Ensemble-based Chemical Data Assimilation III: Filter Localization

Data assimilation is the process of integrating observational data and model predictions to obtain an optimal representation of the state of the atmosphere. As more chemical observations in the troposphere are becoming available, chemical data assimilation is expected to play an essential role in air quality forecasting, similar to the role it has in numerical weather prediction. Considerable progress has been made recently in the development of variational tools for chemical data assimilation. In this paper we implement and assess the performance of a localized ``perturbed observations'' ensemble Kalman filter (LEnKF). We analyze different settings of the ensemble localization, and investigate the joint assimilation of the state, emissions and boundary conditions. Results with a real model and real observations show that LEnKF is a promising approach for chemical data assimilation. The results also point to several issues on which future research is necessary

Ensemble-based chemical data assimilation II: Real observations

Data assimilation is the process of integrating observational data and model predictions to obtain an optimal representation of the state of the atmosphere. As more chemical observations in the troposphere are becoming available, chemical data assimilation is expected to play an essential role in air quality forecasting, similar to the role it has in numerical weather prediction. Considerable progress has been made recently in the development of variational tools for chemical data assimilation. In this paper we assess the performance of the ensemble Kalman filter (EnKF) and compare it with a state of the art 4D-Var approach. We analyze different aspects that affect the assimilation process, investigate several ways to avoid filter divergence, and investigate the assimilation of emissions. Results with a real model and real observations show that EnKF is a promising approach for chemical data assimilation. The results also point to several issues on which further research is necessary

Ensemble-based chemical data assimilation I: An idealized setting

Data assimilation is the process of integrating observational data and model predictions to obtain an optimal representation of the state of the atmosphere. As more chemical observations in the troposphere are becoming available, chemical data assimilation is expected to play an essential role in air quality forecasting, similar to the role it has in numerical weather prediction. Considerable progress has been made recently in the development of variational tools for chemical data assimilation. In this paper we assess the performance of the ensemble Kalman filter (EnKF). Results in an idealized setting show that EnKF is promising for chemical data assimilation

Autoregressive Models of Background Errors for Chemical Data Assimilation

The task of providing an optimal analysis of the state of the atmosphere requires the development of dynamic data-driven systems that efficiently integrate the observational data and the models. Data assimilation (DA) is the process of adjusting the states or parameters of a model in such a way that its outcome (prediction) is close, in some distance metric, to observed (real) states. It is widely accepted that a key ingredient of successful data assimilation is a realistic estimation of the background error distribution. This paper introduces a new method for estimating the background errors which are modeled using autoregressive processes. The proposed approach is computationally inexpensive and captures the error correlations along the flow lines

Significant wintertime PM_(2.5) mitigation in the Yangtze River Delta, China, from 2016 to 2019: observational constraints on anthropogenic emission controls

Ambient fine particulate matter (PM_(2.5)) 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 PM_(2.5) evolution but also accurate meteorological fields. On this basis, we isolate meteorological factors to achieve reliable estimates of surface PM_(2.5) 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 PM_(2.5) 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 PM_(2.5) 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 PM_(2.5) 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 PM_(2.5) mitigation potential across the YRD, revealing significantly additional room for curbing PM_(2.5) levels

Improving regional ozone modeling through systematic evaluation of errors using the aircraft observations during the International Consortium for Atmospheric Research on Transport and Transformation

During the operational phase of the ICARTT field experiment in 2004, the regional air quality model STEM showed a strong positive surface bias and a negative upper troposphere bias (compared to observed DC-8 and WP-3 observations) with respect to ozone. After updating emissions from NEI 1999 to NEI 2001 (with a 2004 large point sources inventory update), and modifying boundary conditions, low-level model bias decreases from 11.21 to 1.45 ppbv for the NASA DC-8 observations and from 8.26 to −0.34 for the NOAA WP-3. Improvements in boundary conditions provided by global models decrease the upper troposphere negative ozone bias, while accounting for biomass burning emissions improved model performance for CO. The covariances of ozone bias were highly correlated to NOz, NOy, and HNO3 biases. Interpolation of bias information through kriging showed that decreasing emissions in SE United States would reduce regional ozone model bias and improve model correlation coefficients. The spatial distribution of forecast errors was analyzed using kriging, which identified distinct features, which when compared to errors in postanalysis simulations, helped document improvements. Changes in dry deposition to crops were shown to reduce substantially high bias in the forecasts in the Midwest, while updated emissions were shown to account for decreases in bias in the eastern United States. Observed and modeled ozone production efficiencies for the DC-8 were calculated and shown to be very similar (7.8) suggesting that recurring ozone bias is due to overestimation of NOx emissions. Sensitivity studies showed that ozone formation in the United States is most sensitive to NOx emissions, followed by VOCs and CO. PAN as a reservoir of NOx can contribute to a significant amount of surface ozone through thermal decomposition

Improving regional ozone modeling through systematic evaluation of errors using the aircraft observations during the International Consortium for Atmospheric Research on Transport and Transformation

During the operational phase of the ICARTT field experiment in 2004, the regional air quality model STEM showed a strong positive surface bias and a negative upper troposphere bias (compared to observed DC-8 and WP-3 observations) with respect to ozone. After updating emissions from NEI 1999 to NEI 2001 (with a 2004 large point sources inventory update), and modifying boundary conditions, low-level model bias decreases from 11.21 to 1.45 ppbv for the NASA DC-8 observations and from 8.26 to -0.34 for the NOAA WP-3. Improvements in boundary conditions provided by global models decrease the upper troposphere negative ozone bias, while accounting for biomass burning emissions improved model performance for CO. The covariances of ozone bias were highly correlated to NOz, NOy, and HNO3biases. Interpolation of bias information through kriging showed that decreasing emissions in SE United States would reduce regional ozone model bias and improve model correlation coefficients. The spatial distribution of forecast errors was analyzed using kriging, which identified distinct features, which when compared to errors in postanalysis simulations, helped document improvements. Changes in dry deposition to crops were shown to reduce substantially high bias in the forecasts in the Midwest, while updated emissions were shown to account for decreases in bias in the eastern United States. Observed and modeled ozone production efficiencies for the DC-8 were calculated and shown to be very similar (7.8) suggesting that recurring ozone bias is due to overestimation of NOxemissions. Sensitivity studies showed that ozone formation in the United States is most sensitive to NOxemissions, followed by VOCs and CO. PAN as a reservoir of NOxcan contribute to a significant amount of surface ozone through thermal decomposition

Influence of lateral and top boundary conditions on regional air quality prediction: A multiscale study coupling regional and global chemical transport models

The sensitivity of regional air quality model to various lateral and top boundary conditions is studied at 2 scales: a 60 km domain covering the whole USA and a 12 km domain over northeastern USA. Three global models (MOZART-NCAR, MOZART-GFDL and RAQMS) are used to drive the STEM-2K3 regional model with time-varied lateral and top boundary conditions (BCs). The regional simulations with different global BCs are examined using ICARTT aircraft measurements performed in the summer of 2004, and the simulations are shown to be sensitive to the boundary conditions from the global models, especially for relatively long-lived species, like CO and O3. Differences in the mean CO concentrations from three different global-model boundary conditions are as large as 40 ppbv, and the effects of the BCs on CO are shown to be important throughout the troposphere, even near surface. Top boundary conditions show strong effect on O3 predictions above 4 km. Over certain model grids, the model’s sensitivity to BCs is found to depend not only on the distance from the domain’s top and lateral boundaries, downwind/upwind situation, but also on regional emissions and species properties. The near-surface prediction over polluted area is usually not as sensitive to the variation of BCs, but to the magnitude of their background concentrations. We also test the sensitivity of model to temporal and spatial variations of the BCs by comparing the simulations with time-varied BCs to the corresponding simulations with time-mean and profile BCs. Removing the time variation of BCs leads to a significant bias on the variation prediction and sometime causes the bias in predicted mean values. The effect of model resolution on the BC sensitivity is also studied