Theoretical and global scale model studies of the atmospheric sulfur/aerosol system

The primary focus during the third-phase of our on-going multi-year research effort has been on 3 activities. These are: (1) a global-scale model study of the anthropogenic component of the tropospheric sulfur cycle; (2) process-scale model studies of the factors influencing the distribution of aerosols in the remote marine atmosphere; and (3) an investigation of the mechanism of the OH-initiated oxidation of DMS in the remote marine boundary layer. In this paper, we describe in more detail our research activities in each of these areas. A major portion of our activities during the fourth and final phase of this project will involve the preparation and submission of manuscripts describing the results from our model studies of marine boundary-layer aerosols and DMS-oxidation mechanisms

Continental-Scale Partitioning of Fire Emissions During the 1997 to 2001 El Niño/La Niña Period

During the 1997 to 1998 El Niño, drought conditions triggered widespread increases in fire activity, releasing CH_4 and CO_2 to the atmosphere. We evaluated the contribution of fires from different continents to variability in these greenhouse gases from 1997 to 2001, using satellite-based estimates of fire activity, biogeochemical modeling, and an inverse analysis of atmospheric CO anomalies. During the 1997 to 1998 El Niño, the fire emissions anomaly was 2.1 ± 0.8 petagrams of carbon, or 66 ± 24% of the CO_2 growth rate anomaly. The main contributors were Southeast Asia (60%), Central and South America (30%), and boreal regions of Eurasia and North America (10%)

Top-down estimates of global CO sources using MOPITT measurements

We present a synthesis inversion of CO emissions from various geographical regions and for various source categories for the year 2000 using CO retrievals from the MOPITT (Measurements of Pollution in the Troposphere) instrument. We find a large discrepancy between our top‐down estimates and recent bottom‐up estimates of CO emissions from fossil fuel/biofuel (FFBF) use in Asia. A key conclusion of this study is that CO emissions in East Asia (EAS) are about a factor of 1.8–2 higher than recent bottom‐up estimates

Top-down estimate of a large source of atmospheric carbon monoxide associated with fuel combustion in Asia

We simulate the oceanic and atmospheric distribution of methyl iodide (CH3I) with a global 3-D model driven by assimilated meteorological observations from the Goddard Earth Observing System of the NASA Data Assimilation Office and coupled to an oceanic mixed layer model. A global compilation of atmospheric and oceanic observations is used to constrain and evaluate the simulation. Seawater CH3I(aq) in the model is produced photochemically from dissolved organic carbon, and is removed by reaction with Cl− and emission to the atmosphere. The net oceanic emission to the atmosphere is 214 Gg yr−1. Small terrestrial emissions from rice paddies, wetlands, and biomass burning are also included in the model. The model captures 40% of the variance in the observed seawater CH3I(aq) concentrations. Simulated concentrations at midlatitudes in summer are too high, perhaps because of a missing biological sink of CH3I(aq). We define a marine convection index (MCI) as the ratio of upper tropospheric (8–12 km) to lower tropospheric (0–2.5 km) CH3I concentrations averaged over coherent oceanic regions. The MCI in the observations ranges from 0.11 over strongly subsiding regions (southeastern subtropical Pacific) to 0.40 over strongly upwelling regions (western equatorial Pacific). The model reproduces the observed MCI with no significant global bias (offset of only +11%) but accounts for only 15% of its spatial and seasonal variance. The MCI can be used to test marine convection in global models, complementing the use of radon-222 as a test of continental convection.Engineering and Applied Science

An assessment of high carbon stock and high conservation value approaches to sustainable oil palm cultivation in Gabon

Industrial-scale oil palm cultivation is rapidly expanding in Gabon, where it has the potential to drive economic growth, but also threatens forest, biodiversity and carbon resources. The Gabonese government is promoting an ambitious agricultural expansion strategy, while simultaneously committing to minimize negative environmental impacts of oil palm agriculture. This study estimates the extent and location of suitable land for oil palm cultivation in Gabon, based on an analysis of recent trends in plantation permitting. We use the resulting suitability map to evaluate two proposed approaches to minimizing negative environmental impacts: a High Carbon Stock (HCS) approach, which emphasizes forest protection and climate change mitigation, and a High Conservation Value (HCV) approach, which focuses on safeguarding biodiversity and ecosystems. We quantify the forest area, carbon stock, and biodiversity resources protected under each approach, using newly developed maps of priority species distributions and forest biomass for Gabon. We find 2.7–3.9 Mha of suitable or moderately suitable land that avoid HCS areas, 4.4 million hectares (Mha) that avoid HCV areas, and 1.2–1.7 Mha that avoid both. This suggests that Gabon's oil palm production target could likely be met without compromising important ecosystem services, if appropriate safeguards are put in place. Our analysis improves understanding of suitability for oil palm in Gabon, determines how conservation strategies align with national targets for oil palm production, and informs national land use planning

Predicting Fire Season Severity in South America Using Sea Surface Temperature Anomalies

Fires in South America cause forest degradation and contribute to carbon emissions associated with land use change. Here we investigated the relationship between year-to-year changes in satellite-derived estimates of fire activity in South America and sea surface temperature (SST) anomalies. We found that the Oceanic Ni o Index (ONI) was correlated with interannual fire activity in the eastern Amazon whereas the Atlantic Multidecadal Oscillation (AMO) index was more closely linked with fires in the southern and southwestern Amazon. Combining these two climate indices, we developed an empirical model that predicted regional annual fire season severity (FSS) with 3-5 month lead times. Our approach provides the foundation for an early warning system for forecasting the vulnerability of Amazon forests to fires, thus enabling more effective management with benefits for mitigation of greenhouse gas and air pollutant emissions

Separating the influence of temperature, drought, and fire on interannual variability in atmospheric CO 2

The response of the carbon cycle in prognostic Earth system models (ESMs) contributes significant uncertainty to projections of global climate change. Quantifying contributions of known drivers of interannual variability in the growth rate of atmospheric carbon dioxide (CO 2 ) is important for improving the representation of terrestrial ecosystem processes in these ESMs. Several recent studies have identified the temperature dependence of tropical net ecosystem exchange (NEE) as a primary driver of this variability by analyzing a single, globally averaged time series of CO 2 anomalies. Here we examined how the temporal evolution of CO 2 in different latitude bands may be used to separate contributions from temperature stress, drought stress, and fire emissions to CO 2 variability. We developed atmospheric CO 2 patterns from each of these mechanisms during 1997–2011 using an atmospheric transport model. NEE responses to temperature, NEE responses to drought, and fire emissions all contributed significantly to CO 2 variability in each latitude band, suggesting that no single mechanism was the dominant driver. We found that the sum of drought and fire contributions to CO 2 variability exceeded direct NEE responses to temperature in both the Northern and Southern Hemispheres. Additional sensitivity tests revealed that these contributions are masked by temporal and spatial smoothing of CO 2 observations. Accounting for fires, the sensitivity of tropical NEE to temperature stress decreased by 25% to 2.9 ± 0.4 Pg C yr −1  K −1 . These results underscore the need for accurate attribution of the drivers of CO 2 variability prior to using contemporary observations to constrain long‐term ESM responses. Key Points Accurate attribution of CO 2 variability is required to constrain coupled models Combined influence of drought and fire exceed ecosystem responses to temperature Temporal and spatial smoothing of CO 2 observations masks variability from firePeer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/109962/1/gbc20215.pd

Top-down estimates of global CO sources using MOPITT measurements

We present a synthesis inversion of CO emissions from various geographical regions and for various source categories for the year 2000 using CO retrievals from the MOPITT (Measurements of Pollution in the Troposphere) instrument. We find a large discrepancy between our top‐down estimates and recent bottom‐up estimates of CO emissions from fossil fuel/biofuel (FFBF) use in Asia. A key conclusion of this study is that CO emissions in East Asia (EAS) are about a factor of 1.8–2 higher than recent bottom‐up estimates

Global impact of nitrate photolysis in sea-salt aerosol on NOx, OH, and O3 in the marine boundary layer

Recent field studies have suggested that sea-salt particulate nitrate (NITs) photolysis may act as a significant local source of nitrogen oxides (NOx) over oceans. We present a study of the global impact of this process on oxidant concentrations in the marine boundary layer (MBL) using the GEOS-Chem model, after first updating the model to better simulate observed gas-particle phase partitioning of nitrate in the marine boundary layer. Model comparisons with long-term measurements of NOx from the Cape Verde Atmospheric Observatory (CVAO) in the eastern tropical North Atlantic provide support for an in situ source of NOx from NITs photolysis, with NITs photolysis coefficients about 25-50 times larger than corresponding HNO3 photolysis coefficients. Short-term measurements of nitrous acid (HONO) at this location show a clear daytime peak, with average peak mixing ratios ranging from 3 to 6 pptv. The model reproduces the general shape of the diurnal HONO profile only when NITs photolysis is included, but the magnitude of the daytime peak mixing ratio is under-predicted. This under-prediction is somewhat reduced if HONO yields from NITs photolysis are assumed to be close to unity. The combined NOx and HONO analysis suggests that the upper limit of the ratio of NITs : HNO3 photolysis coefficients is about 100. The largest simulated relative impact of NITs photolysis is in the tropical and subtropical marine boundary layer, with peak local enhancements ranging from factors of 5 to 20 for NOx, 1.2 to 1.6 for OH, and 1.1 to 1.3 for ozone. Since the spatial extent of the sea-salt aerosol (SSA) impact is limited, global impacts on NOx, ozone, and OH mass burdens are small ( ∼ 1-3 %). We also present preliminary analysis showing that particulate nitrate photolysis in accumulation-mode aerosols (predominantly over continental regions) could lead to ppbv-level increases in ozone in the continental boundary layer. Our results highlight the need for more comprehensive long-term measurements of NOx, and related species like HONO and sea-salt particulate nitrate, to better constrain the impact of particulate nitrate photolysis on marine boundary layer oxidant chemistry. Further field and laboratory studies on particulate nitrate photolysis in other aerosol types are also needed to better understand the impact of this process on continental boundary layer oxidant chemistry