Person: Murray, Lee Thomas
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Lee Thomas
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Murray, Lee Thomas
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Publication Optimized regional and interannual variability of lightning in a global chemical transport model constrained by LIS/OTD satellite data(Wiley-Blackwell, 2012) Murray, Lee Thomas; Jacob, Daniel; Logan, Jennifer; Hudman, Rynda C.; Koshak, William J.Nitrogen oxides (NOx≡ NO + NO2) produced by lightning make a major contribution to the global production of tropospheric ozone and OH. Lightning distributions inferred from standard convective parameterizations in global chemical transport models (CTMs) fail to reproduce observations from the Lightning Imaging Sensor (LIS) and the Optical Transient Detector (OTD) satellite instruments. We present an optimal regional scaling algorithm for CTMs to fit the lightning NOx source to the satellite lightning data in a way that preserves the coupling to deep convective transport. We show that monthly scaling using ~35 global regions significantly improves the tropical ozone simulation in the GEOS-Chem CTM as compared to a simulation unconstrained by the satellite data, and performs equally well to a simulation with local scaling. The coarse regional scaling preserves sufficient statistics in the satellite data to constrain the interannual variability (IAV) of lightning. After processing the LIS data to remove its diurnal sampling bias, we construct a monthly time series of lightning flash rates for 1998-2010 and 35ºS-35ºN. We find a correlation of IAV in tropical lightning with El Niño but not with the solar cycle or the quasi-biennial oscillation. The resulting global lightning NOx source in GEOS-Chem is 6.0 ± 0.5 Tg N a-1, compared to 5.5 ± 0.8 Tg N a-1 for the biomass burning source. Lightning NOx could have a large influence on the IAV of tropospheric ozone because it is released in the upper troposphere where ozone production is most efficient.Publication Factors Controlling Variability in the Oxidative Capacity of the Troposphere on Interannual to Interglacial Time Scales(2013-08-21) Murray, Lee Thomas; Jacob, Daniel J.; Kuang, Zhiming; Logan, JenniferThis thesis explores the natural forces controlling variability of the tropospheric oxidants on interannual to glacial-interglacial time scales. The oxidants (primarily OH and ozone) determine the lifetime of many trace gases of human interest, including air pollutants and long-lived greenhouse gases such as methane. The oxidants respond to meteorological conditions, precursor emissions (natural and anthropogenic), and surface and overhead stratospheric boundary conditions, all of which have changed since the Last Glacial Maximum (LGM; ~21ka). This dissertation first examines in mechanistic detail the effect of variability in the lightning source of nitrogen oxides \((NO_x)\) precursors on interannual variability (IAV) of the oxidants in the recent past. An optimized technique is presented to constrain the lightning \(NO_x\) source in the GEOS-Chem global chemical transport model (CTM) to time-varying satellite data from the Lightning Imaging Sensor. This constraint improves the ability of the CTM to reproduce observed IAV in 9-year (1998-2006) hindcasts of tropical ozone and OH. IAV in ozone and OH is more sensitive to lightning than to biomass burning, despite greater IAV in \(NO_x\) from the latter source. The sensitivity of OH to lightning reflects positive chemical feedbacks on ozone production, \(HO_x\) recycling, and loss frequencies. This dissertation next introduces an offline-coupled climate-biosphere-chemistry framework for determining oxidant levels at and since the LGM. Detailed simulations of tropospheric composition are performed by GEOS-Chem driven by meteorological fields from the GISS ModelE general circulation model, land cover from the BIOME4-TG global terrestrial equilibrium vegetation model, and fire emissions from the LMfire model. Time slice simulations are presented for the present day, preindustrial, and two different possible representations of the LGM climate. Sensitivity of the results to uncertainty in lightning and biomass burning emissions is tested. Though well-buffered, all simulations find net reduced oxidative capacities relative to the present day. The most important parameters for controlling tropospheric oxidants over glacial-interglacial periods are changes in overhead ozone, tropospheric \(H_2O\), and lightning. The results are discussed in the context of the ice-core record, particularly for methane.Publication Improved estimate of the policy-relevant background ozone in the United States using the GEOS-Chem global model with 1/2° × 2/3° horizontal resolution over North America(Elsevier BV, 2011) Zhang, Lin; Jacob, Daniel; Downey, Nicole V.; Wood, Dana A.; Blewitt, Doug; Carouge, Claire C.; van Donkelaar, Aaron; Jones, Dylan B.A.; Murray, Lee Thomas; Wang, YuxuanThe policy-relevant background (PRB) ozone is defined by the US Environmental Protection Agency (EPA) as the surface ozone concentration that would be present over the US in the absence of North American anthropogenic emissions. It is intended to provide a baseline for risk and exposure assessments used in setting the National Ambient Air Quality Standard (NAAQS). We present here three-year statistics (2006–2008) of PRB ozone over the US calculated using the GEOS-Chem global 3-D model of atmospheric composition with 1/2° × 2/3° horizontal resolution over North America and adjacent oceans (2° × 2.5° for the rest of the world). We also provide estimates of the US background (no anthropogenic US emissions) and natural background (no anthropogenic emissions worldwide and pre-industrial methane). Our work improves on previous GEOS-Chem PRB estimates through the use of higher model resolution, 3-year statistics, better representation of stratospheric influence, and updated emissions. PRB is particularly high in the intermountain West due to high elevation, arid terrain, and large-scale subsidence. We present for this region a detailed model evaluation showing that the model is successful in reproducing ozone exceedances up to 70 ppbv. However, the model cannot reproduce PRB-relevant exceptional events associated with wildfires or stratospheric intrusions. The mean PRB estimates for spring–summer are 27 ± 8 ppbv at low-altitude sites and 40 ± 7 ppbv at high-altitude sites. Differences between the PRB simulation and the natural simulation indicate a mean enhancement from intercontinental pollution and anthropogenic methane of 9 ppbv at low-altitude sites and 13 ppbv at high-altitude sites. The PRB is higher than average when ozone exceeds 60 ppbv, particularly in the intermountain West. Our PRB estimates are on average 4 ppbv higher than previous GEOS-Chem studies and we attribute this to higher lighting, increasing Asian emissions, and improved model resolution. Whereas previous studies found no occurrences of PRB exceeding 60 ppbv, we find here some occurrences in the intermountain West. The annual 4th-highest PRB values in the intermountain West are typically 50–60 ppbv, as compared to 35–45 ppbv in the East or on the West Coast. Such high PRB values in the intermountain West suggest that special consideration of this region may be needed if the ozone NAAQS is decreased to a value in the 60–70 ppbv range.Publication Interannual Variability in Tropical Tropospheric Ozone and OH: The Role of Lightning(Wiley-Blackwell, 2013) Murray, Lee Thomas; Logan, Jennifer; Jacob, DanielNitrogen oxide radicals (NOx) produced by lightning are natural precursors for the production of the dominant tropospheric oxidants, OH and ozone. Observations of the interannual variability (IAV) of tropical ozone and of global mean OH (from the methyl chloroform proxy) offer a window for understanding the sensitivity of ozone and OH to environmental factors. We present the results of simulations for 1998–2006 using the GEOS-Chem chemical transport model (CTM) with IAV in tropical lightning constrained by satellite observations from the Lightning Imaging Sensor. We find that this imposed IAV in lightning NOx improves the ability of the model to reproduce observed IAV in tropical ozone and OH. Lightning is far more important than biomass burning in driving the IAV of tropical ozone, even though the IAV of NOx emissions from fires is greater than that from lightning. Our results indicate that the IAV in tropospheric OH is highly sensitive to lightning relative to other emissions and suggest that lightning contributes an important fraction of the observed IAV in OH inferred from the methyl chloroform proxy. Lightning affects OH through the HO2+ NO reaction, an effect compounded by positive feedback from the resulting increase in ozone production and in CO loss. We can account in the model for the observed increase in OH in 1998–2004 and for its IAV, but the model fails to explain the OH decrease in 2004–2006. We find that stratospheric ozone plays little role in driving IAV in OH during 1998–2006, in contrast to previous studies that examined earlier periods.Publication Surface and Lightning Sources of Nitrogen Oxides over the United States: Magnitudes, Chemical Evolution, and Outflow(American Geophysical Union, 2007) Hudman, R. C.; Jacob, Daniel; Turquety, Solene; Leibensperger, Eric Michael; Murray, Lee Thomas; Wu, S.; Gilliland, A. B.; Avery, M.; Bertram, T. H.; Brune, W.; Cohen, R. C.; Dibb, J. E.; Flocke, F. M.; Fried, A.; Holloway, J.; Neuman, J. A.; Orville, R.; Perring, A.; Ren, X.; Sachse, G. W.; Singh, H. B.; Swanson, A.; Wooldridge, P. J.We use observations from two aircraft during the ICARTT campaign over the eastern United States and North Atlantic during summer 2004, interpreted with a global 3-D model of tropospheric chemistry (GEOS-Chem) to test current understanding of regional sources, chemical evolution, and export of NOx. The boundary layer NOx data provide top-down verification of a 50% decrease in power plant and industry NOx emissions over the eastern United States between 1999 and 2004. Observed NOx concentrations at 8–12 km altitude were 0.55 ± 0.36 ppbv, much larger than in previous U.S. aircraft campaigns (ELCHEM, SUCCESS, SONEX) though consistent with data from the NOXAR program aboard commercial aircraft. We show that regional lightning is the dominant source of this upper tropospheric NOx and increases upper tropospheric ozone by 10 ppbv. Simulating ICARTT upper tropospheric NOx observations with GEOS-Chem requires a factor of 4 increase in modeled NOx yield per flash (to 500 mol/flash). Observed OH concentrations were a factor of 2 lower than can be explained from current photochemical models, for reasons that are unclear. A NOy-CO correlation analysis of the fraction f of North American NOx emissions vented to the free troposphere as NOy (sum of NOx and its oxidation products) shows observed f = 16 ± 10% and modeled f = 14 ± 9%, consistent with previous studies. Export to the lower free troposphere is mostly HNO3 but at higher altitudes is mostly PAN. The model successfully simulates NOy export efficiency and speciation, supporting previous model estimates of a large U.S. anthropogenic contribution to global tropospheric ozone through PAN export.Publication Biogenic Versus Anthropogenic Sources of CO in the United States(American Geophysical Union, 2008) Hudman, R.C.; Murray, Lee Thomas; Jacob, Daniel; Millet, D.B.; Turquety, S.; Wu, S.; Blake, D.R.; Goldstein, A.H.; Holloway, J.; Sachse, G.W.Aircraft observations of carbon monoxide (CO) from the ICARTT campaign over the eastern United States in summer 2004 (July 1–August 15), interpreted with a global 3-D model of tropospheric chemistry (GEOS-Chem), show that the national anthropogenic emission inventory from the U.S. Environmental Protection Agency (93 Tg CO y−1) is too high by 60% in summer. Our best estimate of the CO anthropogenic source for the ICARTT period is 6.4 Tg CO, including 4.6 Tg from direct emission and 1.8 Tg CO from oxidation of anthropogenic volatile organic compounds (VOCs). The biogenic CO source for the same period from the oxidation of isoprene and other biogenic VOCs is 8.3 Tg CO, and is independently constrained by ICARTT observations of formaldehyde (HCHO). Anthropogenic emissions of CO in the U.S. have decreased to the point that they are now lower than the biogenic source in summer.Publication North American Influence on Tropospheric Ozone and the Effects of Recent Emission Reductions: Constraints from ICARTT Observations(American Geophysical Union, 2009) Hudman, R.C.; Murray, Lee Thomas; Jacob, Daniel; Turquety, S.; Wu, S.; Millet, D.B.; Avery, M.; Goldstein, A.H.; Holloway, J.We use observations from the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) campaign over eastern North America in summer 2004, interpreted with a global 3‐D model of tropospheric chemistry (GEOS‐Chem), to improve and update estimates of North American influence on global tropospheric ozone and the effect of recent U.S. anthropogenic reductions on surface ozone pollution. We find that the 50% decrease in U.S. stationary NOx sources since 1999 has decreased mean U.S. boundary layer ozone concentrations by 6–8 ppbv in the southeast and 4–6 ppbv in the Midwest. The observed dO3/dCO molar enhancement ratio in the U.S. boundary layer during ICARTT was 0.46 mol mol−1, larger than the range of 0.3–0.4 from studies in the early 1990s, possibly reflecting the decrease in the NOx/CO emission ratio as well as an increase in the ozone production efficiency per unit NOx. North American NOx emissions during summer 2004 as constrained by the ICARTT observations (0.72 Tg N fossil fuel, 0.11 Tg N biomass burning, 0.28 Tg N lightning for 1 July to 15 August) enhanced the hemispheric tropospheric ozone burden by 12.4%, with comparable contributions from fossil fuel and lightning (5–6%), but only 1% from biomass burning emissions despite 2004 being a record fire year over Alaska and western Canada.