Person: Yantosca, Robert
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Yantosca
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Yantosca, Robert
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Publication Source Attribution and Interannual Variability of Arctic Pollution in Spring Constrained by Aircraft (ARCTAS, ARCPAC) and Satellite (AIRS) Observations of Carbon Monoxide(European Geosciences Union, 2010) Fisher, J. A.; Jacob, Daniel; Purdy, M. T.; Kopacz, M.; Le Sager, P; Carouge, C.; Holmes, C. D.; Yantosca, Robert; Batchelor, R. L.; Strong, K.; Diskin, G. S.; Fuelberg, H. E.; Holloway, J. S.; Hyer, E. J.; McMillan, W. W.; Warner, J.; Streets, D. G.; Zhang, Q.; Wang, Y.; Wu, S.We use aircraft observations of carbon monoxide (CO) from the NASA ARCTAS and NOAA ARCPAC campaigns in April 2008 together with multiyear (2003–2008) CO satellite data from the AIRS instrument and a global chemical transport model (GEOS-Chem) to better understand the sources, transport, and interannual variability of pollution in the Arctic in spring. Model simulation of the aircraft data gives best estimates of CO emissions in April 2008 of \(26 Tg month^{−1}\) for Asian anthropogenic, 9.4 for European anthropogenic, 4.1 for North American anthropogenic, 15 for Russian biomass burning (anomalously large that year), and 23 for Southeast Asian biomass burning. We find that Asian anthropogenic emissions are the dominant source of Arctic CO pollution everywhere except in surface air where European anthropogenic emissions are of similar importance. Russian biomass burning makes little contribution to mean CO (reflecting the long CO lifetime) but makes a large contribution to CO variability in the form of combustion plumes. Analysis of two pollution events sampled by the aircraft demonstrates that AIRS can successfully observe pollution transport to the Arctic in the mid-troposphere. The 2003–2008 record of CO from AIRS shows that interannual variability averaged over the Arctic cap is very small. AIRS CO columns over Alaska are highly correlated with the Ocean Niño Index, suggesting a link between El Niño and Asian pollution transport to the Arctic. AIRS shows lower-than-average CO columns over Alaska during April 2008, despite the Russian fires, due to a weakened Aleutian Low hindering transport from Asia and associated with the moderate 2007–2008 La Niña. This suggests that Asian pollution influence over the Arctic may be particularly large under strong El Niño conditions.Publication Global Estimates of CO Sources with High Resolution by Adjoint Inversion of Multiple Satellite Datasets (MOPITT, AIRS, SCIAMACHY, TES)(European Geosciences Union, 2010) Kopacz, M.; Jacob, Daniel; Fisher, John; Logan, Jennifer; Zhang, L.; Megretskaia, Inna; Yantosca, Robert; Singh, K.; Henze, D. K.; Burrows, J. P.; Buchwitz, M.; Khlystova, I.; McMillan, W. W.; Gille, J. C.; Edwards, D. P.; Eldering, A.; Thouret, V.; Nedelec, P.We combine CO column measurements from the MOPITT, AIRS, SCIAMACHY, and TES satellite instruments in a full-year (May 2004–April 2005) global inversion of CO sources at 4°×5° spatial resolution and monthly temporal resolution. The inversion uses the GEOS-Chem chemical transport model (CTM) and its adjoint applied to MOPITT, AIRS, and SCIAMACHY. Observations from TES, surface sites (NOAA/GMD), and aircraft (MOZAIC) are used for evaluation of the a posteriori solution. Using GEOS-Chem as a common intercomparison platform shows global consistency between the different satellite datasets and with the in situ data. Differences can be largely explained by different averaging kernels and a priori information. The global CO emission from combustion as constrained in the inversion is \(1350 Tg a^{−1}\). This is much higher than current bottom-up emission inventories. A large fraction of the correction results from a seasonal underestimate of CO sources at northern mid-latitudes in winter and suggests a larger-than-expected CO source from vehicle cold starts and residential heating. Implementing this seasonal variation of emissions solves the long-standing problem of models underestimating CO in the northern extratropics in winter-spring. A posteriori emissions also indicate a general underestimation of biomass burning in the GFED2 inventory. However, the tropical biomass burning constraints are not quantitatively consistent across the different datasets.Publication Gas-Particle Partitioning of Atmospheric Hg(II) and Its Effect on Global Mercury Deposition(Copernicus GmbH, 2012) Amos, Helen; Jacob, Daniel; Holmes, C. D.; Fisher, Jenny; Wang, Qiaoqiao; Yantosca, Robert; Corbitt, Elizabeth Sturges; Galarneau, E.; Rutter, A. P.; Gustin, M. S.; Steffen, A.; Schauer, J. J.; Graydon, J. A.; Louis, V. L. St.; Talbot, R. W.; Edgerton, E. S.; Zhang, Y.; Sunderland, ElynorAtmospheric deposition of Hg(II) represents a major input of mercury to surface environments. The phase of Hg(II) (gas or particle) has important implications for deposition. We use long-term observations of reactive gaseous mercury (RGM, the gaseous component of Hg(II)), particle-bound mercury (PBM, the particulate component of Hg(II)), fine particulate matter (PM2.5), and temperature (T) at five sites in North America to derive an empirical gas-particle partitioning relationship log10(K−1) = (10±1)–(2500±300)/T where K = (PBM/PM2.5)/RGM with PBM and RGM in common mixing ratio units, PM2.5 in μg m−3, and T in K. This relationship is within the range of previous work but is based on far more extensive data from multiple sites. We implement this empirical relationship in the GEOS-Chem global 3-D Hg model to partition Hg(II) between the gas and particle phases. The resulting gas-phase fraction of Hg(II) ranges from over 90 % in warm air with little aerosol to less than 10 % in cold air with high aerosol. Hg deposition to high latitudes increases because of more efficient scavenging of particulate Hg(II) by precipitating snow. Model comparison to Hg observations at the North American surface sites suggests that subsidence from the free troposphere (warm air, low aerosol) is a major factor driving the seasonality of RGM, while elevated PBM is mostly associated with high aerosol loads. Simulation of RGM and PBM at these sites is improved by including fast in-plume reduction of Hg(II) emitted from coal combustion and by assuming that anthropogenic particulate Hg(p) behaves as semi-volatile Hg(II) rather than as a refractory particulate component. We improve the simulation of Hg wet deposition fluxes in the US relative to a previous version of GEOS-Chem; this largely reflects independent improvement of the washout algorithm. The observed wintertime minimum in wet deposition fluxes is attributed to inefficient snow scavenging of gas-phase Hg(II).Publication The Role of the Ocean in the Global Atmospheric Budget of Acetone(Wiley-Blackwell, 2012) Fischer, E. V.; Jacob, Daniel; Millet, D. B.; Yantosca, Robert; Mao, J.[1] Acetone is one of the most abundant carbonyl compounds in the atmosphere and it plays an important role in atmospheric chemistry. The role of the ocean in the global atmospheric acetone budget is highly uncertain, with past studies reaching opposite conclusions as to whether the ocean is a source or sink. Here we use a global 3-D chemical transport model (GEOS-Chem) simulation of atmospheric acetone to evaluate the role of air-sea exchange in the global budget. Inclusion of updated (slower) photolysis loss in the model means that a large net ocean source is not needed to explain observed acetone in marine air. We find that a simulation with a fixed seawater acetone concentration of 15 nM based on observations can reproduce the observed global patterns of atmospheric concentrations and air-sea fluxes. The Northern Hemisphere oceans are a net sink for acetone while the tropical oceans are a net source. On a global scale the ocean is in near-equilibrium with the atmosphere. Prescribing an ocean concentration of acetone as a boundary condition in the model assumes that ocean concentrations are controlled by internal production and loss, rather than by air-sea exchange. An implication is that the ocean plays a major role in controlling atmospheric acetone. This hypothesis needs to be tested by better quantification of oceanic acetone sources and sinks.Publication An Improved Global Model for Air-Sea Exchange of Mercury: High Concentrations over the North Atlantic(American Chemical Society (ACS), 2010) Soerensen, Anne; Sunderland, Elynor; Holmes, Christopher D.; Jacob, Daniel; Yantosca, Robert; Skov, Henrik; Christensen, Jesper H.; Strode, Sarah A.; Mason, Robert P.We develop an improved treatment of the surface ocean in the GEOS-Chem global 3-D biogeochemical model for mercury (Hg). We replace the globally uniform subsurface ocean Hg concentrations used in the original model with basin-specific values based on measurements. Updated chemical mechanisms for Hg0/HgII redox reactions in the surface ocean include both photochemical and biological processes, and we improved the parametrization of particle-associated Hg scavenging. Modeled aqueous Hg concentrations are consistent with limited surface water observations. Results more accurately reproduce high-observed MBL concentrations over the North Atlantic (NA) and the associated seasonal trends. High seasonal evasion in the NA is driven by inputs from Hg enriched subsurface waters through entrainment and Ekman pumping. Globally, subsurface waters account for 40% of Hg inputs to the ocean mixed layer, and 60% is from atmospheric deposition. Although globally the ocean is a net sink for 3.8 Mmol Hg y−1, the NA is a net source to the atmosphere, potentially due to enrichment of subsurface waters with legacy Hg from historical anthropogenic sources.Publication Convective outflow of South Asian pollution: A global CTM simulation compared with EOS MLS observations(Wiley-Blackwell, 2005) Li, Qinbin; Jiang, Jonathan H.; Wu, Dong L.; Read, William G.; Livesey, Nathaniel J.; Waters, Joe W.; Zhang, Yongsheng; Wang, Bin; Filipiak, Mark J.; Davis, Cory P.; Turquety, Solene; Wu, Shiliang; Park, Rokjin J.; Yantosca, Robert; Jacob, DanielA global 3-D chemical transport model is used to analyze observations of carbon monoxide (CO) and upper tropospheric clouds from the EOS Microwave Limb Sounder (MLS). MLS observations during 25 August–6 September 2004 reveal elevated CO and dense high clouds in the upper troposphere over the Tibetan plateau and southwest China, collocating with the upper level Tibetan anticyclone. Model simulations indicate the transport of boundary layer pollution by Asian summer monsoon (ASM) convection and orographic lifting to the upper troposphere over South Asia, where simulated distributions of CO resemble MLS observations. Model results also show elevated aerosols in the anticyclone region. Analysis of model simulated CO and aerosols indicate that the Tibetan anticyclone could ‘trap’ anthropogenic emissions lifted from northeast India and southwest China. These aerosols may be responsible for the formation of some of the dense high clouds.Publication Global and regional decreases in tropospheric oxidants from photochemical effects of aerosols(Wiley-Blackwell, 2003) Martin, Randall V.; Jacob, Daniel; Yantosca, Robert; Chin, Mian; Ginoux, PaulWe evaluate the sensitivity of tropospheric OH, O3, and O3 precursors to photochemical effects of aerosols not usually included in global models: (1) aerosol scattering and absorption of ultraviolet radiation and (2) reactive uptake of HO2, NO2, and NO3. Our approach is to couple a global 3-D model of tropospheric chemistry (GEOS-CHEM) with aerosol fields from a global 3-D aerosol model (GOCART). Reactive uptake by aerosols is computed using reaction probabilities from a recent review (γHO2 = 0.2, γNO2 = 10−4, γNO3 = 10−3). Aerosols decrease the O3 [RIGHTWARDS ARROW] O(1D) photolysis frequency by 5–20% at the surface throughout the Northern Hemisphere (largely due to mineral dust) and by a factor of 2 in biomass burning regions (largely due to black carbon). Aerosol uptake of HO2 accounts for 10–40% of total HOx radical (≡ OH + peroxy) loss in the boundary layer over polluted continental regions (largely due to sulfate and organic carbon) and for more than 70% over tropical biomass burning regions (largely due to organic carbon). Uptake of NO2 and NO3 accounts for 10–20% of total HNO3 production over biomass burning regions and less elsewhere. Annual mean OH concentrations decrease by 9% globally and by 5–35% in the boundary layer over the Northern Hemisphere. Simulated CO increases by 5–15 ppbv in the remote Northern Hemisphere, improving agreement with observations. Simulated boundary layer O3 decreases by 15–45 ppbv over India during the biomass burning season in March and by 5–9 ppbv over northern Europe in August, again improving comparison with observations. We find that particulate matter controls would increase surface O3 over Europe and other industrial regions.Publication Atmospheric Peroxyacetyl Nitrate (PAN): A Global Budget and Source Attribution(Copernicus GmbH, 2014) Fischer, E. V.; Jacob, Daniel; Yantosca, Robert; Sulprizio, Melissa; Millet, D. B.; Mao, J.; Paulot, F.; Singh, H. B.; Roiger, A.; Ries, L.; Talbot, R. W.; Dzepina, K.; Pandey Deolal, S.Peroxyacetyl nitrate (PAN) formed in the atmospheric oxidation of non-methane volatile organic compounds (NMVOCs) is the principal tropospheric reservoir for nitrogen oxide radicals \((NO_x = NO + NO_2)\). PAN enables the transport and release of \(NO_x\) to the remote troposphere with major implications for the global distributions of ozone and OH, the main tropospheric oxidants. Simulation of PAN is a challenge for global models because of the dependence of PAN on vertical transport as well as complex and uncertain NMVOC sources and chemistry. Here we use an improved representation of NMVOCs in a global 3-D chemical transport model (GEOS-Chem) and show that it can simulate PAN observations from aircraft campaigns worldwide. The immediate carbonyl precursors for PAN formation include acetaldehyde (44% of the global source), methylglyoxal (30%), acetone (7%), and a suite of other isoprene and terpene oxidation products (19%). A diversity of NMVOC emissions is responsible for PAN formation globally including isoprene (37%) and alkanes (14%). Anthropogenic sources are dominant in the extratropical Northern Hemisphere outside the growing season. Open fires appear to play little role except at high northern latitudes in spring, although results are very sensitive to plume chemistry and plume rise. Lightning \(NO_x\) is the dominant contributor to the observed PAN maximum in the free troposphere over the South Atlantic.Publication A global three-dimensional model analysis of the atmospheric budgets of HCN and CH 3 CN: Constraints from aircraft and ground measurements(Wiley-Blackwell, 2003) Li, Qinbin; Jacob, Daniel; Yantosca, Robert; Heald, Colette; Singh, Hanwant; Koike, Makoto; Zhao, Yongjing; Sachse, Glen; Streets, DavidWe construct global atmospheric budgets of HCN and CH3CN through a three-dimensional (3-D) model simulation of the HCN-CH3CN-CO system constrained and evaluated with aircraft observations from the Transport and Chemical Evolution Over the Pacific (TRACE-P) mission over the NW Pacific in February–April 2001. Observed background vertical gradients of HCN and CH3CN imply a dominant ocean sink for both gases, with deposition velocity of 0.13 cm s−1 for both and saturation ratios of 0.79 for HCN and 0.88 for CH3CN. Observations for both gases in the free troposphere imply a dominant source from biomass burning. Enhancement of HCN observed in Chinese urban plumes is attributed tentatively to residential coal burning. Biomass burning and residential coal burning emission ratios relative to CO of 0.27% and 1.6%, respectively, for HCN, and of 0.20% and 0.25%, respectively, for CH3CN, are consistent with observations in biomass burning and Chinese urban plumes. They provide the best model simulation of the ensemble of TRACE-P observations including vertical profiles and HCN-CH3CN-CO correlations. They also allow successful simulation of the long-term observations of HCN columns at sites in the Northern Hemisphere, and of the CH3CN vertical distribution observed over the northern Indian Ocean. Global biomass burning and Asian residential coal burning sources in the model are 0.63 and 0.2 Tg N yr−1, respectively, for HCN and 0.47 and 0.03 Tg N yr−1, respectively, for CH3CN. Ocean uptake is the dominant sink for both gases, with oxidation by OH representing an additional minor sink. The resulting tropospheric lifetimes are 5.3 months for HCN and 5.8 months for CH3CN. The model predicts very low HCN and CH3CN concentrations at high southern latitudes, reflecting the assumption of a uniform saturation ratio for ocean uptake; observations in that region are needed. In the free troposphere, the dominance of biomass burning sources (70–85% for HCN and 90–95% for CH3CN) implies that both gases can be used as biomass burning tracers. In the boundary layer, CH3CN appears to be a better biomass burning tracer. More work is needed to identify the origin of the Chinese urban source of HCN.Publication Transport pathways for Asian pollution outflow over the Pacific: Interannual and seasonal variations(Wiley-Blackwell, 2003) Liu, Hongyu; Jacob, Daniel; Bey, Isabelle; Yantosca, Robert; Duncan, Bryan; Sachse, GlenThe meteorological pathways contributing to Asian pollution outflow over the Pacific are examined with a global three-dimensional model analysis of CO observations from the Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission (February–April 2001). The model is used also to place the TRACE-P observations in an interannual (1994–2001) and seasonal context. The major process driving Asian pollution outflow in spring is frontal lifting ahead of southeastward-moving cold fronts (the leading edge of cold surges) and transport in the boundary layer behind the cold fronts. Orographic lifting over central and eastern China combines with the cold fronts to promote the transport of Chinese pollution to the free troposphere. Outflow of seasonal biomass burning in Southeast Asia during spring takes place mostly by deep convection but also by northeastward transport and frontal lifting, mixing with the anthropogenic outflow. Boundary layer outflow over the western Pacific is largely devoid of biomass burning influence. European and African (biomass burning) plumes in Asian outflow during TRACE-P were weak (<60 ppbv and 20 ppbv CO, respectively) and were not detectable in the observations because of superposition of the much larger Asian pollution signal. Spring 2001 (La Niña) was characterized by unusually frequent cold surge events in the Asian Pacific rim and strong convection in Southeast Asia, leading to unusually strong boundary layer outflow of anthropogenic emissions and convective outflow of biomass burning emissions in the upper troposphere. The Asian outflow flux of CO to the Pacific is found to vary seasonally by a factor of 3–4 (maximum in March and minimum in summer). The March maximum results from frequent cold surge events and seasonal biomass burning emissions.