Person: Mickley, Loretta
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Mickley
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Loretta
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Mickley, Loretta
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Publication Formaldehyde (HCHO) As a Hazardous Air Pollutant: Mapping Surface Air Concentrations from Satellite and Inferring Cancer Risks in the United States(American Chemical Society (ACS), 2017-05-05) Zhu, Lei; Jacob, Daniel; Keutsch, Frank; Mickley, Loretta; Scheffe, Richard; Strum, Madeleine; González Abad, Gonzalo; Chance, Kelly; Yang, Kai; Rappenglück, Bernhard; Millet, Dylan; Baasandorj, Munkhbayar; Jaeglé, Lyatt; Shah, ViralFormaldehyde (HCHO) is the most important carcinogen in outdoor air among the 187 hazardous air pollutants (HAPs) identified by the U.S. Environmental Protection Agency (EPA), not including ozone and particulate matter. However, surface observations of HCHO are sparse and the EPA monitoring network could be prone to positive interferences. Here we use 2005–2016 summertime HCHO column data from the OMI satellite instrument, validated with high-quality aircraft data and oversampled on a 5 × 5 km2 grid, to map surface air HCHO concentrations across the contiguous U.S. OMI-derived summertime HCHO values are converted to annual averages using the GEOS-Chem chemical transport model. Results are in good agreement with high-quality summertime observations from urban sites (−2% bias, r = 0.95) but a factor of 1.9 lower than annual means from the EPA network. We thus estimate that up to 6600–12 500 people in the U.S. will develop cancer over their lifetimes by exposure to outdoor HCHO. The main HCHO source in the U.S. is atmospheric oxidation of biogenic isoprene, but the corresponding HCHO yield decreases as the concentration of nitrogen oxides (NOx ≡ NO + NO2) decreases. A GEOS-Chem sensitivity simulation indicates that HCHO levels would decrease by 20–30% in the absence of U.S. anthropogenic NOx emissions. Thus, NOx emission controls to improve ozone air quality have a significant cobenefit in reducing HCHO-related cancer risks.Publication Strong Dependence of U.S. Summertime Air Quality on the Decadal Variability of Atlantic Sea Surface Temperatures(John Wiley and Sons Inc., 2017) Shen, Lulu; Mickley, Loretta; Leibensperger, Eric M.; Li, MingweiAbstract We find that summertime air quality in the eastern U.S. displays strong dependence on North Atlantic sea surface temperatures, resulting from large‐scale ocean‐atmosphere interactions. Using observations, reanalysis data sets, and climate model simulations, we further identify a multidecadal variability in surface air quality driven by the Atlantic Multidecadal Oscillation (AMO). In one‐half cycle (~35 years) of the AMO from cold to warm phase, summertime maximum daily 8 h ozone concentrations increase by 1–4 ppbv and PM2.5 concentrations increase by 0.3–1.0 μg m−3 over much of the east. These air quality changes are related to warmer, drier, and more stagnant weather in the AMO warm phase, together with anomalous circulation patterns at the surface and aloft. If the AMO shifts to the cold phase in future years, it could partly offset the climate penalty on U.S. air quality brought by global warming, an effect which should be considered in long‐term air quality planning.Publication Southeast Atmosphere Studies: learning from model-observation syntheses(2018) Mao, Jingqiu; Carlton, Annmarie; Cohen, Ronald C.; Brune, William H.; Brown, Steven S.; Wolfe, Glenn M.; Jimenez, Jose L.; Pye, Havala O. T.; Ng, Nga Lee; Xu, Lu; McNeill, V. Faye; Tsigaridis, Kostas; McDonald, Brian C.; Warneke, Carsten; Guenther, Alex; Alvarado, Matthew J.; de Gouw, Joost; Mickley, Loretta; Leibensperger, Eric M.; Mathur, Rohit; Nolte, Christopher G.; Portmann, Robert W.; Unger, Nadine; Tosca, Mika; Horowitz, Larry W.Concentrations of atmospheric trace species in the United States have changed dramatically over the past several decades in response to pollution control strategies, shifts in domestic energy policy and economics, and economic development (and resulting emission changes) elsewhere in the world. Reliable projections of the future atmosphere require models to not only accurately describe current atmospheric concentrations, but to do so by representing chemical, physical and biological processes with conceptual and quantitative fidelity. Only through incorporation of the processes controlling emissions and chemical mechanisms that represent the key transformations among reactive molecules can models reliably project the impacts of future policy, energy and climate scenarios. Efforts to properly identify and implement the fundamental and controlling mechanisms in atmospheric models benefit from intensive observation periods, during which collocated measurements of diverse, speciated chemicals in both the gas and condensed phases are obtained. The Southeast Atmosphere Studies (SAS, including SENEX, SOAS, NOMADSS and SEAC4RS) conducted during the summer of 2013 provided an unprecedented opportunity for the atmospheric modeling community to come together to evaluate, diagnose and improve the representation of fundamental climate and air quality processes in models of varying temporal and spatial scales. This paper is aimed at discussing progress in evaluating, diagnosing and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models. The effort focused primarily on model representation of fundamental atmospheric processes that are essential to the formation of ozone, secondary organic aerosol (SOA) and other trace species in the troposphere, with the ultimate goal of understanding the radiative impacts of these species in the southeast and elsewhere. Here we address questions surrounding four key themes: gas-phase chemistry, aerosol chemistry, regional climate and chemistry interactions, and natural and anthropogenic emissions. We expect this review to serve as a guidance for future modeling efforts.Publication Regional warming from aerosol removal over the United States: Results from a transient 2010–2050 climate simulation(Elsevier BV, 2012) Mickley, Loretta; Leibensperger, Eric Michael; Jacob, Daniel; Rind, D.We use a general circulation model (NASA Goddard Institute for Space Studies GCM 3) to investigate the regional climate response to removal of aerosols over the United States. We perform a pair of transient 2010–2050 climate simulations following a scenario of increasing greenhouse gas concentrations, with and without aerosols over the United States and with present-day aerosols elsewhere. We find that removing U.S. aerosol significantly enhances the warming from greenhouse gases in a spatial pattern that strongly correlates with that of the aerosol. Warming is nearly negligible outside the United States, but annual mean surface temperatures increase by 0.4–0.6 K in the eastern United States. Temperatures during summer heat waves in the Northeast rise by as much as 1–2 K due to aerosol removal, driven in part by positive feedbacks involving soil moisture and low cloud cover. Reducing U.S. aerosol sources to achieve air quality objectives could thus have significant unintended regional warming consequences.Publication Meteorological Modes of Variability for Fine Particulate Matter (PM2.5) Air Quality in the United States: Implications for PM2.5 Sensitivity to Climate Change(European Geosciences Union, 2012) Tai, A. P. K.; Mickley, Loretta; Jacob, Daniel; Leibensperger, Eric Michael; Zhang, L.; Fisher, Jenny; Pye, H. O. T.We applied a multiple linear regression model to understand the relationships of PM2.5 with meteorological variables in the contiguous US and from there to infer the sensitivity of PM2.5 to climate change. We used 2004–2008 PM2.5 observations from ~1000 sites (~200 sites for PM2.5 components) and compared to results from the GEOS-Chem chemical transport model (CTM). All data were deseasonalized to focus on synoptic-scale correlations. We find strong positive correlations of PM2.5 components with temperature in most of the US, except for nitrate in the Southeast where the correlation is negative. Relative humidity (RH) is generally positively correlated with sulfate and nitrate but negatively correlated with organic carbon. GEOS-Chem results indicate that most of the correlations of PM2.5 with temperature and RH do not arise from direct dependence but from covariation with synoptic transport. We applied principal component analysis and regression to identify the dominant meteorological modes controlling PM2.5 variability, and show that 20–40% of the observed PM2.5 day-to-day variability can be explained by a single dominant meteorological mode: cold frontal passages in the eastern US and maritime inflow in the West. These and other synoptic transport modes drive most of the overall correlations of PM2.5 with temperature and RH except in the Southeast. We show that interannual variability of PM2.5 in the US Midwest is strongly correlated with cyclone frequency as diagnosed from a spectral-autoregressive analysis of the dominant meteorological mode. An ensemble of five realizations of 1996–2050 climate change with the GISS general circulation model (GCM) using the same climate forcings shows inconsistent trends in cyclone frequency over the Midwest (including in sign), with a likely decrease in cyclone frequency implying an increase in PM2.5. Our results demonstrate the need for multiple GCM realizations (because of climate chaos) when diagnosing the effect of climate change on PM2.5, and suggest that analysis of meteorological modes of variability provides a computationally more affordable approach for this purpose than coupled GCM-CTM studies.Publication Correlations between Fine Particulate Matter \((PM_{2.5})\) and Meteorological Variables in the United States: Implications for the Sensitivity of \(PM_{2.5}\) to Climate Change(Elsevier, 2010) Tai, Amos P.K.; Mickley, Loretta; Jacob, DanielWe applied a multiple linear regression (MLR) model to study the correlations of total \(PM_{2.5}\) and its components with meteorological variables using an 11-year (1998–2008) observational record over the contiguous US. The data were deseasonalized and detrended to focus on synoptic-scale correlations. We find that daily variation in meteorology as described by the MLR can explain up to 50% of \(PM_{2.5}\) variability with temperature, relative humidity (RH), precipitation, and circulation all being important predictors. Temperature is positively correlated with sulfate, organic carbon (OC) and elemental carbon (EC) almost everywhere. The correlation of nitrate with temperature is negative in the Southeast but positive in California and the Great Plains. RH is positively correlated with sulfate and nitrate, but negatively with OC and EC. Precipitation is strongly negatively correlated with all \(PM_{2.5}\) components. We find that \(PM_{2.5}\) concentrations are on average \(2.6 \mu g m^{−3}\) higher on stagnant vs. non-stagnant days. Our observed correlations provide a test for chemical transport models used to simulate the sensitivity of \(PM_{2.5}\) to climate change. They point to the importance of adequately representing the temperature dependence of agricultural, biogenic and wildfire emissions in these models.Publication Impacts of Changes in Land Use and Land Cover on Atmospheric Chemistry and Air Quality over the 21st Century(European Geosciences Union, 2012) Wu, S.; Mickley, Loretta; Kaplan, J. O.; Jacob, DanielThe effects of future land use and land cover change on the chemical composition of the atmosphere and air quality are largely unknown. To investigate the potential effects associated with future changes in vegetation driven by atmospheric CO2 concentrations, climate, and anthropogenic land use over the 21st century, we performed a series of model experiments combining a general circulation model with a dynamic global vegetation model and an atmospheric chemical-transport model. Our results indicate that climate- and CO2-induced changes in vegetation composition and density between 2100 and 2000 could lead to decreases in summer afternoon surface ozone of up to 10 ppb over large areas of the northern mid-latitudes. This is largely driven by the substantial increases in ozone dry deposition associated with increases in vegetation density in a warmer climate with higher atmospheric CO2 abundance. Climate-driven vegetation changes over the period 2000–2100 lead to general increases in isoprene emissions, globally by 15% in 2050 and 36% in 2100. These increases in isoprene emissions result in decreases in surface ozone concentrations where the NOx levels are low, such as in remote tropical rainforests. However, over polluted regions, such as the northeastern United States, ozone concentrations are calculated to increase with higher isoprene emissions in the future. Increases in biogenic emissions also lead to higher concentrations of secondary organic aerosols, which increase globally by 10% in 2050 and 20% in 2100. Summertime surface concentrations of secondary organic aerosols are calculated to increase by up to 1 μg m−3 and double for large areas in Eurasia over the period of 2000–2100. When we use a scenario of future anthropogenic land use change, we find less increase in global isoprene emissions due to replacement of higher-emitting forests by lower-emitting cropland. The global atmospheric burden of secondary organic aerosols changes little by 2100 when we account for future land use change, but both secondary organic aerosols and ozone show large regional changes at the surface.Publication Climatic Effects of 1950-2050 Changes in US Anthropogenic Aerosols - Part 2: Climate Response(European Geosciences Union, 2012) Leibensperger, Eric Michael; Mickley, Loretta; Jacob, Daniel; Chen, W.-T.; Seinfeld, J. H.; Nenes, A.; Adams, P. J.; Streets, D. G.; Kumar, N.; Rind, D.We investigate the climate response to changing US anthropogenic aerosol sources over the 1950–2050 period by using the NASA GISS general circulation model (GCM) and comparing to observed US temperature trends. Time-dependent aerosol distributions are generated from the GEOS-Chem chemical transport model applied to historical emission inventories and future projections. Radiative forcing from US anthropogenic aerosols peaked in 1970–1990 and has strongly declined since due to air quality regulations. We find that the regional radiative forcing from US anthropogenic aerosols elicits a strong regional climate response, cooling the central and eastern US by 0.5–1.0 °C on average during 1970–1990, with the strongest effects on maximum daytime temperatures in summer and autumn. Aerosol cooling reflects comparable contributions from direct and indirect (cloud-mediated) radiative effects. Absorbing aerosol (mainly black carbon) has negligible warming effect. Aerosol cooling reduces surface evaporation and thus decreases precipitation along the US east coast, but also increases the southerly flow of moisture from the Gulf of Mexico resulting in increased cloud cover and precipitation in the central US. Observations over the eastern US show a lack of warming in 1960–1980 followed by very rapid warming since, which we reproduce in the GCM and attribute to trends in US anthropogenic aerosol sources. Present US aerosol concentrations are sufficiently low that future air quality improvements are projected to cause little further warming in the US (0.1 °C over 2010–2050). We find that most of the warming from aerosol source controls in the US has already been realized over the 1980–2010 period.Publication Climatic Effects of 1950-2050 Changes in US Anthropogenic Aerosols - Part 1: Aerosol Trends and Radiative Forcing(European Geosciences Union, 2012) Leibensperger, Eric Michael; Mickley, Loretta; Jacob, Daniel; Chen, W.-T.; Seinfeld, J. H.; Nenes, A.; Adams, P. J.; Streets, D. G.; Kumar, N.; Rind, D.We calculate decadal aerosol direct and indirect (warm cloud) radiative forcings from US anthropogenic sources over the 1950–2050 period. Past and future aerosol distributions are constructed using GEOS-Chem and historical emission inventories and future projections from the IPCC A1B scenario. Aerosol simulations are evaluated with observed spatial distributions and 1980–2010 trends of aerosol concentrations and wet deposition in the contiguous US. Direct and indirect radiative forcing is calculated using the GISS general circulation model and monthly mean aerosol distributions from GEOS-Chem. The radiative forcing from US anthropogenic aerosols is strongly localized over the eastern US. We find that its magnitude peaked in 1970–1990, with values over the eastern US (east of 100° W) of −2.0 W m−2 for direct forcing including contributions from sulfate (−2.0 W m−2), nitrate (−0.2 W m−2), organic carbon (−0.2 W m−2), and black carbon (+0.4 W m−2). The uncertainties in radiative forcing due to aerosol radiative properties are estimated to be about 50%. The aerosol indirect effect is estimated to be of comparable magnitude to the direct forcing. We find that the magnitude of the forcing declined sharply from 1990 to 2010 (by 0.8 W m−2 direct and 1.0 W m−2 indirect), mainly reflecting decreases in SO2 emissions, and project that it will continue declining post-2010 but at a much slower rate since US SO2 emissions have already declined by almost 60% from their peak. This suggests that much of the warming effect of reducing US anthropogenic aerosol sources has already been realized. The small positive radiative forcing from US BC emissions (+0.3 W m−2 over the eastern US in 2010; 5% of the global forcing from anthropogenic BC emissions worldwide) suggests that a US emission control strategy focused on BC would have only limited climate benefit.Publication Tropospheric Bromine Chemistry: Implications for Present and Pre-Industrial Ozone and Mercury(European Geosciences Union, 2012) Parrella, J. P.; Jacob, Daniel; Liang, Q.; Zhang, Y.; Mickley, Loretta; Miller, Benjamin Franklin; Evans, M. J.; Yang, X.; Pyle, J. A.; Theys, N.; Van Roozendael, M.We present a new model for the global tropospheric chemistry of inorganic bromine (Bry) coupled to oxidant-aerosol chemistry in the GEOS-Chem chemical transport model (CTM). Sources of tropospheric Bry include debromination of sea-salt aerosol, photolysis and oxidation of short-lived bromocarbons, and transport from the stratosphere. Comparison to a GOME-2 satellite climatology of tropospheric BrO columns shows that the model can reproduce the observed increase of BrO with latitude, the northern mid-latitudes maximum in winter, and the Arctic maximum in spring. This successful simulation is contingent on the HOBr + HBr reaction taking place in aqueous aerosols and ice clouds. Bromine chemistry in the model decreases tropospheric ozone mixing ratios by <1–8 nmol mol−1 (6.5% globally), with the largest effects in the northern extratropics in spring. The global mean tropospheric OH concentration decreases by 4%. Inclusion of bromine chemistry improves the ability of global models (GEOS-Chem and p-TOMCAT) to simulate observed 19th-century ozone and its seasonality. Bromine effects on tropospheric ozone are comparable in the present-day and pre-industrial atmospheres so that estimates of anthropogenic radiative forcing are minimally affected. Br atom concentrations are 40% higher in the pre-industrial atmosphere due to lower ozone, which would decrease by a factor of 2 the atmospheric lifetime of elemental mercury against oxidation by Br. This suggests that historical anthropogenic mercury emissions may have mostly deposited to northern mid-latitudes, enriching the corresponding surface reservoirs. The persistent rise in background surface ozone at northern mid-latitudes during the past decades could possibly contribute to the observations of elevated mercury in subsurface waters of the North Atlantic.