1. Interactions between climate and atmospheric chemistry in the US Loretta J. Mickley, Harvard University Collaborators: Rynda Hudman, Daniel Jacob, Eric Leibensperger, Jennifer Logan, Havala Pye, Dominick Spracklen, Amos Tai, Shiliang Wu, Moeko Yoshitomi Funding for this work: NASA, EPA, EPRI Smog over Pittsburgh, ranked #1 city for particulate pollution in 2008 by American Lung Association Effects of climate change on air quality Effects of short-lived species on climate

2. Part 1: Effects of climate change on air quality.

3. Millions of people in U.S. already live in areas of high pollution. How will a changing climate affect pollution? Calculated with new 0.075 ppm standard Number of people living in areas that exceed the national ambient air quality standards (NAAQS) in 2008. EPA’s Technical Support Document for the proposed finding on CO 2 as a pollutant. Cites the threat of climate change to air quality. Public hearings last week on EPA proposed finding in Detroit + NYC.

4. O3O3 O2O2 h O3O3 OHHO 2 h, H 2 O Deposition NO H2O2H2O2 CO, VOC NO 2 h STRATOSPHERE TROPOSPHERE 8-18 km Nitrogen oxide radicals; NO x = NO + NO 2 combustion, soil, lightning Methane wetlands, livestock, natural gas Nonmethane volatile organic compounds (VOCs) vegetation, combustion, industry CO (carbon monoxide) combustion, VOC oxidation Tropospheric ozone precursors Stagnation promotes ozone production Chemistry of tropospheric ozone: oxidation of CO, VOCs, and methane in the presence of NOx

5. Weather plays a large role in ozone air quality. The total derivative d[O 3 ]/dT is the sum of partial derivatives (  O 3 /  x i )(  x i /  T). x = ensemble of ozone forcing variables that are temperature-related. Lin et al., 2001 Probability of ozone exceedance vs. daily max. temperature Curves include effects of Biogenic emissions Stagnation Clear skies Northeast Southeast Los Angeles Temperature (K) Probability Days Number of summer days with ozone exceedances, mean over sites in Northeast 1988, hottest on record

6. Low pressure systems (aka cyclones) cross southern Canada and sweep out ozone pollution from Eastern US. Stalled high pressure system associated with: increased biogenic emissions clear skies weak winds high temperatures. cold front EPA ozone levels 3 days later Cold front pushes smog poleward and aloft on a warm conveyor belt. cold front Hazardous levels of ozone L L

7. Sample storm tracks, summer 1979-1981 Correlation between cyclone number each summer in red and green boxes and number of US ozone episodes Strong anti-correlation of cyclone number and number of ozone episodes in eastern US: Leibensperger et al., 2008 Cyclone passage through southern Canada/Great Lakes region strongly affects frequency and duration of U.S. ozone episodes. 27 year record Fewer cyclones per summer in green box leads to more ozone episodes in US.

8. 1950-2000 observed trend in cyclone frequency matches that in climate model with increasing greenhouse gases. Trend in cyclones appears due in part to weakened meridional temperature gradients, reduction of baroclinicity over midlatitudes. What does this trend mean for ozone pollution in US? Emissions of ozone precursors have declined during this period. Mickley et al., 2004; Leibensperger et al., 2008 1950-2006 trend in JJA cyclones in S. Canada 0.14 yr -1 0.16 yr -1 NCEP/NCAR obs

9. Trend in emissions and trend in cyclones have competing effects on surface ozone. Mickley et al., 2004; Leibensperger et al., 2008 Cyclones: less frequent cyclones + cold fronts mean more persistent pollution episodes Emissions: reduced emissions means fewer episodes. NE ozone episodes cyclones 1980-2006 trends Decline in emissions of ozone precursors from US mobile sources. Parrish 2006.

10. Ozone pollution days in the Northeast US days yr -1 Trend in pollution days due to decline in emissions We find that if 1980-2006 cyclone frequency had remained constant, we would have had zero episodes over Northeast. Trend in pollution days due to decline in cyclone frequency If emissions had remained constant, decline in mid-latitude cyclone number over Canada would have meant more persistent stagnation episodes, more ozone. Climate response

11. Particulate matter (PM, aerosols) sources and processes SO 2 H 2 SO 4 NH 3 VOCs NO x RCO… HNO 3 nucleation coagulation condensation carbonaceous combustion particles soil dust sea salt...... oxidation cycling ultra-fine (<0.01  m) fine (0.01-1  m) cloud (1-100  m) combustion biosphere volcanoes agriculture biosphere coarse (1-10  m) scavenging precursor gases wildfires

12. Observed correlations of total PM2.5 with meteorology Precipitation Stagnation Temperature Positive correlation with temperature occurs due to: Increased oxidation of SO 2 Greater biogenic emissions Results from EPA AQS database: 1000+ sites sampled every 1-6 days from 1998 to 2007. Observed correlations provide means to test model simulations. Temperature Precipitation Stagnation Tai et al., ms.

13. met fields chemistry fields What do models project for future air quality? We have developed GCAP (Global Change and Air Pollution). Regional climate model Regional chemistry model met fields Chemistry model driven by GCM meteorology to study influence of climate on air quality. Mickley et al., 2004 GEOS-Chem Chemical transport model chemistry, emissions 2050s 1990s 2000-2050 decrease in cyclone frequency leads to increased stagnation. CO tracer Northeast, Jul-Aug AIR QUALITY GISS GCM Physics of the atmosphere Qflux ocean, well- mixed GHGs

14. 2000-2050 change in max daily 8-hour average JJA ozone Climate penalty for air quality: Harvard model shows 2-12 ppb increase in surface ozone in East 2000-2050 change in max daily 8-hour average JJA ozone Multi-model comparison Weaver et al., 2009 Most models agree that surface ozone will increase over the Northeast. Disagreement occurs elsewhere due to differences in chemistry and cloud cover change. How will US surface ozone change in a changing climate? ppb

15. Calculated response in surface PM to +2.5 o C temperature change applied uniformly for July. Dawson et al., 2007 Uncertainty in response of surface PM to changing meteorology is large. We can use present-day observations to test models. (μg/m 3 ) Observed correlation between surface temperature and surface PM concentrations. Tai et al, ms. in progress Positive correlation with T due to: Increased oxidation of SO 2 Greater biogenic emissions

16. Part 2: Effects of short-lived species on climate. Case study of US aerosols and regional climate change. Radiative forcing: Easily calculated metric of climate change Suggests the relative magnitude of surface temperature response to a given perturbation.

17. Present-day radiative forcing due to aerosols over the eastern US is comparable in magnitude, but opposite in sign, to global forcing due to CO 2. Globally averaged radiative forcing due to CO 2 is +1.7 Wm -2. warming Due to short lifetime, forcing due to aerosols is not uniform across globe. Over the US, radiative forcing due to sulfate aerosols is -2 Wm -2. cooling IPCC, 2007; Liao et al., 2004

18. Comparison to observed sulfate concentrations shows good agreement. Sequence shows increasing sulfate from 1950-1980, followed by a decline in recent years. 19501960 19701980 19902001 Leibensperger et al., ms Calculated trend in surface sulfate concentrations, 1950- 2001. Trend in aerosols over United States suggests cleaner skies, possible warming?

19. Recent US Climate Change report suggests more global than regional response, but the report looks at an ensemble of short-lived species all over the globe. – U.S. Climate Change Science Program, Synthesis and Assessment Product 3.2 Harvard’s work to date suggests more regional than global response at least for US aerosols. Decline in the aerosol burden over the eastern US will lead to regional warming, in a way that the US Climate Change report would not have recognized. Is the climate response to changing aerosols regional or global? Calculated present-day aerosol optical depths

20. What is the influence of changing aerosol on regional climate? In pilot study, we zero out aerosol optical depths over US. For pilot study, 2 scenarios were simulated: Control: aerosol optical depths fixed at 1990s levels. Sensitivity: U.S. aerosol optical depths set to zero (providing a radiative forcing of about +2 W m -2 locally over the US); elsewhere, same as in control simulation. Each scenario includes an ensemble of 3 simulations. Caveats: No transport, only direct effect considered in this pilot study. GISS GCM

21. Removal of anthropogenic aerosols over US increases annual mean surface temperatures by 0.5 o C. Summertime temperatures increase as much as 1.5 o C. Mean 2010-2050 temperature difference: No-US-aerosol case – Control White areas signify no significant difference. Results from an ensemble of 3 for each case. Annual mean surface temperature change in Control. Warming due to 2010-2050 trend in greenhouse gases. Additional warming/ cooling due to zeroing of US aerosols Mickley et al., ms. 2009 oCoC oCoC

22. The regional surface temperature response to aerosol removal persists for many decades in the model. Temperature ( o C) No-US-aerosols case Control, with US aerosols Annual mean temperature trends over Eastern US Mickley et al., ms Bottom line: Efforts to clear the air of anthropogenic aerosol over the US may exacerbate regional warming.

23. GEOS-Chem chemistry transport model GISS GCM III climate model Calculation of cloud droplet number concentrations aerosol concentrations aerosol indirect effect We use historical/projected emissions of SO 2, NO x, BC, and OC to quantify the climatic role of US aerosols in the past and future. 1950-2050 Control simulation (EDGAR/Tami Bond historical emissions and A1B; includes rising U.S. aerosol sources until 1980 and subsequent decline) Sensitivity simulations: 1950-2050 No US aerosols. Quantifies the past effect of U.S. anthropogenic sources on regional climate. 2010-2050 Constant US emissions Quantifies the warming effect from the projected decrease in U.S. emissions. Ongoing study: Perform realistic simulation of changing aerosol optical depths over the US, together with sensitivity studies. Climate response to aerosol trends over the US

24. Implications for policymakers Policymakers need to consider “climate change penalty,” i.e., the additional emission controls necessary to meet a given air quality target. Efforts to clear the air of anthropogenic aerosol over the US may exacerbate regional warming. Directions for future research Understand causes in interannual variability of air quality. Investigate model sensitivity of pollutants to meteorology, and compare to observations. Understand chemistry of biogenic species, e.g. isoprene Improve emission inventories for recent past/future, especially for NH 3, black carbon, organic carbon, mercury Understand secondary organic aerosols: sources, chemistry. Improve modeling of fine scale features, investigate how best to downscale meteorology from global climate models, test effects of land use change. Understand aerosol-cloud interactions, characterize aerosol composition

25. Extra slides

26. Multiple linear regression to fit 1998-2008 deseasonalized EPA/AQS data for PM 2.5 : xkxk Meteorological Parameter (NCEP/NCAR Reanalysis 1 & NOAA CPC) x1x1 Surface temperature (K) x2x2 Relative humidity (10%) x3x3 Precipitation (cm/d) x4x4 Cloud cover (10%) x5x5 Geopotential height at 850 hPa (100 m) x6x6 dSLP/dt (hPa/d) x7x7 Wind speed (m/s) x8x8 E-W wind direction indicator (cosθ) x9x9 N-S wind direction indicator (sinθ) Observed Correlations of PM 2.5 with Meteorology  Observed +ve correlation with sulfate is larger by 10x  stagnation and air mass origins  Strong +ve correlation with nitrate in the west and north  agricultural NH 3 and soil NO x emissions  Strong +ve correlation with OC  VOC emissions and fires

27. 2000-2050 climate change increases JJA surface ozone: 1-5 ppb on average across US, 5-10 ppb during heat waves in Midwest Daily max 8h-avg ozone averaged in JJA (ppb) Wu et al., 2007 We define the climate change penalty as the effort required to meet air quality standards under future climate change. Effect of climate change alone Increase of summer max- 8h-avg ozone Cumulative probability (%) Max. 8-hr-avg ozone 2000s conditions 2050s climate 2050s emissions 2050s climate & emis 99 th percentile Midwest

28. We define the climate change penalty as the effort required to meet air quality goals in the future atmosphere. present-day NOx emissions + climate 40% cut in NOx + present-day climate 40% cut in NOx + 2050s climate 50% cut in NOx + 2050s climate 2000–2050 climate change implies an additional 25% effort in NOx emission controls to achieve the same ozone air quality. Wu et al., 2007 climate change penalty } Midwest surface ozone

29. Weaver et al., 2009 Models tend to agree on 2000-2050 changes in surface temperature over the United States. Most models agree that surface ozone will increase over the Northeast. Disagreement occurs elsewhere due to differences in chemistry and cloud cover change. 2000-2050 JJA surface temperature change 2000-2050 change in max daily 8-hour average ozone

30. Change in annual mean surface inorganic aerosol from 2000-2050 climate change (no change in emissions) Increase in Northeast due to increased temperature and accelerated oxidation rates Decrease in Southeast due mainly to increased precipitation. Calculation of future aerosol levels is challenging because of uncertainty in future rainfall over mid-latitudes. Also, mix of aerosol species is expected to change, so sensitivity to climate will also change. Pye et al., 2009 sulfate nitrate ammonium Present-day annual average

31. Projected increase in wildfires could affect air quality in the US. We predict future wildfires using observed relationships between meteorology and area burned for different ecosystems. 2000-2050 changes in fire season surface ozone. Perturbation due to climate change only Spracklen et al., 2009 Hudman et al, ms. 198020001990 R 2 =52% Area burned / 10 6 Ha 0.5 0.25 observations model May-Oct area burned in Pacific Northwest 1990

32. Projected increase in wildfires could affect air quality in the US. 2000-2050 change in JJA surface organic aerosol due to increased wildfires  g m -3 We have developed a fire prediction tool based on observed relationships between meteorology and area burned. Applying these relationships to GCM meteorology, we predict area burned and future emissions of wildfire pollutants. Changes in JJA surface ozone concentrations Perturbation due to climate change only Spracklen et al., 2009 Hudman et al, ms.

33. Observations of a possible relationship between trends in aerosol optical depths and surface temperature. Smoothed monthly mean AOD for sites in Europe Ruckstuhl et al., 2008 Annual mean fluxes, temperatures Anomaly of clear sky shortwave downward radiation at surface Surface temperature anomalies averaged over all sites, excluding 2003. Pinatubo +0.42 C /decade