Nonlinearity in atmospheric response: A direct sensitivity analysis approach

The decoupled direct method (DDM) is used for efficient and accurate calculation of the higher-order sensitivity coefficients in a regional photochemical air quality model with detailed chemical mechanism (Statewide Air Pollution Research Center (SAPRC-99)). High-order DDM (HDDM) is an extension to a previous implementation of DDM in three-dimensional air quality models (DDM-3D) that directly calculates the higher-order derivatives (with respect to one parameter, as well as cross derivatives) with similar computational efficiency as the first-order implementation and is also modified for better accuracy. (H)DDM results show very good agreement with brute force (finite difference) sensitivity coefficients for the first- and second-order derivatives, but the agreement deteriorates for higher-order coefficients. The nature of the truncation errors and other inaccuracies in the brute force approximations are explored. The difference between the first-order brute force and DDM derivatives is dominated (and largely explained) by the truncation errors as calculated from HDDM results. Taylor expansion is used for parametric scaling of the response with the use of sensitivity coefficients. Use of higher-order coefficients can significantly improve the accuracy of such projections. Finally, higher-order sensitivity coefficients of ozone with respect to NOx and volatile organic compound emissions (including cross derivatives) are used to create time- and location-dependent ozone isopleths. Copyright 2004 by the American Geophysical Union

Differences between magnitudes and health impacts of BC emissions across the United States using 12 km scale seasonal source apportionment

Recent assessments have analyzed the health impacts of PM2.5 from emissions from different locations and sectors using simplified or reduced-form air quality models. Here we present an alternative approach using the adjoint of the Community Multiscale Air Quality (CMAQ) model, which provides source-receptor relationships at highly resolved sectoral, spatial, and temporal scales. While damage resulting from anthropogenic emissions of BC is strongly correlated with population and premature death, we found little correlation between damage and emission magnitude, suggesting that controls on the largest emissions may not be the most efficient means of reducing damage resulting from anthropogenic BC emissions. Rather, the best proxy for locations with damaging BC emissions is locations where premature deaths occur. Onroad diesel and nonroad vehicle emissions are the largest contributors to premature deaths attributed to exposure to BC, while onroad gasoline emissions cause the highest deaths per amount emitted. Emissions in fall and winter contribute to more premature deaths (and more per amount emitted) than emissions in spring and summer. Overall, these results show the value of the high-resolution source attribution for determining the locations, seasons, and sectors for which BC emission controls have the most effective health benefits

Premature deaths attributed to source-specific BC emissions in six urban US regions

Recent studies have shown that exposure to particulate black carbon (BC) has significant adverse health effects and may be more detrimental to human health than exposure to PM2.5 as a whole. Mobile source BC emission controls, mostly on diesel-burning vehicles, have successfully decreased mobile source BC emissions to less than half of what they were 30 years ago. Quantification of the benefits of previous emissions controls conveys the value of these regulatory actions and provides a method by which future control alternatives could be evaluated. In this study we use the adjoint of the Community Multiscale Air Quality (CMAQ) model to estimate highly-resolved spatial distributions of benefits related to emission reductions for six urban regions within the continental US. Emissions from outside each of the six chosen regions account for between 7% and 27% of the premature deaths attributed to exposure to BC within the region. While we estimate that nonroad mobile and onroad diesel emissions account for the largest number of premature deaths attributable to exposure to BC, onroad gasoline is shown to have more than double the benefit per unit emission relative to that of nonroad mobile and onroad diesel. Within the region encompassing New York City and Philadelphia, reductions in emissions from large industrial combustion sources that are not classified as EGUs (i.e., non-EGU) are estimated to have up to triple the benefits per unit emission relative to reductions to onroad diesel sectors, and provide similar benefits per unit emission to that of onroad gasoline emissions in the region. While onroad mobile emissions have been decreasing in the past 30 years and a majority of vehicle emission controls that regulate PM focus on diesel emissions, our analysis shows the most efficient target for stricter controls is actually onroad gasoline emissions