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

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

The distribution of snow black carbon observed in the Arctic and compared to the GISS-PUCCINI model

In this study, we evaluate the ability of the latest NASA GISS composition-climate model, GISS-E2-PUCCINI, to simulate the spatial distribution of snow BC (sBC) in the Arctic relative to present-day observations. Radiative forcing due to BC deposition onto Arctic snow and sea ice is also estimated. Two sets of model simulations are analyzed, where meteorology is linearly relaxed towards National Centers for Environmental Prediction (NCEP) and towards NASA Modern Era Reanalysis for Research and Applications (MERRA) reanalyses. Results indicate that the modeled concentrations of sBC are comparable with present-day observations in and around the Arctic Ocean, except for apparent underestimation at a few sites in the Russian Arctic. That said, the model has some biases in its simulated spatial distribution of BC deposition to the Arctic. The simulations from the two model runs are roughly equal, indicating that discrepancies between model and observations come from other sources. Underestimation of biomass burning emissions in Northern Eurasia may be the main cause of the low biases in the Russian Arctic. Comparisons of modeled aerosol BC (aBC) with long-term surface observations at Barrow, Alert, Zeppelin and Nord stations show significant underestimation in winter and spring concentrations in the Arctic (most significant in Alaska), although the simulated seasonality of aBC has been greatly improved relative to earlier model versions. This is consistent with simulated biases in vertical profiles of aBC, with underestimation in the lower and middle troposphere but overestimation in the upper troposphere and lower stratosphere, suggesting that the wet removal processes in the current model may be too weak or that vertical transport is too rapid, although the simulated BC lifetime seems reasonable. The combination of observations and modeling provides a comprehensive distribution of sBC over the Arctic. On the basis of this distribution, we estimate the decrease in snow and sea ice albedo and the resulting radiative forcing. We suggest that the albedo reduction due to BC deposition presents significant space-time variations, with highest mean reductions of 1.25% in the Russian Arctic, which are much larger than those in other Arctic regions (0.39% to 0.64%). The averaged value over the Arctic north of 66° N is 0.4–0.6% during spring, leading to regional surface radiative forcings of 0.7, 1.1 and 1.0 W m<sup>−2</sup> in spring 2007, 2008 and 2009, respectively

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

Impacts of aerosol-cloud interactions on past and future changes in tropospheric composition

The development of effective emissions control policies that are beneficial to both climate and air quality requires a detailed understanding of all the feedbacks in the atmospheric composition and climate system. We perform sensitivity studies with a global atmospheric composition-climate model to assess the impact of aerosols on tropospheric chemistry through their modification on clouds, aerosol-cloud interactions (ACI). The model includes coupling between both tropospheric gas-phase and aerosol chemistry and aerosols and liquid-phase clouds. We investigate past impacts from preindustrial (PI) to present day (PD) and future impacts from PD to 2050 (for the moderate IPCC A1B scenario) that embrace a wide spectrum of precursor emission changes and consequential ACI. The aerosol indirect effect (AIE) is estimated to be -2.0 Wm{sup -2} for PD-PI and -0.6 Wm{sup -2} for 2050-PD, at the high end of current estimates. Inclusion of ACI substantially impacts changes in global mean methane lifetime across both time periods, enhancing the past and future increases by 10% and 30%, respectively. In regions where pollution emissions increase, inclusion of ACI leads to 20% enhancements in in-cloud sulfate production and {approx}10% enhancements in sulfate wet deposition that is displaced away from the immediate source regions. The enhanced in-cloud sulfate formation leads to larger increases in surface sulfate across polluted regions ({approx}10-30%). Nitric acid wet deposition is dampened by 15-20% across the industrialized regions due to ACI allowing additional re-release of reactive nitrogen that contributes to 1-2 ppbv increases in surface ozone in outflow regions. Our model findings indicate that ACI must be considered in studies of methane trends and projections of future changes to particulate matter air quality

Global and regional temperature-change potentials for near-term climate forcers

We examine the climate effects of the emissions of near-term climate forcers (NTCFs) from 4 continental regions (East Asia, Europe, North America and South Asia) using radiative forcing from the task force on hemispheric transport of air pollution source-receptor global chemical transport model simulations. These simulations model the transport of 3 aerosol species (sulphate, particulate organic matter and black carbon) and 4 ozone precursors (methane, nitric oxides (NOx), volatile organic compounds and carbon monoxide). From the equilibrium radiative forcing results we calculate global climate metrics, global warming potentials (GWPs) and global temperature change potentials (GTPs) and show how these depend on emission region, and can vary as functions of time. For the aerosol species, the GWP(100) values are −37±12, −46±20, and 350±200 for SO2, POM and BC respectively for the direct effects only. The corresponding GTP(100) values are −5.2±2.4, −6.5±3.5, and 50±33. This analysis is further extended by examining the temperature-change impacts in 4 latitude bands. This shows that the latitudinal pattern of the temperature response to emissions of the NTCFs does not directly follow the pattern of the diagnosed radiative forcing. For instance temperatures in the Arctic latitudes are particularly sensitive to NTCF emissions in the northern mid-latitudes. At the 100-yr time horizon the ARTPs show NOx emissions can have a warming effect in the northern mid and high latitudes, but cooling in the tropics and Southern Hemisphere. The northern mid-latitude temperature response to northern mid-latitude emissions of most NTCFs is approximately twice as large as would be implied by the global average