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Many regions of the planet have experienced an increase in fire activity in recent decades. Although such increases are consistent with warming and drying under continued climate change, the driving mechanisms remain uncertain. Here, we investigate the effects of increasing atmospheric carbon dioxide concentrations on future fire activity using seven Earth system models. Centered on the time of carbon dioxide doubling, the multi-model mean percent change in fire carbon emissions is 66.4 ± 38.8% (versus 1850 carbon dioxide concentrations, under fixed 1850 land-use conditions). A substantial increase is associated with enhanced vegetation growth due to carbon dioxide biogeochemical impacts at 60.1 ± 46.9%. In contrast, carbon dioxide radiative impacts, including warming and drying, yield a negligible response of fire carbon emissions at 1.7 ± 9.4%. Although model representation of fire processes remains uncertain, our results show the importance of vegetation dynamics to future increases in fire activity under increasing carbon dioxide, with potentially important policy implications.

 

Previous studies suggest that greenhouse gas-induced warming can lead to increased fine particulate matter concentrations and degraded air quality. However, significant uncertainties remain regarding the sign and magnitude of the response to warming and the underlying mechanisms. Here, we show that thirteen models from the Coupled Model Intercomparison Project Phase 6 all project an increase in global average concentrations of fine particulate matter in response to rising carbon dioxide concentrations, but the range of increase across models is wide. The two main contributors to this increase are increased abundance of dust and secondary organic aerosols via intensified West African monsoon and enhanced emissions of biogenic volatile organic compounds, respectively. Much of the inter-model spread is related to different treatment of biogenic volatile organic compounds. Our results highlight the importance of natural aerosols in degrading air quality under current warming, while also emphasizing that improved understanding of biogenic volatile organic compounds emissions due to climate change is essential for numerically assessing future air quality.

 

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. 

We assess the effective radiative forcing due to ozone‐depleting substances using models participating in the Aerosols and Chemistry and Radiative Forcing Model Intercomparison Projects (AerChemMIP, RFMIP). A large intermodel spread in this globally averaged quantity necessitates an “emergent constraint” approach whereby we link the radiative forcing to ozone declines measured and simulated during 1979–2000, excluding two volcanically perturbed periods. During this period, ozone‐depleting substances were increasing, and several merged satellite‐based climatologies document the ensuing decline of total‐column ozone. Using these analyses, we find an effective radiative forcing of−0.05 to 0.13 W m⁻². Our best estimate (0.04 W m⁻²) is on the edge of the “likely” range given by the Fifth Assessment Report of IPCC of 0.03 to 0.33 W m⁻²but is in better agreement with two other literature results.

 

We use a 0-D photochemical box model and a 3-D global chemistry-climate model, combined with observations from the NOAA Southeast Nexus (SENEX) aircraft campaign, to understand the sources and sinks of glyoxal over the Southeast United States. Box model simulations suggest a large difference in glyoxal production among three isoprene oxidation mechanisms (AM3ST, AM3B, and MCM v3.3.1). These mechanisms are then implemented into a 3-D global chemistry-climate model. Comparison with field observations shows that the average vertical profile of glyoxal is best reproduced by AM3ST with an effective reactive uptake coefficient γglyx of 2 × 10-3, and AM3B without heterogeneous loss of glyoxal. The two mechanisms lead to 0-0.8 µg m-3 secondary organic aerosol (SOA) from glyoxal in the boundary layer of the Southeast U.S. in summer. We consider this to be the lower limit for the contribution of glyoxal to SOA, as other sources of glyoxal other than isoprene are not included in our model. In addition, we find that AM3B shows better agreement on both formaldehyde and the correlation between glyoxal and formaldehyde (RGF = [GLYX]/[HCHO]), resulting from the suppression of δ-isoprene peroxy radicals (δ-ISOPO2). We also find that MCM v3.3.1 may underestimate glyoxal production from isoprene oxidation, in part due to an underestimated yield from the reaction of IEPOX peroxy radicals (IEPOXOO) with HO2. Our work highlights that the gas-phase production of glyoxal represents a large uncertainty in quantifying its contribution to SOA.