Search for: All records

Future climate change may bring local benefits or penalties to surface air pollution, resulting from changing temperature, precipitation, and transport patterns, as well as changes in climate-sensitive natural precursor emissions. Here, we estimate the climate penalties and benefits at the end of this century with regard to surface ozone and fine particulate matter (PM ${}_{2.5}$; excluding dust and smoke) using a one-way offline coupling between a general circulation model and a global 3-D chemical-transport model. We archive meteorology for the present day (2005 to 2014) and end of this century (2090 to 2099) for seven future scenarios developed for Phase 6 of the Coupled Model Intercomparison Project. The model isolates the impact of forecasted anthropogenic precursor emission changes versus that of climate-only driven changes on surface ozone and PM ${}_{2.5}$for scenarios ranging from extreme mitigation to extreme warming. We then relate these changes to impacts on human mortality and crop production. We find ozone penalties over nearly all land areas with increasing warming. We find net benefits due to climate-driven changes in PM ${}_{2.5}$in the Northern Extratropics, but net penalties in the Tropics and Southern Hemisphere, where most population growth is forecast for the coming century. 

Abstract Estimating fire emissions prior to the satellite era is challenging because observations are limited, leading to large uncertainties in the calculated aerosol climate forcing following the preindustrial era. This challenge further limits the ability of climate models to accurately project future climate change. Here, we reconstruct a gridded dataset of global biomass burning emissions from 1750 to 2010 using inverse analysis that leveraged a global array of 31 ice core records of black carbon deposition fluxes, two different historical emission inventories as a priori estimates, and emission-deposition sensitivities simulated by the atmospheric chemical transport model GEOS-Chem. The reconstructed emissions exhibit greater temporal variabilities which are more consistent with paleoclimate proxies. Our ice core constrained emissions reduced the uncertainties in simulated cloud condensation nuclei and aerosol radiative forcing associated with the discrepancy in preindustrial biomass burning emissions. The derived emissions can also be used in studies of ocean and terrestrial biogeochemistry. 

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. 

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. 

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.