ALBERT

Description: 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.

Description: Smoke forecasts have been challenged by high uncertainty in fire emission estimates. We develop an inverse modeling system, the HYSPLIT-based Emissions Inverse Modeling System for wildfires (or HEIMS-fire), that estimates wildfire emissions from the transport and dispersion of smoke plumes as measured by satellite observations. A cost function quantifies the differences between model predictions and satellite measurements, weighted by their uncertainties. The system then minimizes this cost function by adjusting smoke sources until wildfire smoke emission estimates agree well with satellite observations. Based on HYSPLIT and Geostationary Operational Environmental Satellite (GOES) Aerosol/Smoke Product (GASP), the system resolves smoke source strength as a function of time and vertical level. Using a wildfire event that took place in the southeastern United States during November 2016, we tested the system's performance and its sensitivity to varying configurations of modeling options, including vertical allocation of emissions and spatial and temporal coverage of constraining satellite observations. Compared with currently operational BlueSky emission predictions, emission estimates from this inverse modeling system outperform in both reanalysis (21 out of 21 d; −27 % average root-mean-square-error change) and hindcast modes (29 out of 38 d; −6 % average root-mean-square-error change) compared with satellite observed smoke mass loadings.

Description: Currently, the National Oceanic and Atmospheric Administration (NOAA) National Weather Service (NWS) runs the HYSPLIT dispersion model with a unit mass release rate to predict the transport and dispersion of volcanic ash. The model predictions provide information for the Volcanic Ash Advisory Centers (VAAC) to issue advisories to meteorological watch offices, area control centers, flight information centers, and others. This research aims to provide quantitative forecasts of ash distributions generated by objectively and optimally estimating the volcanic ash source strengths, vertical distribution, and temporal variations using an observation-modeling inversion technique. In this top-down approach, a cost functional is defined to quantify the differences between the model predictions and the satellite measurements of column-integrated ash concentrations weighted by the model and observation uncertainties. Minimizing this cost functional by adjusting the sources provides the volcanic ash emission estimates. As an example, MODIS (Moderate Resolution Imaging Spectroradiometer) satellite retrievals of the 2008 Kasatochi volcanic ash clouds are used to test the HYSPLIT volcanic ash inverse system. Because the satellite retrievals include the ash cloud top height but not the bottom height, there are different model diagnostic choices for comparing the model results with the observed mass loadings. Three options are presented and tested. Although the emission estimates vary significantly with different options, the subsequent model predictions with the different release estimates all show decent skill when evaluated against the unassimilated satellite observations at later times. Among the three options, integrating over three model layers yields slightly better results than integrating from the surface up to the observed volcanic ash cloud top or using a single model layer. Inverse tests also show that including the ash-free region to constrain the model is not beneficial for the current case. In addition, extra constraints on the source terms can be given by explicitly enforcing no-ash for the atmosphere columns above or below the observed ash cloud top height. However, in this case such extra constraints are not helpful for the inverse modeling. It is also found that simultaneously assimilating observations at different times produces better hindcasts than only assimilating the most recent observations.

Description: This study applies the Gridpoint Statistical Interpolation (GSI) 3D-Var assimilation tool originally developed by the National Centers for Environmental Prediction (NCEP), to improve surface PM2.5 predictions over the contiguous United States (CONUS) by assimilating aerosol optical depth (AOD) and surface PM2.5 in version 5.1 of the Community Multi-scale Air Quality (CMAQ) modeling system. An optimal interpolation (OI) method implemented earlier (Tang et al., 2015) for the CMAQ modeling system is also tested for the same period (July 2011) over the same CONUS. Both GSI and OI methods assimilate surface PM2.5 observations at 00:00, 06:00, 12:00 and 18:00 UTC, and MODIS AOD at 18:00 UTC. The assimilations of observations using both GSI and OI generally help reduce the prediction biases and improve correlation between model predictions and observations. In the GSI experiments, assimilation of surface PM2.5 (particle matter with diameter 

Description: This study applies the Gridpoint Statistical Interpolation (GSI) 3D-Var assimilation tool originally developed by the National Centers for Environmental Prediction (NCEP), to improve surface PM2.5 predictions over the contiguous United States (CONUS) by assimilating aerosol optical depth (AOD) and surface PM2.5 in version 5.1 of the Community Multi-scale Air Quality (CMAQ) modeling system. GSI results are compared with those obtained using the optimal interpolation (OI) method (Tang et al., 2015) for July, 2011 over CONUS. Both GSI and OI assimilate surface PM2.5 observations at 00, 06, 12, and 18 UTC, and MODIS AOD at 18 UTC. In the GSI experiments, assimilation of surface PM2.5 leads to stronger increments in surface PM2.5 compared to the MODIS AOD assimilation. In contrast, we find a stronger impact of MODIS AOD on surface aerosols at 18 UTC compared to the surface PM2.5 OI assimilation. The increments resulting from the OI assimilation are spread in 11×11 horizontal grid cells (12 km horizontal resolution) while the spatial distribution of GSI increments is controlled by its background error covariances, and the horizontal/vertical length scales. The assimilations of observations using both GSI and OI generally help reduce the prediction biases, and improve correlation between model predictions and observations. GSI produces smoother result and yields overall better correlation coefficient and root mean squared error (RMSE). In this study, OI uses the relatively big model uncertainties, which helps yield better mean biases, but sometimes causes the RMSE increase. We also examine and discuss the sensitivity of the assimilation experiments results to the AOD forward operators

Description: Currently NOAA's National Weather Service (NWS) runs the HYSPLIT dispersion model with a unit mass release rate to predict the transport and dispersion of volcanic ash. The model predictions provide information for the Volcanic Ash Advisory Centers (VAAC) to issue advisories to meteorological watch offices, area control centers, flight information centers, and others. This research aims provide quantitative forecasts of ash distributions generated by objectively and optimally estimating the volcanic ash source strengths, vertical distribution and temporal variations using an observation-modeling inversion technique. In this top-down approach, a cost functional is defined to mainly quantify the differences between model predictions and the satellite measurements of column integrated ash concentrations, weighted by the model and observation uncertainties. Minimizing this cost functional by adjusting the sources provides the volcanic ash emission estimates. As an example, MODIS (MOderate Resolution Imaging Spectroradiometer) satellite retrievals of the 2008 Kasatochi volcanic ash clouds are used to test the HYSPLIT volcanic ash inverse system. Because the satellite retrievals include the ash cloud top height but not the bottom height, three options for matching the model concentrations to the observed mass loadings are tested. Although the emission estimates vary significantly with different options the subsequent model predictions with the different release estimates all show decent skill when evaluated against the unassimilated satellite observations at later times. Among the three options, integrating over three model layers yields slightly better results than integrating from the surface up to the volcanic ash cloud top or using a single model layer. Inverse tests also show that including the ash-free region to constrain the model is not beneficial for the current case. In addition, extra constraints to the source terms can be given by explicitly enforcing ``no-ash'' for the atmosphere columns above or below the observed ash cloud top height. However, in this case such extra constraints are not helpful for the inverse modeling. It is also found that simultaneously assimilating observations at different times produces better hindcasts than only assimilating the most recent observations.

Description: A HYSPLIT inverse system that is based on variational data assimilation and a Lagrangian dispersion transfer coefficient matrix (TCM) is evaluated using the Cross Appalachian Tracer Experiment (CAPTEX) data collected from six controlled releases. For simplicity, the initial tests are applied to release 2 for which the HYSPLIT has the best performance. Before introducing model uncertainty terms, the tests using concentration differences in the cost function results in severe underestimation while those using logarithm concentrations differences results in overestimation of the release rate. Adding model uncertainty terms improves results for both choices of the metric variables in the cost function. A cost function normalization scheme is later introduced to avoid spurious minimal source term solutions when using logarithm concentration differences. The scheme is effective in eliminating the spurious solutions and it also helps to improve the release estimates for both choices of the metric variables. The tests also show that calculating logarithm concentration differences generally yield better results than calculating concentration differences and the estimates are more robust for a reasonable range of model uncertainty parameters. This is further confirmed with nine ensemble HYSPLIT runs in which meteorological fields were generated with varying planetary boundary layer (PBL) schemes. In addition, it is found that the emission estimate using a combined TCM by taking the average or median values of the nine TCMs is similar to the median of the nine estimates using each of the TCMs individually. The inverse system is then applied to the other CAPTEX releases with a fixed set of observational and model uncertainty parameters and the largest relative error among the six releases is 53.3%. At last, the system is tested for its capability to find a single source location as well as its source strength. In these tests, the location and strength that yield the best match between the predicted and the observed concentrations are considered as the inverse modeling results. The estimated release rates are mostly not as good as the cases in which the exact release locations are assumed known, but they are all within a factor of 3 for all the six releases. However, the estimated location may have large errors.

Description: A Hybrid Single-Particle Lagrangian Integrated Trajectory version 4 (HYSPLIT-4) inverse system that is based on variational data assimilation and a Lagrangian dispersion transfer coefficient matrix (TCM) is evaluated using the Cross-Appalachian Tracer Experiment (CAPTEX) data collected from six controlled releases. For simplicity, the initial tests are applied to release 2, for which the HYSPLIT has the best performance. Before introducing model uncertainty terms that will change with source estimates, the tests using concentration differences in the cost function result in severe underestimation, while those using logarithm concentration differences result in overestimation of the release rate. Adding model uncertainty terms improves results for both choices of the metric variables in the cost function. A cost function normalization scheme is later introduced to avoid spurious minimal source term solutions when using logarithm concentration differences. The scheme is effective in eliminating the spurious solutions and it also helps to improve the release estimates for both choices of the metric variables. The tests also show that calculating logarithm concentration differences generally yields better results than calculating concentration differences, and the estimates are more robust for a reasonable range of model uncertainty parameters. This is further confirmed with nine ensemble HYSPLIT runs in which meteorological fields were generated with varying planetary boundary layer (PBL) schemes. In addition, it is found that the emission estimate using a combined TCM by taking the average or median values of the nine TCMs is similar to the median of the nine estimates using each of the TCMs individually. The inverse system is then applied to the other CAPTEX releases with a fixed set of observational and model uncertainty parameters, and the largest relative error among the six releases is 53.3 %. At last, the system is tested for its capability to find a single source location as well as its source strength. In these tests, the location and strength that yield the best match between the predicted and the observed concentrations are considered as the inverse modeling results. The estimated release rates are mostly not as good as the cases in which the exact release locations are assumed known, but they are all within a factor of 3 for all six releases. However, the estimated location may have large errors.

Description: Ambient fine particulate matter (PM2.5) mitigation relies strongly on anthropogenic emission control measures, the actual effectiveness of which is challenging to pinpoint owing to the complex synergies between anthropogenic emissions and meteorology. Here, observational constraints on model simulations allow us to derive not only reliable PM2.5 evolution but also accurate meteorological fields. On this basis, we isolate meteorological factors to achieve reliable estimates of surface PM2.5 responses to both long-term and emergency emission control measures from 2016 to 2019 over the Yangtze River Delta (YRD), China. The results show that long-term emission control strategies play a crucial role in curbing PM2.5 levels, especially in the megacities and other areas with abundant anthropogenic emissions. The G20 summit hosted in Hangzhou in 2016 provides a unique and ideal opportunity involving the most stringent, even unsustainable, emergency emission control measures. These emergency measures lead to the largest decrease (∼ 35 µg m−3, ∼ 59 %) in PM2.5 concentrations in Hangzhou. The hotspots also emerge in megacities, especially in Shanghai (32 µg m−3, 51 %), Nanjing (27 µg m−3, 55 %), and Hefei (24 µg m−3, 44 %) because of the emergency measures. Compared to the long-term policies from 2016 to 2019, the emergency emission control measures implemented during the G20 Summit achieve more significant decreases in PM2.5 concentrations (17 µg m−3 and 41 %) over most of the whole domain, especially in Hangzhou (24 µg m−3, 48 %) and Shanghai (21 µg m−3, 45 %). By extrapolation, we derive insight into the magnitude and spatial distribution of PM2.5 mitigation potential across the YRD, revealing significantly additional room for curbing PM2.5 levels.

Description: Ammonia (NH3) emissions have large impacts on air quality and nitrogen deposition, influencing human health and the well-being of sensitive ecosystems. Large uncertainties exist in the “bottom-up” NH3 emission inventories due to limited source information and a historical lack of measurements, hindering the assessment of NH3-related environmental impacts. The increasing capability of satellites to measure NH3 abundance and the development of modeling tools enable us to better constrain NH3 emission estimates at high spatial resolution. In this study, we constrain the NH3 emission estimates from the widely used 2011 National Emissions Inventory (2011 NEI) in the US using Infrared Atmospheric Sounding Interferometer NH3 column density measurements (IASI-NH3) gridded at a 36 km by 36 km horizontal resolution. With a hybrid inverse modeling approach, we use the Community Multiscale Air Quality Modeling System (CMAQ) and its multiphase adjoint model to optimize NH3 emission estimates in April, July, and October. Our optimized emission estimates suggest that the total NH3 emissions are biased low by 26 % in 2011 NEI in April with overestimation in the Midwest and underestimation in the Southern States. In July and October, the estimates from NEI agree well with the optimized emission estimates, despite a low bias in hotspot regions. Evaluation of the inversion performance using independent observations shows reduced underestimation in simulated ambient NH3 concentration in all 3 months and reduced underestimation in NH4+ wet deposition in April. Implementing the optimized NH3 emission estimates improves the model performance in simulating PM2.5 concentration in the Midwest in April. The model results suggest that the estimated contribution of ammonium nitrate would be biased high in a priori NEI-based assessments. The higher emission estimates in this study also imply a higher ecological impact of nitrogen deposition originating from NH3 emissions.