133 research outputs found
Recommended from our members
A multiphase CMAQ version 5.0 adjoint
We present the development of a multiphase adjoint for the Community Multiscale Air Quality (CMAQ) model, a widely used chemical transport model. The adjoint model provides location- and time-specific gradients that can be used in various applications such as backward sensitivity analysis, source attribution, optimal pollution control, data assimilation, and inverse modeling. The science processes of the CMAQ model include gas-phase chemistry, aerosol dynamics and thermodynamics, cloud chemistry and dynamics, diffusion, and advection. Discrete adjoints are implemented for all the science processes, with an additional continuous adjoint for advection. The development of discrete adjoints is assisted with algorithmic differentiation (AD) tools. Particularly, the Kinetic PreProcessor (KPP) is implemented for gas-phase and aqueous chemistry, and two different automatic differentiation tools are used for other processes such as clouds, aerosols, diffusion, and advection. The continuous adjoint of advection is developed manually. For adjoint validation, the brute-force or finite-difference method (FDM) is implemented process by process with box- or column-model simulations. Due to the inherent limitations of the FDM caused by numerical round-off errors, the complex variable method (CVM) is adopted where necessary. The adjoint model often shows better agreement with the CVM than with the FDM. The adjoints of all science processes compare favorably with the FDM and CVM. In an example application of the full multiphase adjoint model, we provide the first estimates of how emissions of particulate matter (PM2.5) affect public health across the US.
</div
Recommended from our members
The impact of future emission policies on tropospheric ozone using a parameterised approach
This study quantifies future changes in tropospheric ozone (O3) using a simple parameterisation of source–receptor relationships based on simulations from a range of models participating in the Task Force on Hemispheric Transport of Air Pollutants (TF-HTAP) experiments. Surface and tropospheric O3 changes are calculated globally and across 16 regions from perturbations in precursor emissions (NOx, CO, volatile organic compounds – VOCs) and methane (CH4) abundance only, neglecting any impact from climate change. A source attribution is provided for each source region along with an estimate of uncertainty based on the spread of the results from the models. Tests against model simulations using the Hadley Centre Global Environment Model version 2 – Earth system configuration (HadGEM2-ES) confirm that the approaches used within the parameterisation perform well for most regions. The O3 response to changes in CH4 abundance is slightly larger in the TF-HTAP Phase 2 than in the TF-HTAP Phase 1 assessment (2010) and provides further evidence that controlling CH4 is important for limiting future O3 concentrations. Different treatments of chemistry and meteorology in models remain one of the largest uncertainties in calculating the O3 response to perturbations in CH4 abundance and precursor emissions, particularly over the Middle East and south Asia regions. Emission changes for the future Evaluating the CLimate and Air Quality ImPacts of Short-livEd Pollutants (ECLIPSE) scenarios and a subset of preliminary Shared Socioeconomic Pathways (SSPs) indicate that surface O3 concentrations will increase regionally by 1 to 8 ppbv in 2050. Source attribution analysis highlights the growing importance of CH4 in the future under current legislation. A change in the global tropospheric O3 radiative forcing of +0.07 W m−2 from 2010 to 2050 is predicted using the ECLIPSE scenarios and SSPs, based solely on changes in CH4 abundance and tropospheric O3 precursor emissions and neglecting any influence of climate change. Current legislation is shown to be inadequate in limiting the future degradation of surface ozone air quality and enhancement of near-term climate warming. More stringent future emission controls provide a large reduction in both surface O3 concentrations and O3 radiative forcing. The parameterisation provides a simple tool to highlight the different impacts and associated uncertainties of local and hemispheric emission control strategies on both surface air quality and the near-term climate forcing by tropospheric O3
Recommended from our members
Four-dimensional variational inversion of black carbon emissions during ARCTAS-CARB with WRFDA-Chem
Biomass burning emissions of atmospheric aerosols, including black carbon, are growing due to increased global drought, and comprise a large source of uncertainty in regional climate and air quality studies. We develop and apply new incremental four-dimensional variational (4D-Var) capabilities in WRFDA-Chem to find optimal spatially and temporally distributed biomass burning (BB) and anthropogenic black carbon (BC) aerosol emissions. The constraints are provided by aircraft BC concentrations from the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites in collaboration with the California Air Resources Board (ARCTAS-CARB) field campaign and surface BC concentrations from the Interagency Monitoring of PROtected Visual Environment (IMPROVE) network on 22, 23, and 24 June 2008. We consider three BB inventories, including Fire INventory from NCAR (FINN) v1.0 and v1.5 and Quick Fire Emissions Database (QFED) v2.4r8. On 22 June, aircraft observations are able to reduce the spread between a customized QFED inventory and FINNv1.0 from a factor of 3. 5 ( × 3. 5) to only × 2. 1. On 23 and 24 June, the spread is reduced from × 3. 4 to × 1. 4. The posterior corrections to emissions are heterogeneous in time and space, and exhibit similar spatial patterns of sign for both inventories. The posterior diurnal BB patterns indicate that multiple daily emission peaks might be warranted in specific regions of California. The US EPA's 2005 National Emissions Inventory (NEI05) is used as the anthropogenic prior. On 23 and 24 June, the coastal California posterior is reduced by × 2, where highway sources dominate, while inland sources are increased near Barstow by × 5. Relative BB emission variances are reduced from the prior by up to 35 % in grid cells close to aircraft flight paths and by up to 60 % for fires near surface measurements. Anthropogenic variance reduction is as high as 40 % and is similarly limited to sources close to observations. We find that the 22 June aircraft observations are able to constrain approximately 14 degrees of freedom of signal (DOF), while surface and aircraft observations together on 23/24 June constrain 23 DOF. Improving hourly- to daily-scale concentration predictions of BC and other aerosols during BB events will require more comprehensive and/or targeted measurements and a more complete accounting of sources of error besides the emissions
Response of the ozone-related health burden in Europe to changes in local anthropogenic emissions of ozone precursors
Recommended from our members
Sources of springtime surface black carbon in the Arctic: an adjoint analysis for April 2008
We quantify source contributions to springtime (April 2008) surface black carbon (BC) in the Arctic by interpreting surface observations of BC at five receptor sites (Denali, Barrow, Alert, Zeppelin, and Summit) using a global chemical transport model (GEOS-Chem) and its adjoint. Contributions to BC at Barrow, Alert, and Zeppelin are dominated by Asian anthropogenic sources (40–43 %) before 18 April and by Siberian open biomass burning emissions (29–41 %) afterward. In contrast, Summit, a mostly free tropospheric site, has predominantly an Asian anthropogenic source contribution (24–68 %, with an average of 45 %). We compute the adjoint sensitivity of BC concentrations at the five sites during a pollution episode (20–25 April) to global emissions from 1 March to 25 April. The associated contributions are the combined results of these sensitivities and BC emissions. Local and regional anthropogenic sources in Alaska are the largest anthropogenic sources of BC at Denali (63 % of total anthropogenic contributions), and natural gas flaring emissions in the western extreme north of Russia (WENR) are the largest anthropogenic sources of BC at Zeppelin (26 %) and Alert (13 %). We find that long-range transport of emissions from Beijing–Tianjin–Hebei (also known as Jing–Jin–Ji), the biggest urbanized region in northern China, contribute significantly (∼ 10 %)to surface BC across the Arctic. On average, it takes ∼ 12 days for Asian anthropogenic emissions and Siberian biomass burning emissions to reach the Arctic lower troposphere, supporting earlier studies. Natural gas flaring emissions from the WENR reach Zeppelin in about a week. We find that episodic transport events dominate BC at Denali (87 %), a site outside the Arctic front, which is a strong transport barrier. The relative contribution of these events to surface BC within the polar dome is much smaller (∼ 50 % at Barrow and Zeppelin and ∼ 10 % at Alert). The large contributions from Asian anthropogenic sources are predominately in the form of chronic pollution (∼ 40 % at Barrow, 65 % at Alert, and 57 % at Zeppelin) on about a 1-month timescale. As such, it is likely that previous studies using 5- or 10-day trajectory analyses strongly underestimated the contribution from Asia to surface BC in the Arctic
Recommended from our members
How well can inverse analyses of high-resolution satellite data resolve heterogeneous methane fluxes? Observing system simulation experiments with the GEOS-Chem adjoint model (v35)
We perform observing system simulation experiments (OSSEs) with the GEOS-Chem adjoint model to test how well methane emissions over North America can be resolved using measurements from the TROPOspheric Monitoring Instrument (TROPOMI) and similar high-resolution satellite sensors. We focus analysis on the impacts of (i) spatial errors in the prior emissions and (ii) model transport errors. Along with a standard scale factor (SF) optimization we conduct a set of inversions using alternative formalisms that aim to overcome limitations in the SF-based approach that arise for missing sources. We show that 4D-Var analysis of the TROPOMI data can improve monthly emission estimates at 25 km even with a spatially biased prior or model transport errors (42 %–93 % domain-wide bias reduction; R increases from 0.51 up to 0.73). However, when both errors are present, no single inversion framework can successfully improve both the overall bias and spatial distribution of fluxes relative to the prior on the 25 km model grid. In that case, the ensemble-mean optimized fluxes have a domain-wide bias of 77 Gg d−1 (comparable to that in the prior), with spurious source adjustments compensating for the transport errors. Increasing observational coverage through longer-timeframe inversions does not significantly change this picture. An inversion formalism that optimizes emission enhancements rather than scale factors exhibits the best performance for identifying missing sources, while an approach combining a uniform background emission with the prior inventory yields the best performance in terms of overall spatial fidelity – even in the presence of model transport errors. However, the standard SF optimization outperforms both of these for the magnitude of the domain-wide flux. For the common scenario in which prior errors are non-random, approximate posterior error reduction calculations (derived via gradient-based randomization) for the inversions reflect the sensitivity to observations but have no spatial correlation with the actual emission improvements. This demonstrates that such information content analysis can be used for general observing system characterization but does not describe the spatial accuracy of the posterior emissions or of the actual emission improvements. Findings here highlight the need for careful evaluation of potential missing sources in prior emission datasets and for robust accounting of model transport errors in inverse analyses of the methane budget.
</div
Assessing Public Health Burden Associated with Exposure to Ambient Black Carbon in the United States
Black carbon (BC) is a significant component of fine particulate matter (PM2.5) air pollution, which has been linked to a series of adverse health effects, in particular premature mortality. Recent scientific research indicates that BC also plays an important role in climate change. Therefore, controlling black carbon emissions provides an opportunity for a double dividend. This study quantifies the national burden of mortality and morbidity attributable to exposure to ambient BC in the United States (US). We use GEOS–Chem, a global 3-D model of atmospheric composition to estimate the 2010 annual average BC levels at 0.5 x 0.667° resolution, and then re-grid to 12-km grid resolution across the continental US. Using PM2.5 mortality risk coefficient drawn from the American Cancer Society cohort study, the numbers of deaths due to BC exposure were estimated for each 12-km grid, and then aggregated to the county, state and national level. Given evidence that BC particles may pose a greater risk on human health than other components of PM2.5, we also conducted sensitivity analysis using BC-specific risk coefficients drawn from recent literature. We estimated approximately 14,000 deaths to result from the 2010 BC levels, and hundreds of thousands of illness cases, ranging from hospitalizations and emergency department visits to minor respiratory symptoms. Sensitivity analysis indicates that the total BC-related mortality could be even significantly larger than the above mortality estimate. Our findings indicate that controlling BC emissions would have substantial benefits for public health in the US
Assessing Public Health Burden Associated with Exposure to Ambient Black Carbon in the United States
Black carbon (BC) is a significant component of fine particulate matter (PM2.5) air pollution, which has been linked to a series of adverse health effects, in particular premature mortality. Recent scientific research indicates that BC also plays an important role in climate change. Therefore, controlling black carbon emissions provides an opportunity for a double dividend. This study quantifies the national burden of mortality and morbidity attributable to exposure to ambient BC in the United States (US). We use GEOS–Chem, a global 3-D model of atmospheric composition to estimate the 2010 annual average BC levels at 0.5 x 0.667° resolution, and then re-grid to 12-km grid resolution across the continental US. Using PM2.5 mortality risk coefficient drawn from the American Cancer Society cohort study, the numbers of deaths due to BC exposure were estimated for each 12-km grid, and then aggregated to the county, state and national level. Given evidence that BC particles may pose a greater risk on human health than other components of PM2.5, we also conducted sensitivity analysis using BC-specific risk coefficients drawn from recent literature. We estimated approximately 14,000 deaths to result from the 2010 BC levels, and hundreds of thousands of illness cases, ranging from hospitalizations and emergency department visits to minor respiratory symptoms. Sensitivity analysis indicates that the total BC-related mortality could be even significantly larger than the above mortality estimate. Our findings indicate that controlling BC emissions would have substantial benefits for public health in the US
- …