Inverse modeling and mapping US air quality influences of inorganic PM_(2.5) precursor emissions using the adjoint of GEOS-Chem

Influences of specific sources of inorganic PM_(2.5) on peak and ambient aerosol concentrations in the US are evaluated using a combination of inverse modeling and sensitivity analysis. First, sulfate and nitrate aerosol measurements from the IMPROVE network are assimilated using the four-dimensional variational (4D-Var) method into the GEOS-Chem chemical transport model in order to constrain emissions estimates in four separate month-long inversions (one per season). Of the precursor emissions, these observations primarily constrain ammonia (NH_3). While the net result is a decrease in estimated US~NH_3 emissions relative to the original inventory, there is considerable variability in adjustments made to NH_3 emissions in different locations, seasons and source sectors, such as focused decreases in the midwest during July, broad decreases throughout the US~in January, increases in eastern coastal areas in April, and an effective redistribution of emissions from natural to anthropogenic sources. Implementing these constrained emissions, the adjoint model is applied to quantify the influences of emissions on representative PM_(2.5) air quality metrics within the US. The resulting sensitivity maps display a wide range of spatial, sectoral and seasonal variability in the susceptibility of the air quality metrics to absolute emissions changes and the effectiveness of incremental emissions controls of specific source sectors. NH_3 emissions near sources of sulfur oxides (SO_x) are estimated to most influence peak inorganic PM_(2.5) levels in the East; thus, the most effective controls of NH_3 emissions are often disjoint from locations of peak NH_3 emissions. Controls of emissions from industrial sectors of SO_x and NO_x are estimated to be more effective than surface emissions, and changes to NH_3 emissions in regions dominated by natural sources are disproportionately more effective than regions dominated by anthropogenic sources. NOx controls are most effective in northern states in October; in January, SO_x controls may be counterproductive. When considering ambient inorganic PM_(2.5) concentrations, intercontinental influences are small, though transboundary influences within North America are significant, with SO_x emissions from surface sources in Mexico contributing almost a fourth of the total influence from this sector

Specific Adhesion of Membranes Simultaneously Supports Dual Heterogeneities in Lipids and Proteins

Membrane adhesion is a vital component of many biological processes. Heterogeneities in lipid and protein composition are often associated with the adhesion site. These heterogeneities are thought to play functional roles in facilitating signalling. Here we experimentally examine this phenomenon using model membranes made of a mixture of lipids that is near a phase boundary at room temperature. Non-adherent model membranes are in a well-mixed, disordered-fluid lipid phase indicated by homogeneous distribution of a fluorescent dye that is a marker for the fluid-disordered (Ld) phase. We specifically adhere membranes to a flat substrate bilayer using biotin–avidin binding. Adhesion produces two types of coexisting heterogeneities: an ordered lipid phase that excludes binding proteins and the fluorescent membrane dye, and a disordered lipid phase that is enriched in both binding proteins and membrane dye compared with the non-adhered portion of the same membrane. Thus, a single type of adhesion interaction (biotin–avidin binding), in an initially-homogeneous system, simultaneously stabilizes both ordered-phase and disordered-phase heterogeneities that are compositionally distinct from the non-adhered portion of the vesicle. These heterogeneities are long-lived and unchanged upon increased temperature.This work was funded by start-up funds from The University of Texas at Austin (UT Austin) to VDG. MR was supported in part by undergraduate research fellowships from UT Austin. We are grateful to Professor Jeanne Stachowiak (Biomedical Engineering, UT Austin) for helpful conversations about membrane formation and to her and her group for technical assistance. We thank Professor Ernst-Ludwig Florin (Physics, UT Austin) for the extruder and for cover glasses. We thank Professor Lauren Ehrlich (Molecular Biosciences, UT Austin) for helpful conversations about the immune synapse.Center for Nonlinear Dynamic

Climate and air-quality benefits of a realistic phase-out of fossil fuels

The combustion of fossil fuels produces emissions of the long-lived greenhouse gas carbon dioxide and of short-lived pollutants, including sulfur dioxide, that contribute to the formation of atmospheric aerosols1. Atmospheric aerosols can cool the climate, masking some of the warming effect that results from the emission of greenhouse gases1. However, aerosol particulates are highly toxic when inhaled, leading to millions of premature deaths per year2,3. The phasing out of unabated fossil-fuel combustion will therefore provide health benefits, but will also reduce the extent to which the warming induced by greenhouse gases is masked by aerosols. Because aerosol levels respond much more rapidly to changes in emissions relative to carbon dioxide, large near-term increases in the magnitude and rate of climate warming are predicted in many idealized studies that typically assume an instantaneous removal of all anthropogenic or fossil-fuel-related emissions1,4,5,6,7,8,9. Here we show that more realistic modelling scenarios do not produce a substantial near-term increase in either the magnitude or the rate of warming, and in fact can lead to a decrease in warming rates within two decades of the start of the fossil-fuel phase-out. Accounting for the time required to transform power generation, industry and transportation leads to gradually increasing and largely offsetting climate impacts of carbon dioxide and sulfur dioxide, with the rate of warming further slowed by reductions in fossil-methane emissions. Our results indicate that even the most aggressive plausible transition to a clean-energy society provides benefits for climate change mitigation and air quality at essentially all decadal to centennial timescales

The Net Climate Impact of Coal-Fired Power Plant Emissions

Coal-fired power plants influence climate via both the emission of long-lived carbon dioxide (CO2) and short-lived ozone and aerosol precursors. Using a climate model, we perform the first study of the spatial and temporal pattern of radiative forcing specifically for coal plant emissions. Without substantial pollution controls, we find that near-term net global mean climate forcing is negative due to the well-known aerosol masking of the effects of CO2. Imposition of pollution controls on sulfur dioxide and nitrogen oxides leads to a rapid realization of the full positive forcing from CO2, however. Long-term global mean forcing from stable (constant) emissions is positive regardless of pollution controls. Emissions from coal-fired power plants until 1970, including roughly 1/3 of total anthropogenic CO2 emissions, likely contributed little net global mean climate forcing during that period though they may have induce weak Northern Hemisphere mid-latitude (NHml) cooling. After that time many areas imposed pollution controls or switched to low sulfur coal. Hence forcing due to emissions from 1970 to 2000 and CO2 emitted previously was strongly positive and contributed to rapid global and especially NHml warming. Most recently, new construction in China and India has increased rapidly with minimal application of pollution controls. Continuation of this trend would add negative near-term global mean climate forcing but severely degrade air quality. Conversely, following the Western and Japanese pattern of imposing air quality pollution controls at a later time could accelerate future warming rates, especially at NHmls. More broadly, our results indicate that due to spatial and temporal inhomogeneities in forcing, climate impacts of multi-pollutant emissions can vary strongly from region to region and can include substantial effects on maximum rate-of-change, neither of which are captured by commonly used global metrics. The method we introduce here to estimate regional temperature responses may provide additional insight

Evaluation of the Absolute Regional Temperature Potential

The Absolute Regional Temperature Potential (ARTP) is one of the few climate metrics that provides estimates of impacts at a sub-global scale. The ARTP presented here gives the time-dependent temperature response in four latitude bands (90-28degS, 28degS-28degN, 28-60degN and 60-90degN) as a function of emissions based on the forcing in those bands caused by the emissions. It is based on a large set of simulations performed with a single atmosphere-ocean climate model to derive regional forcing/response relationships. Here I evaluate the robustness of those relationships using the forcing/response portion of the ARTP to estimate regional temperature responses to the historic aerosol forcing in three independent climate models. These ARTP results are in good accord with the actual responses in those models. Nearly all ARTP estimates fall within +/-20%of the actual responses, though there are some exceptions for 90-28degS and the Arctic, and in the latter the ARTP may vary with forcing agent. However, for the tropics and the Northern Hemisphere mid-latitudes in particular, the +/-20% range appears to be roughly consistent with the 95% confidence interval. Land areas within these two bands respond 39-45% and 9-39% more than the latitude band as a whole. The ARTP, presented here in a slightly revised form, thus appears to provide a relatively robust estimate for the responses of large-scale latitude bands and land areas within those bands to inhomogeneous radiative forcing and thus potentially to emissions as well. Hence this metric could allow rapid evaluation of the effects of emissions policies at a finer scale than global metrics without requiring use of a full climate model

An exploration of ozone changes and their radiative forcing prior to the chlorofluorocarbon era

International audienceUsing historical observations and model simulations, we investigate ozone trends prior to the mid-1970s onset of halogen-induced ozone depletion. Though measurements are quite limited, an analysis based on multiple, independent data sets (direct and indirect) provides better constraints than any individual set of observations. We find that three data sets support an apparent long-term stratospheric ozone trend of -7.2 ± 2.3 DU during 1957-1975, which modeling attributes primarily to water vapor increases. The results suggest that 20th century stratospheric ozone depletion may have been roughly 50% more than is generally supposed. Similarly, three data sets support tropospheric ozone increases over polluted Northern Hemisphere continental regions of 8.2 ± 2.1 DU during this period, which are mutually consistent with the stratospheric trends. As with paleoclimate data, which is also based on indirect proxies and/or limited spatial coverage, these results must be interpreted with caution. However, they provide the most thorough estimates presently available of ozone changes prior to the coincident onset of satellite data and halogen dominated ozone changes. If these apparent trends were real, the radiative forcing by stratospheric ozone since the 1950s would then have been -0.15 ± 0.05 W/m2, and -0.2 W/m2 since the preindustrial. For tropospheric ozone, it would have been 0.38 ± 0.10 W/m2 since the late 1950s. Combined with even a very conservative estimate of tropospheric ozone forcing prior to that time, this would be larger than current estimates since 1850 which are derived from models that are even less well constrained. These calculations demonstrate the importance of gaining a better understanding of historical ozone changes

Linkages Between Ozone-depleting Substances, Tropospheric Oxidation and Aerosols

Coupling between the stratosphere and the troposphere allows changes in stratospheric ozone abundances to affect tropospheric chemistry. Large-scale effects from such changes on chemically produced tropospheric aerosols have not been systematically examined in past studies. We use a composition-climate model to investigate potential past and future impacts of changes in stratospheric ozone depleting substances (ODS) on tropospheric oxidants and sulfate aerosols. In most experiments, we find significant responses in tropospheric photolysis and oxidants, with small but significant effects on methane radiative forcing. The response of sulfate aerosols is sizeable when examining the effect of increasing future nitrous oxide (N2O) emissions. We also find that without the regulation of chlorofluorocarbons (CFCs) through the Montreal Protocol, sulfate aerosols could have increased by 2050 by a comparable amount to the decreases predicted due to relatively stringent sulfur emissions controls. The individual historical radiative forcings of CFCs and N2O through their indirect effects on methane (22.6mW/sq. m for CFCs and 6.7mW/sq. m for N2O) and sulfate aerosols (3.0mW/sq. m for CFCs and +6.5mW/sq. m for N2O when considering the direct aerosol effect) discussed here are non-negligible when compared to known historical ODS forcing. Our results stress the importance of accounting for stratosphere-troposphere, gas-aerosol and composition-climate interactions when investigating the effects of changing emissions on atmospheric composition and climate

Membrane Adhesion and the Formation of Heterogeneities: Biology, Biophysics, and Biotechnology

a. The University of Texas at Austin, Department of Physics and Center for Nonlinear Dynamics, 2515 Speedway, Stop C1610, Austin, Texas 78712-1199, USA. E-mail: [email protected] b.The University of Texas at Austin, Department of Molecular Biosciences, Institute for Cellular and Molecular Biology, Austin, Texas 78712-1199, USAMembrane adhesion is essential to many vital biological processes. Sites of membrane adhesion are often associated with heterogeneities in the lipid and protein composition of the membrane. These heterogeneities are thought to play functional roles by facilitating interactions between proteins. However, the causal links between membrane adhesion and membrane heterogeneities are not known. Here we survey the state of the field and indicate what we think are understudied areas ripe for development.This work is supported by startup funds from UT Austin and a gift from ExxonMobile to VDG and by NIH R01 R01 GM089896 to T.J.O.Center for Nonlinear Dynamic

Precipitation response to regional radiative forcing

Precipitation shifts can have large impacts on human society and ecosystems. Many aspects of how inhomogeneous radiative forcings influence precipitation remain unclear, however. Here we investigate regional precipitation responses to various forcings imposed in different latitude bands in a climate model. We find that several regions show strong, significant responses to most forcings, but that the magnitude and even the sign depends upon the forcing location and type. Aerosol and ozone forcings typically induce larger responses than equivalent carbon dioxide (CO<sub>2</sub>) forcing, and the influence of remote forcings often outweighs that of local forcings. Consistent with this, ozone and especially aerosols contribute greatly to precipitation changes over the Sahel and South and East Asia in historical simulations, and inclusion of aerosols greatly increases the agreement with observed trends in these areas, which cannot be attributed to either greenhouse gases or natural forcings. Estimates of precipitation responses derived from multiplying our Regional Precipitation Potentials (RPP; the response per unit forcing relationships) by historical forcings typically capture the actual response in full transient climate simulations fairly well, suggesting that these relationships may provide useful metrics. The strong sensitivity to aerosol and ozone forcing suggests that although some air quality improvements may unmask greenhouse gas-induced warming, they have large benefits for reducing regional disruption of the hydrologic cycle

Nitrate aerosols today and in 2030: a global simulation including aerosols and tropospheric ozone

International audienceNitrate aerosols are expected to become more important in the future atmosphere due to the expected increase in nitrate precursor emissions and the decline of ammonium-sulphate aerosols in wide regions of this planet. The GISS climate model is used in this study, including atmospheric gas- and aerosol phase chemistry to investigate current and future (2030, following the SRES A1B emission scenario) atmospheric compositions. A set of sensitivity experiments was carried out to quantify the individual impact of emission- and physical climate change on nitrate aerosol formation. We found that future nitrate aerosol loads depend most strongly on changes that may occur in the ammonia sources. Furthermore, microphysical processes that lead to aerosol mixing play a very important role in sulphate and nitrate aerosol formation. The role of nitrate aerosols as climate change driver is analyzed and set in perspective to other aerosol and ozone forcings under pre-industrial, present day and future conditions. In the near future, year 2030, ammonium nitrate radiative forcing is about ?0.14 W/m² and contributes roughly 10% of the net aerosol and ozone forcing. The present day nitrate and pre-industrial nitrate forcings are ?0.11 and ?0.05 W/m², respectively. The steady increase of nitrate aerosols since industrialization increases its role as a non greenhouse gas forcing agent. However, this impact is still small compared to greenhouse gas forcings, therefore the main role nitrate will play in the future atmosphere is as an air pollutant, with annual mean near surface air concentrations, in the fine particle mode, rising above 3 ?g/m³ in China and therefore reaching pollution levels, like sulphate aerosols