Person:

Mickley, Loretta

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.

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.

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.

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.

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.

Radiative forcing by aerosols and tropospheric ozone could play a significant role in recent Arctic warming. These species are in general poorly accounted for in climate models. We use the GEOS-Chem global chemical transport model to construct a 3-D representation of Arctic aerosols and ozone that is consistent with observations and can be used in climate simulations. We focus on 2008, when extensive observations were made from different platforms as part of the International Polar Year. Comparison to aircraft, surface, and ship cruise observations suggests that GEOS-Chem provides in general a successful year-round simulation of Arctic black carbon (BC), organic carbon (OC), sulfate, and dust aerosol. BC has major fuel combustion and boreal fire sources, OC is mainly from fires, sulfate has a mix of anthropogenic and natural sources, and dust is mostly from the Sahara. The model is successful in simulating aerosol optical depth (AOD) observations from Aerosol Robotics Network stations in the Arctic; the sharp drop from spring to summer appears driven in part by the smaller size of sulfate aerosol in summer. The anthropogenic contribution to Arctic AOD is a factor of 4 larger in spring than in summer and is mainly sulfate. Simulation of absorbing aerosol optical depth (AAOD) indicates that non-BC aerosol (OC and dust) contributed 24% of Arctic AAOD at 550 nm and 37% of absorbing mass deposited to the snow pack in 2008. Open fires contributed half of AAOD at 550 nm and half of deposition to the snowpack.

Satellite observations of formaldehyde (HCHO) columns provide top-down constraints on emissions of highly reactive volatile organic compounds (HRVOCs). This approach has been used previously in the US to estimate isoprene emissions from vegetation, but application to anthropogenic emissions has been stymied by lack of a discernable HCHO signal. Here we show that temporal oversampling of HCHO data from the Ozone Monitoring Instrument (OMI) for 2005–2008 enables detection of urban and industrial plumes in eastern Texas including Houston, Port Arthur, and Dallas/Fort Worth. By spatially integrating the HCHO enhancement in the Houston plume observed by OMI we estimate an anthropogenic HCHO source of 250 ± 140 kmol h−1. This implies that anthropogenic HRVOC emissions in Houston are 4.8 ± 2.7 times higher than reported by the US Environmental Protection Agency inventory, and is consistent with field studies identifying large ethene and propene emissions from petrochemical industrial sources.

Land clearing by fire in Equatorial Asia, a substantial fraction for conversion to oil palm plantations, can lead to high smoke concentrations across this densely populated region and represents a serious public health concern. Here we use the adjoint of the GEOS-Chem chemical transport model to show that population exposure to the smoke is highly dependent on where the fires from clearing (and other activities) take place. In 2006, we find that Sumatran fires disproportionately contributed to the regional population-weighted smoke exposure (37% of regional fire emissions, 63% of the exposure). The information from the adjoint can provide guidance for targeted land conservation as oil palm agriculture expands. Protecting peatswamp forests in Southeast Sumatra emerges as a high priority. We present the adjoint as a tool that can be useful in a cost-benefit analysis to inform policymakers on the relative merits of targeting conservation in different regions of Equatorial Asia.

Studies of the effect of climate change on fine particulate matter (PM2.5) air quality using general circulation models (GCMs) show inconsistent results including in the sign of the effect. This reflects uncertainty in the GCM simulations of the regional meteorological variables affecting PM2.5. Here we use the CMIP3 archive of data from fifteen different IPCC AR4 GCMs to obtain improved statistics of 21st-century trends in the meteorological modes driving PM2.5 variability over the contiguous US. We analyze 1999–2010 observations to identify the dominant meteorological modes driving interannual PM2.5 variability and their synoptic periods T. We find robust correlations (r > 0.5) of annual mean PM2.5 with T, especially in the eastern US where the dominant modes represent frontal passages. The GCMs all have significant skill in reproducing present-day statistics for T and we show that this reflects their ability to simulate atmospheric baroclinicity. We then use the local PM2.5-to-period sensitivity (dPM2.5/dT) from the 1999–2010 observations to project PM2.5 changes from the 2000–2050 changes in T simulated by the 15 GCMs following the SRES A1B greenhouse warming scenario. By weighted-average statistics of GCM results we project a likely 2000–2050 increase of ~ 0.1 μg m−3 in annual mean PM2.5 in the eastern US arising from less frequent frontal ventilation, and a likely decrease albeit with greater inter-GCM variability in the Pacific Northwest due to more frequent maritime inflows. Potentially larger regional effects of 2000–2050 climate change on PM2.5 may arise from changes in temperature, biogenic emissions, wildfires, and vegetation, but are still unlikely to affect annual PM2.5 by more than 0.5 μg m−3.

The 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.