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  1. Abstract

    Decadal trends in fire activity can reveal important human and climate-driven influences across a multitude of landscapes from croplands to savannas. We use 16 years of daily satellite observations from 2003 to 2018 to search globally for stationary temporal shifts in fire activity during the primary burning season. We focus on southwest Russia and north Australia as case study regions; both regions experienced nearly 40 d shifts over a 16 year period but in opposite directions. In southwest Russia, a major wheat-growing region, we trace the delay in post-harvest fires to several potential drivers: modernization in the agricultural system and recent droughts, followed by government restrictions on wheat exports. In north Australia, prescribed burns in the early dry season are a key practice in Aboriginal fire management of savannas, and the increasing trend of such fires has limited the size and extent of fast-spreading late dry season fires, thereby shifting overall fire activity earlier. In both regions, human action, through controlling fire ignition and extent, is an important driver of the temporal shifts in fire activity with climate as both a harbinger and an amplifier of human-induced changes.

     
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  2. Abstract. This paper describes version 2.0 of the Global Change and Air Pollution (GCAP 2.0) model framework, a one-way offline coupling between version E2.1 of the NASA Goddard Institute for Space Studies (GISS) general circulation model (GCM) and the GEOS-Chem global 3-D chemical-transport model (CTM). Meteorology for driving GEOS-Chem has been archived from the E2.1 contributions to phase 6 of the Coupled Model Intercomparison Project (CMIP6) for the pre-industrial era and the recent past. In addition, meteorology is available for the near future and end of the century for seven future scenarios ranging from extreme mitigation to extreme warming. Emissions and boundary conditions have been prepared for input to GEOS-Chem that are consistent with the CMIP6 experimental design. The model meteorology, emissions, transport, and chemistry are evaluated in the recent past and found to be largely consistent with GEOS-Chem driven by the Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2) product and with observational constraints. 
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  3. Abstract

    Since 2013, Chinese policies have dramatically reduced emissions of particulates and their gas‐phase precursors, but the implications of these reductions for aerosol‐radiation interactions are unknown. Using a global, coupled chemistry‐climate model, we examine how the radiative impacts of Chinese air pollution in the winter months of 2012 and 2013 affect local meteorology and how these changes may, in turn, influence surface concentrations of PM2.5, particulate matter with diameter <2.5 μm. We then investigate how decreasing emissions through 2016 and 2017 alter this impact. We find that absorbing aerosols aloft in winter 2012 and 2013 heat the middle‐ and lower troposphere by ∼0.5–1 K, reducing cloud liquid water, snowfall, and snow cover. The subsequent decline in surface albedo appears to counteract the ∼15–20 W m−2decrease in shortwave radiation reaching the surface due to attenuation by aerosols overhead. The net result of this novel cloud‐snowfall‐albedo feedback in winters 2012–2013 is a slight increase in surface temperature of ∼0.5–1 K in some regions and little change elsewhere. The aerosol heating aloft, however, stabilizes the atmosphere and decreases the seasonal mean planetary boundary layer (PBL) height by ∼50 m. In winter 2016 and 2017, the ∼20% decrease in mean PM2.5weakens the cloud‐snowfall‐albedo feedback, though it is still evident in western China, where the feedback again warms the surface by ∼0.5–1 K. Regardless of emissions, we find that aerosol‐radiation interactions enhance mean surface PM2.5pollution by 10%–20% across much of China during all four winters examined, mainly though suppression of PBL heights.

     
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  4. Concentrations of atmospheric trace species in the United States have changed dramatically over the past several decades in response to pollution control strategies, shifts in domestic energy policy and economics, and economic development (and resulting emission changes) elsewhere in the world. Reliable projections of the future atmosphere require models to not only accurately describe current atmospheric concentrations, but to do so by representing chemical, physical and biological processes with conceptual and quantitative fidelity. Only through incorporation of the processes controlling emissions and chemical mechanisms that represent the key transformations among reactive molecules can models reliably project the impacts of future policy, energy and climate scenarios. Efforts to properly identify and implement the fundamental and controlling mechanisms in atmospheric models benefit from intensive observation periods, during which collocated measurements of diverse, speciated chemicals in both the gas and condensed phases are obtained. The Southeast Atmosphere Studies (SAS, including SENEX, SOAS, NOMADSS and SEAC4RS) conducted during the summer of 2013 provided an unprecedented opportunity for the atmospheric modeling community to come together to evaluate, diagnose and improve the representation of fundamental climate and air quality processes in models of varying temporal and spatial scales.

    This paper is aimed at discussing progress in evaluating, diagnosing and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models. The effort focused primarily on model representation of fundamental atmospheric processes that are essential to the formation of ozone, secondary organic aerosol (SOA) and other trace species in the troposphere, with the ultimate goal of understanding the radiative impacts of these species in the southeast and elsewhere. Here we address questions surrounding four key themes: gas-phase chemistry, aerosol chemistry, regional climate and chemistry interactions, and natural and anthropogenic emissions. We expect this review to serve as a guidance for future modeling efforts. 
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  5. Abstract

    Sulfur compounds are an important constituent of particulate matter, with impacts on climate and public health. While most sulfur observed in particulate matter has been assumed to be sulfate, laboratory experiments reveal that hydroxymethanesulfonate (HMS), an adduct formed by aqueous phase chemical reaction of dissolved HCHO and SO2, may be easily misinterpreted in measurements as sulfate. Here we present observational and modeling evidence for a ubiquitous global presence of HMS. We find that filter samples collected in Shijiazhuang, China, and examined with ion chromatography within 9 days show as much as 7.6 μg m−3of HMS, while samples from Singapore examined 9–18 months after collection reveal ~0.6 μg m−3of HMS. The Shijiazhuang samples show only minor traces of HMS 4 months later, suggesting that HMS had decomposed over time during sample storage. In contrast, the Singapore samples do not clearly show a decline in HMS concentration over 2 months of monitoring. Measurements from over 150 sites, primarily derived from the IMPROVE network across the United States, suggest the ubiquitous presence of HMS in at least trace amounts as much as 60 days after collection. The degree of possible HMS decomposition in the IMPROVE observations is unknown. Using the GEOS‐Chem chemical transport model, we estimate that HMS may account for 10% of global particulate sulfur in continental surface air and over 25% in many polluted regions. Our results suggest that reducing emissions of HCHO and other volatile organic compounds may have a co‐benefit of decreasing particulate sulfur.

     
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