Constraining remote oxidation capacity with ATom observations.

The global oxidation capacity, defined as the tropospheric mean concentration of the hydroxyl radical (OH), controls the lifetime of reactive trace gases in the atmosphere such as methane and carbon monoxide (CO). Models tend to underestimate the methane lifetime and CO concentrations throughout the troposphere, which is consistent with excessive OH. Approximately half of the oxidation of methane and non-methane volatile organic compounds (VOCs) is thought to occur over the oceans where oxidant chemistry has received little validation due to a lack of observational constraints. We use observations from the first two deployments of the NASA ATom aircraft campaign during July-August 2016 and January-February 2017 to evaluate the oxidation capacity over the remote oceans and its representation by the GEOS-Chem chemical transport model. The model successfully simulates the magnitude and vertical profile of remote OH within the measurement uncertainties. Comparisons against the drivers of OH production (water vapor, ozone, and NO y concentrations, ozone photolysis frequencies) also show minimal bias, with the exception of wintertime NO y . The severe model overestimate of NO y during this period may indicate insufficient wet scavenging and/or missing loss on sea-salt aerosols. Large uncertainties in these processes require further study to improve simulated NO y partitioning and removal in the troposphere, but preliminary tests suggest that their overall impact could marginally reduce the model bias in tropospheric OH. During the ATom-1 deployment, OH reactivity (OHR) below 3 km is significantly enhanced, and this is not captured by the sum of its measured components (cOHRobs) or by the model (cOHRmod). This enhancement could suggest missing reactive VOCs but cannot be explained by a comprehensive simulation of both biotic and abiotic ocean sources of VOCs. Additional sources of VOC reactivity in this region are difficult to reconcile with the full suite of ATom measurement constraints. The model generally reproduces the magnitude and seasonality of cOHRobs but underestimates the contribution of oxygenated VOCs, mainly acetaldehyde, which is severely underestimated throughout the troposphere despite its calculated lifetime of less than a day. Missing model acetaldehyde in previous studies was attributed to measurement uncertainties that have been largely resolved. Observations of peroxyacetic acid (PAA) provide new support for remote levels of acetaldehyde. The underestimate in both model acetaldehyde and PAA is present throughout the year in both hemispheres and peaks during Northern Hemisphere summer. The addition of ocean sources of VOCs in the model increases cOHRmod by 3% to 9% and improves model-measurement agreement for acetaldehyde, particularly in winter, but cannot resolve the model summertime bias. Doing so would require 100 Tg yr-1 of a long-lived unknown precursor throughout the year with significant additional emissions in the Northern Hemisphere summer. Improving the model bias for remote acetaldehyde and PAA is unlikely to fully resolve previously reported model global biases in OH and methane lifetime, suggesting that future work should examine the sources and sinks of OH over land.

Reconciling oil palm expansion and climate change mitigation in Kalimantan, Indonesia.

Our society faces the pressing challenge of increasing agricultural production while minimizing negative consequences on ecosystems and the global climate. Indonesia, which has pledged to reduce greenhouse gas (GHG) emissions from deforestation while doubling production of several major agricultural commodities, exemplifies this challenge. Here we focus on palm oil, the world's most abundant vegetable oil and a commodity that has contributed significantly to Indonesia's economy. Most oil palm expansion in the country has occurred at the expense of forests, resulting in significant GHG emissions. We examine the extent to which land management policies can resolve the apparently conflicting goals of oil palm expansion and GHG mitigation in Kalimantan, a major oil palm growing region of Indonesia. Using a logistic regression model to predict the locations of new oil palm between 2010 and 2020 we evaluate the impacts of six alternative policy scenarios on future emissions. We estimate net emissions of 128.4-211.4 MtCO2 yr(-1) under business as usual expansion of oil palm plantations. The impact of diverting new plantations to low carbon stock land depends on the design of the policy. We estimate that emissions can be reduced by 9-10% by extending the current moratorium on new concessions in primary forests and peat lands, 35% by limiting expansion on all peat and forestlands, 46% by limiting expansion to areas with moderate carbon stocks, and 55-60% by limiting expansion to areas with low carbon stocks. Our results suggest that these policies would reduce oil palm profits only moderately but would vary greatly in terms of cost-effectiveness of emissions reductions. We conclude that a carefully designed and implemented oil palm expansion plan can contribute significantly towards Indonesia's national emissions mitigation goal, while allowing oil palm area to double.

Global chemical composition of ambient fine particulate matter for exposure assessment.

Epidemiologic and health impact studies are inhibited by the paucity of global, long-term measurements of the chemical composition of fine particulate matter. We inferred PM2.5 chemical composition at 0.1° × 0.1° spatial resolution for 2004-2008 by combining aerosol optical depth retrieved from the MODIS and MISR satellite instruments, with coincident profile and composition information from the GEOS-Chem global chemical transport model. Evaluation of the satellite-model PM2.5 composition data set with North American in situ measurements indicated significant spatial agreement for secondary inorganic aerosol, particulate organic mass, black carbon, mineral dust, and sea salt. We found that global population-weighted PM2.5 concentrations were dominated by particulate organic mass (11.9 ± 7.3 µg/m(3)), secondary inorganic aerosol (11.1 ± 5.0 µg/m(3)), and mineral dust (11.1 ± 7.9 µg/m(3)). Secondary inorganic PM2.5 concentrations exceeded 30 µg/m(3) over East China. Sensitivity simulations suggested that population-weighted ambient PM2.5 from biofuel burning (11 µg/m(3)) could be almost as large as from fossil fuel combustion sources (17 µg/m(3)). These estimates offer information about global population exposure to the chemical components and sources of PM2.5.

Separating the influence of temperature, drought, and fire on interannual variability in atmospheric CO2.

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 (CO2) 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 CO2 anomalies. Here we examined how the temporal evolution of CO2 in different latitude bands may be used to separate contributions from temperature stress, drought stress, and fire emissions to CO2 variability. We developed atmospheric CO2 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 CO2 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 CO2 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 CO2 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 CO2 variability prior to using contemporary observations to constrain long-term ESM responses.

Forecasting 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. We investigated the relationship between year-to-year changes in fire activity in South America and sea surface temperatures. We found that the Oceanic Niño Index was correlated with interannual fire activity in the eastern Amazon, whereas the Atlantic Multidecadal Oscillation index was more closely linked with fires in the southern and southwestern Amazon. Combining these two climate indices, we developed an empirical model to forecast regional fire season severity with lead times of 3 to 5 months. Our approach may contribute to the development of an early warning system for anticipating the vulnerability of Amazon forests to fires, thus enabling more effective management with benefits for climate and air quality.

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 CH4 and CO2 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 CO2 growth rate anomaly. The main contributors were Southeast Asia (60%), Central and South America (30%), and boreal regions of Eurasia and North America (10%).