J. G. Levine

Forest fire plumes over the North Atlantic: p‐TOMCAT model simulations with aircraft and satellite measurements from the ITOP/ICARTT campaign

[1] Intercontinental Transport of Ozone and Precursors (ITOP) (part of International Consortium for Atmospheric Research on Transport and Transformation (ICARTT)) was an intense research effort to measure long-range transport of pollution across the North Atlantic and its impact on O3 production. During the aircraft campaign plumes were encountered containing large concentrations of CO plus other tracers and aerosols from forest fires in Alaska and Canada. A chemical transport model, p-TOMCAT, and new biomass burning emissions inventories are used to study the emissions long-range transport and their impact on the troposphere O3 budget. The fire plume structure is modeled well over long distances until it encounters convection over Europe. The CO values within the simulated plumes closely match aircraft measurements near North America and over the Atlantic and have good agreement with MOPITT CO data. O3 and NOx values were initially too great in the model plumes. However, by including additional vertical mixing of O3 above the fires, and using a lower NO2/CO emission ratio (0.008) for boreal fires, O3 concentrations are reduced closer to aircraft measurements, with NO2 closer to SCIAMACHY data. Too little PAN is produced within the simulated plumes, and our VOC scheme’s simplicity may be another reason for O3 and NOx modeldata discrepancies. In the p-TOMCAT simulations the fire emissions lead to increased tropospheric O3 over North America, the north Atlantic and western Europe from photochemical production and transport. The increased O3 over the Northern Hemisphere in the simulations reaches a peak in July 2004 in the range 2.0 to 6.2 Tg over a baseline of about 150 Tg.

Reconciling the changes in atmospheric methane sources and sinks between the Last Glacial Maximum and the pre-industrial era

We know from the ice record that the concentration of atmospheric methane, [CH4], at the Last Glacial Maximum (LGM) was roughly half that in the pre-industrial era (PI), buthow much of the difference was source-driven, and how much was sink-driven, remains uncertain. Recent developments include: a higher estimate of the LGM-PI change in methane emissions from wetlands―the dominant, natural methane source; and the possible recycling of OH consumed in isoprene oxidation―the principal methane sink. Here, in view of these developments, we use an atmospheric chemistry-transport model to re-examine the main factors affecting OH during this period: changes in air temperature and emissions of non-methane volatile organic compounds from vegetation. We find that their net effect was negligible(with and without an OH recycling mechanism), implyingthe change in [CH4] was almost entirely source driven―a conclusion that, though subject to significant uncertainties,can be reconciled with recent methane source estimates.

Sea salt as an ice core proxy for past sea ice extent: a process-based model study

Sea ice is a reflection of, and a feedback on, the Earths climate. We explore here, using a global atmospheric chemistry-transport model, the use of sea salt in Antarctic ice cores to obtain continuous long-term, regionally integrated records of past sea ice extent, synchronous with ice core records of climate. The model includes the production, transport, and deposition of sea salt aerosol from the open ocean and “blowing snow” on sea ice. Under current climate conditions, we find that meteorology, not sea ice extent, is the dominant control on the atmospheric concentration of sea salt reaching coastal and continental Antarctic sites on interannual timescales. However, through a series of idealized sensitivity experiments, we demonstrate that sea salt has potential as a proxy for larger changes in sea ice extent (e.g., glacial-interglacial). Treating much of the sea ice under glacial conditions as a source of salty blowing snow, we demonstrate that the increase in sea ice extent alone (without changing the meteorology) could drive, for instance, a 68% increase in atmospheric sea salt concentration at the site of the Dome C ice core, which exhibits an approximate twofold glacial increase in sea salt flux. We also show how the sensitivity of this potential proxy decreases toward glacial sea ice extent—the basis of an explanation previously proposed for the lag observed between changes in sea salt flux and δD (an ice core proxy for air temperature) at glacial terminations. The data thereby permit simultaneous changes in sea ice extent and climate.

Controls on the tropospheric oxidizing capacity during an idealized Dansgaard‐Oeschger event, and their implications for the rapid rises in atmospheric methane during the last glacial period

The ice core record reveals large variations in the concentration of atmospheric methane, CH4, over the last 800 kyr. Amongst the most striking natural features are the large, rapid rises in CH4, of 100-200 ppbv, on timescales of less than 100 years, at the beginning of Dansgaard-Oeschger (D-O) events during the last glacial period (21-110 kyr before present). Despite the potential insight they could offer into the likelihood of future rapid rises in CH4, the relative roles of changes in methane sources and sinks during D-O events have been little explored. Here, we use a global atmospheric chemistry-transport model to explore-for the first time, in a process-based fashion-controls on the oxidizing capacity during an idealized D-O event that features a characteristically rapid rise in CH4. We find that the two controls previously identified in the literature as having had significant (though opposing) influences on the oxidizing capacity between glacial and interglacial periods-changes in air temperature and emissions of non-methane volatile organic compounds from vegetation-offset one another between idealized Heinrich stadial and Greenland interstadial states. The result is, the net change in oxidizing capacity is very small, implying the rapid rises in CH4 at the beginning of D-O events were almost entirely source-driven. This poses a challenge to earth-system models-to generate a sufficiently large increase in methane emissions in response to a simulated D-O event, via a more realistic freshwater forcing impacting the strength of the Atlantic meridional overturning circulation or, possibly, other climate-change mechanisms. Citation: Levine, J. G., E. W. Wolff, P. O. Hopcroft, and P. J. Valdes (2012), Controls on the tropospheric oxidizing capacity during an idealized Dansgaard-Oeschger event, and their implications for the rapid rises in atmospheric methane during the last glacial period, Geophys. Res. Lett., 39, L12805, doi:10.1029/2012GL051866.

The role of atomic chlorine in glacial-interglacial changes in the carbon-13 content of atmospheric methane

The ice-core record of the carbon-13 content of atmospheric methane (δ13CH4) has largely been used to constrain past changes in methane sources. The aim of this paper is to explore, for the first time, the contribution that changes in the strength of a minor methane sink―oxidation by atomic chlorine in the marine boundary layer (ClMBL)―could make to changes in δ13CH4 on glacial-interglacial timescales. Combining wind and temperature data from a variety of general circulation models with a simple formulation for the concentration of ClMBL, we find that changes in the strength of this sink, driven solely by changes in the atmospheric circulation, could have been responsible for changes in δ13CH4 of the order of 10% of the glacial-interglacial difference observed. We thus highlight the need to quantify past changes in the strength of this sink, including those relating to changes in the sea-ice source of sea salt aerosol.

Detection of a gas flaring signature in the AERONET optical properties of aerosols at a tropical station in West Africa

The West African region, with its peculiar climate and atmospheric dynamics, is a prominent source of aerosols. Reliable and long-term in situ measurements of aerosol properties are not readily available across the region. In this study, Version 2 Level 1.5 Aerosol Robotic Network (AERONET) data were used to study the absorption and size distribution properties of aerosols from dominant sources identified by trajectory analysis. The trajectory analysis was used to define four sources of aerosols over a 10 year period. Sorting the AERONET aerosol retrievals by these putative sources, the hypothesis that there exists an optically distinct gas flaring signal was tested. Dominance of each source cluster varies with season: desert-dust (DD) and biomass burning (BB) aerosols are dominant in months prior to the West African Monsoon (WAM); urban (UB) and gas flaring (GF) aerosol are dominant during the WAM months. BB aerosol, with single scattering albedo (SSA) at 675 nm value of 0.86 ± 0.03 and GF aerosol with SSA (675 nm) value of 0.9 ± 0.07, is the most absorbing of the aerosol categories. The range of Absorption Angstrӧm Exponent (AAE) for DD, BB, UB and GF classes are 1.99 ± 0.35, 1.45 ± 0.26, 1.21 ± 0.38 and 0.98 ± 0.25, respectively, indicating different aerosol composition for each source. The AAE (440–870 nm) and Angstrӧm Exponent (AE) (440–870 nm) relationships further show the spread and overlap of the variation of these optical and microphysical properties, presumably due in part to similarity in the sources of aerosols and in part, due to mixing of air parcels from different sources en route to the measurement site.

Forest fire plumes over the North Atlantic: p-TOMCAT model simulations with aircraft and satellite measurements from the ITOP/ICARTT campaign

[1] Intercontinental Transport of Ozone and Precursors (ITOP) (part of International Consortium for Atmospheric Research on Transport and Transformation (ICARTT)) was an intense research effort to measure long-range transport of pollution across the North Atlantic and its impact on O3 production. During the aircraft campaign plumes were encountered containing large concentrations of CO plus other tracers and aerosols from forest fires in Alaska and Canada. A chemical transport model, p-TOMCAT, and new biomass burning emissions inventories are used to study the emissions long-range transport and their impact on the troposphere O3 budget. The fire plume structure is modeled well over long distances until it encounters convection over Europe. The CO values within the simulated plumes closely match aircraft measurements near North America and over the Atlantic and have good agreement with MOPITT CO data. O3 and NOx values were initially too great in the model plumes. However, by including additional vertical mixing of O3 above the fires, and using a lower NO2/CO emission ratio (0.008) for boreal fires, O3 concentrations are reduced closer to aircraft measurements, with NO2 closer to SCIAMACHY data. Too little PAN is produced within the simulated plumes, and our VOC scheme’s simplicity may be another reason for O3 and NOx modeldata discrepancies. In the p-TOMCAT simulations the fire emissions lead to increased tropospheric O3 over North America, the north Atlantic and western Europe from photochemical production and transport. The increased O3 over the Northern Hemisphere in the simulations reaches a peak in July 2004 in the range 2.0 to 6.2 Tg over a baseline of about 150 Tg.