HTAP3 Fires: towards a multi-model, multi-pollutant study of fire impacts
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Whaley, Cynthia H.↗
Engineering topics
Wild, Oliver
Publications and source records attributed to Wild, Oliver.
Simulating organic aerosol in Delhi with WRF-Chem using the volatility-basis-set approach: exploring model uncertainty with a Gaussian process emulator
The nature and origin of organic aerosol in the atmosphere remain unclear. The gas–particle partitioning of semi-volatile organic compounds (SVOCs) that constitute primary organic aerosols (POAs) and the multigenerational chemical aging of SVOCs are particularly poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem (Weather Research and Forecasting model with Chemistry), can be a useful tool to describe emissions of POA and its chemical evolution. However, the evaluation of model uncertainty and the optimal model parameterization may be expensive to probe using only WRF-Chem simulations. Gaussian process emulators, trained on simulations from relatively few WRF-Chem simulations, are capable of reproducing model results and estimating the sources of model uncertainty within a defined range of model parameters. In this study, a WRF-Chem VBS parameterization is proposed; we then generate a perturbed parameter ensemble of 111 model runs, perturbing 10 parameters of the WRF-Chem model relating to organic aerosol emissions and the VBS oxidation reactions. This allowed us to cover the model's uncertainty space and to compare outputs from each run to aerosol mass spectrometer observations of organic aerosol concentrations and O:C ratios measured in New Delhi, India. The simulations spanned the organic aerosol concentrations measured with the aerosol mass spectrometer (AMS). However, they also highlighted potential structural errors in the model that may be related to unsuitable diurnal cycles in the emissions and/or failure to adequately represent the dynamics of the planetary boundary layer. While the structural errors prevented us from clearly identifying an optimized VBS approach in WRF-Chem, we were able to apply the emulator in the following two periods: the full period (1–29 May) and a subperiod period of 14:00–16:00 h LT (local time) on 1–29 May. The combination of emulator analysis and model evaluation metrics allowed us to identify plausible parameter combinations for the analyzed periods. We demonstrate that the methodology presented in this study can be used to determine the model uncertainty and to identify the appropriate parameter combination for the VBS approach and hence to provide valuable information to improve our understanding of OA production.
54 ENVIRONMENTAL SCIENCES↗
Multi-Model Impacts of Climate Change on Pollution Transport from Global Emission Source Regions
The impacts of climate change on tropospheric transport, diagnosed from a carbon monoxide (CO)-like tracer species emitted from global CO sources, are evaluated from an ensemble of four chemistry-climate model (CCMs) contributing to the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). Model time-slice simulations for present-day and end of the 21st century conditions were performed under the Representative Concentrations Pathways (RCP) climate scenario RCP 8.5. All simulations reveal a strong seasonality in transport, especially over the tropics. The highest CO-tracer mixing ratios aloft occur during boreal winter when strong vertical transport is co-located with biomass burning emission source regions. A consistent and robust decrease in future CO-tracer mixing ratios throughout most of the troposphere, especially in the tropics, and an increase around the tropopause is found across the four CCMs in both winter and summer. Decreases in CO-tracer mixing ratios in the tropical troposphere are associated with reduced convective mass fluxes in this region, which in turn may reflect a weaker Hadley Cell circulation in the future climate. Increases in CO-tracer mixing ratios near the tropopause are largely attributable to a rise in tropopause height, although a poleward shift in the midlatitude jets may also play an important role in the extra-tropical upper troposphere. An increase in CO-tracer mixing ratios also occurs near the Equator, centred over EquatorialCentral Africa, extending from the surface to the mid troposphere which is most likely related to localised decreases in convection in the vicinity of the Intertropical Convergence Zone, resulting in larger CO-tracer mixing ratios over biomass burning regions and smaller mixing ratios downwind.
Tropospheric Transport↗
The Influence of Ozone Precursor Emissions from Four World Regions on Tropospheric Composition and Radiative Climate Forcing
Ozone (O3) precursor emissions influence regional and global climate and air quality through changes in tropospheric O3 and oxidants, which also influence methane (CH4) and sulfate aerosols (SO4 (sup 2-)). We examine changes in the tropospheric composition of O3, CH4, SO4 (sup 2-) and global net radiative forcing (RF) for 20% reductions in global CH4 burden and in anthropogenic O3 precursor emissions (NOx, NMVOC, and CO) from four regions (East Asia, Europe and Northern Africa, North America, and South Asia) using the Task Force on Hemispheric Transport of Air Pollution Source-Receptor global chemical transport model (CTM) simulations, assessing uncertainty (mean plus or minus 1 standard deviation) across multiple CTMs. We evaluate steady state O3 responses, including long-term feedbacks via CH4. With a radiative transfer model that includes greenhouse gases and the aerosol direct effect, we find that regional NOx reductions produce global, annually averaged positive net RFs (0.2 plus or minus 0.6 to 1.7 2 mWm(sup -2)/Tg N yr(sup -1), with some variation among models. Negative net RFs result from reductions in global CH4 (-162.6 plus or minus 2 mWm(sup -2) for a change from 1760 to 1408 ppbv CH4) and regional NMVOC (-0.4 plus or minus 0.2 to 0.7 plus or minus 0.2 mWm(sup -2)/Tg C yr(sup -1) and CO emissions (-0.13 plus or minus 0.02 to -0.15 plus or minus 0.02 mWm(sup-2)/Tg CO yr(sup-1). Including the effect of O3 on CO2 uptake by vegetation likely makes these net RFs more negative by -1.9 to- 5.2 mWm(sup -2)/Tg N yr(sup -1), -0.2 to -0.7 mWm(sup -2)/Tg C yr(sup -1), and -0.02 to -0.05 mWm(sup -2)/ Tg CO yr(sup -1). Net RF impacts reflect the distribution of concentration changes, where RF is affected locally by changes in SO4 (sup -2), regionally to hemispherically by O3, and globally by CH4. Global annual average SO4 2 responses to oxidant changes range from 0.4 plus or minus 2.6 to -1.9 plus or minus 1.3 Gg for NOx reductions, 0.1 plus or minus 1.2 to -0.9 plus or minus 0.8 Gg for NMVOC reductions, and -0.09 plus or minus 0.5 to -0.9 plus or minus 0.8 Gg for CO reductions, suggesting additional research is needed. The 100-year global warming potentials (GWP(sub 100)) are calculated for the global CH4 reduction (20.9 plus or minus 3.7 without stratospheric O3 or water vapor, 24.2 plus or minus 4.2 including those components), and for the regional NOx, NMVOC, and CO reductions (18.7 plus or minus 25.9 to 1.9 plus or minus 8.7 for NOx, 4.8 plus or minus 1.7 to 8.3 plus or minus 1.9 for NMVOC, and 1.5 plus or minus 0.4 to 1.7 plus or minus 0.5 for CO). Variation in GWP(sub 100) for NOx, NMVOC, and CO suggests that regionally specific GWPs may be necessary and could support the inclusion of O3 precursors in future policies that address air quality and climate change simultaneously. Both global net RF and GWP100 are more sensitive to NOx and NMVOC reductions from South Asia than the other three regions.
ozone↗