining Modeled and Observed Concentrations to Create High-Resolution Ozone Air Quality Surfaces

Abstract Air quality surfaces representing pollutant concentrations across space and time are needed for many applications, including tracking trends and relating air quality to human and ecosystem health. The spatial and temporal characteristics of these surfaces may reveal new information about the associations between emissions, pollution levels, and human exposure and health outcomes that may not have been discernable before. This paper presents four techniques, ranging from simple to complex, to statistically combine observed and modeled daily maximum 8-hr ozone concentrations for a domain covering the greater New York State area for the summer of 2001. Cross-validation results indicate that, for the domain and time period studied, the simpler techniques (additive and multiplicative bias adjustment) perform as well as or better than the more complex techniques. However, the spatial analyses of the resulting ozone concentration surfaces revealed some problems with these simpler techniques in limited areas where the model exhibits difficulty in simulating the complex features such as those observed in the New York City area.

Sensitivity of continental United States atmospheric budgets of oxidized and reduced nitrogen to dry deposition parametrizations

Reactive nitrogen (Nr) is removed by surface fluxes (air–surface exchange) and wet deposition. The chemistry and physics of the atmosphere result in a complicated system in which competing chemical sources and sinks exist and impact that removal. Therefore, uncertainties are best examined with complete regional chemical transport models that simulate these feedbacks. We analysed several uncertainties in regional air quality model resistance analogue representations of air–surface exchange for unidirectional and bi-directional fluxes and their effect on the continental Nr budget. Model sensitivity tests of key parameters in dry deposition formulations showed that uncertainty estimates of continental total nitrogen deposition are surprisingly small, 5 per cent or less, owing to feedbacks in the chemistry and rebalancing among removal pathways. The largest uncertainties (5%) occur with the change from a unidirectional to a bi-directional NH3 formulation followed by uncertainties in bi-directional compensation points (1–4%) and unidirectional aerodynamic resistance (2%). Uncertainties have a greater effect at the local scale. Between unidirectional and bi-directional formulations, single grid cell changes can be up to 50 per cent, whereas 84 per cent of the cells have changes less than 30 per cent. For uncertainties within either formulation, single grid cell change can be up to 20 per cent, but for 90 per cent of the cells changes are less than 10 per cent.

Impact of Enhanced Ozone Deposition and Halogen Chemistry on Tropospheric Ozone over the Northern Hemisphere.

Fate of ozone in marine environments has been receiving increased attention due to the tightening of ambient air quality standards. The role of deposition and halogen chemistry is examined through incorporation of an enhanced ozone deposition algorithm and inclusion of halogen chemistry in a comprehensive atmospheric modeling system. The enhanced ozone deposition treatment accounts for the interaction of iodide in seawater with ozone and increases deposition velocities by 1 order of magnitude. Halogen chemistry includes detailed chemical reactions of organic and inorganic bromine and iodine species. Two different simulations are completed with the halogen chemistry: without and with photochemical reactions of higher iodine oxides. Enhanced deposition reduces mean summer-time surface ozone by ∼3% over marine regions in the Northern Hemisphere. Halogen chemistry without the photochemical reactions of higher iodine oxides reduces surface ozone by ∼15% whereas simulations with the photochemical reactions of higher iodine oxides indicate ozone reductions of ∼48%. The model without these processes overpredicts ozone compared to observations whereas the inclusion of these processes improves predictions. The inclusion of photochemical reactions for higher iodine oxides leads to ozone predictions that are lower than observations, underscoring the need for further refinement of the halogen emissions and chemistry scheme in the model.

Extreme value analysis for evaluating ozone control strategies

Tropospheric ozone is one of six criteria pollutants regulated by the US EPA, and has been linked to respiratory and cardiovascular endpoints and adverse effects on vegetation and ecosystems. Regional photochemical models have been developed to study the impacts of emission reductions on ozone levels. The standard approach is to run the deterministic model under new emission levels and attribute the change in ozone concentration to the emission control strategy. However, running the deterministic model requires substantial computing time, and this approach does not provide a measure of uncertainty for the change in ozone levels. Recently, a reduced form model (RFM) has been proposed to approximate the complex model as a simple function of a few relevant inputs. In this paper, we develop a new statistical approach to make full use of the RFM to study the effects of various control strategies on the probability and magnitude of extreme ozone events. We fuse the model output with monitoring data to calibrate the RFM by modeling the conditional distribution of monitoring data given the RFM using a combination of flexible semiparametric quantile regression for the center of the distribution where data are abundant and a parametric extreme value distribution for the tail where data are sparse. Selected parameters in the conditional distribution are allowed to vary by the RFM value and the spatial location. Also, due to the simplicity of the RFM, we are able to embed the RFM in our Bayesian hierarchical framework to obtain a full posterior for the model input parameters, and propagate this uncertainty to the estimation of the effects of the control strategies. We use the new framework to evaluate three potential control strategies, and find that reducing mobile-source emissions has a larger impact than reducing point-source emissions or a combination of several emission sources.

Linking air quality and watershed models for environmental assessments: Analysis of the effects of model-specific precipitation estimates on calculated water flux

Directly linking air quality and watershed models could provide an effective method for estimating spatially-explicit inputs of atmospheric contaminants to watershed biogeochemical models. However, to adequately link air and watershed models for wet deposition estimates, each models temporal and spatial representation of precipitation needs to be consistent. We explore how precipitation implemented within the Community Multi-Scale Air Quality Model (CMAQ) model algorithms, and multiple spatially-explicit precipitation datasets that could be used to improve the CMAQ model deposition estimates, links with the standard precipitation sources used to calibrate watershed models (i.e., rain gage data) via modeled water fluxes. Simulations are run using a grid-based watershed mercury model (GBMM) in two watersheds. Modeled monthly runoff suggests that multiple resolution Parameter-elevations Regressions on Independent Slopes Model (PRISM) and National Multi-sensor Precipitation Analysis Stage IV (NPA) data generate similar monthly runoff estimates, with comparable or greater accuracy when evaluated against stream gage data than that produced by the base rain gage data. However, across longer time periods, simulated water balances using 36 km Pennsylvania State University/National Center for Atmospheric Research mesoscale model (MM5) data are similar to that of base data. The investigation also examines the implications our results, providing suggestions for linking air quality and watershed fate and transport models.

A spectral method for spatial downscaling

Complex computer models play a crucial role in air quality research. These models are used to evaluate potential regulatory impacts of emission control strategies and to estimate air quality in areas without monitoring data. For both of these purposes, it is important to calibrate model output with monitoring data to adjust for model biases and improve spatial prediction. In this article, we propose a new spectral method to study and exploit complex relationships between model output and monitoring data. Spectral methods allow us to estimate the relationship between model output and monitoring data separately at different spatial scales, and to use model output for prediction only at the appropriate scales. The proposed method is computationally efficient and can be implemented using standard software. We apply the method to compare Community Multiscale Air Quality (CMAQ) model output with ozone measurements in the United States in July 2005. We find that CMAQ captures large-scale spatial trends, but has low correlation with the monitoring data at small spatial scales.

Bayesian analysis of a reduced-form air quality model.

Numerical air quality models are being used for assessing emission control strategies for improving ambient pollution levels across the globe. This paper applies probabilistic modeling to evaluate the effectiveness of emission reduction scenarios aimed at lowering ground-level ozone concentrations. A Bayesian hierarchical model is used to combine air quality model output and monitoring data in order to characterize the impact of emissions reductions while accounting for different degrees of uncertainty in the modeled emissions inputs. The probabilistic model predictions are weighted based on population density in order to better quantify the societal benefits/disbenefits of four hypothetical emission reduction scenarios in which domain-wide NO(x) emissions from various sectors are reduced individually and then simultaneously. Cross validation analysis shows the statistical model performs well compared to observed ozone levels. Accounting for the variability and uncertainty in the emissions and atmospheric systems being modeled is shown to impact how emission reduction scenarios would be ranked, compared to standard methodology.

Characterizing the impact of projected changes in climate and air quality on human exposures to ozone

The impact of climate change on human and environmental health is of critical concern. Population exposures to air pollutants both indoors and outdoors are influenced by a wide range of air quality, meteorological, behavioral, and housing-related factors, many of which are also impacted by climate change. An integrated methodology for modeling changes in human exposures to tropospheric ozone (O3) owing to potential future changes in climate and demographics was implemented by linking existing modeling tools for climate, weather, air quality, population distribution, and human exposure. Human exposure results from the Air Pollutants Exposure Model (APEX) for 12 US cities show differences in daily maximum 8-h (DM8H) exposure patterns and levels by sex, age, and city for all scenarios. When climate is held constant and population demographics are varied, minimal difference in O3 exposures is predicted even with the most extreme demographic change scenario. In contrast, when population is held constant, we see evidence of substantial changes in O3 exposure for the most extreme change in climate. Similarly, we see increases in the percentage of the population in each city with at least one O3 exposure exceedance above 60 p.p.b and 70 p.p.b thresholds for future changes in climate. For these climate and population scenarios, the impact of projected changes in climate and air quality on human exposure to O3 are much larger than the impacts of changing demographics. These results indicate the potential for future changes in O3 exposure as a result of changes in climate that could impact human health.