Validation of Regional CO2 Concentrations in the ECMWF Real-Time Analysis and Carbon-Tracker Reanalysis with Airborne Observations from ACT-A Field Campaign

Through verifying against hundreds of hours of airborne in-situ measurements from the NASA-sponsored Atmospheric Carbon and Transport America (ACT-A) field campaign, this study systematically examines the regional uncertainties and biases of the carbon dioxide (CO2) concentrations from two of the state-of-the-art global analysis products, namely the real-time analysis from the European Center (EC) for Medium Range Forecasting and NOAAs near real-time Carbon Tracker (CT) reanalysis. It is found that both the EC and CT-NRT analyses agree reasonably well with the independent ACT-A flight-level CO2 measurements in the free troposphere but the uncertainties are considerably larger in the boundary layer during both the summer months of 2016 and the winter months of 2017. There are also strong variabilities in accuracy and bias between seasons, and across three different subregions in the United States (Mid-Atlantic, Midwest and South). Overall, the analysis uncertainties of the EC and CT-NRT analyses in terms of root-mean square deviations against airborne data are comparable to each other, both of which are between 1-2 ppm in the free troposphere but can be as large as 10 ppm near the surface, which are grossly consistent with the difference between the two analyses. The current study not only provides systematic uncertainty estimates for both analysis products over North America but also demonstrated that these two independent estimates can be used to approximate the overall regional CO2 analysis uncertainties. Both statistics are important in future studies in quantifying the uncertainties of regional carbon concentration and flux estimates, as well as in assessing the impact of regional transport through more refined regional modeling and analysis systems

Anthropogenic Control over Wintertime Oxidation of Atmospheric Pollutants

Anthropogenic air pollutants such as nitrogen oxides (NO(x) = NO + NO(2)), sulfur dioxide (SO(2)), and volatile organic compounds (VOC), among others, are emitted to the atmosphere throughout the year from energy production and use, transportation, and agriculture. These primary pollutants lead to the formation of secondary pollutants such as fine particulate matter (PM(2.5)) and ozone (O(3)) and perturbations to the abundance and lifetimes of short-lived greenhouse gases. Free radical oxidation reactions driven by solar radiation govern the atmospheric lifetimes and transformations of most primary pollutants and thus their spatial distributions. During winter in the mid and high latitudes, where a large fraction of atmospheric pollutants are emitted globally, such photochemical oxidation is significantly slower. Using observations from a highly instrumented aircraft, we show that multi-phase reactions between gas-phase NO(x) reservoirs and aerosol particles, as well as VOC emissions from anthropogenic activities, lead to a suite of atypical radical precursors dominating the oxidizing capacity in polluted winter air, and thus, the distribution and fate of primary pollutants on a regional to global scale

Observation-based modeling of ozone chemistry in the Seoul metropolitan area during the Korea-United States Air Quality Study (KORUS-AQ)

The Seoul Metropolitan Area (SMA) has a population of 24 million and frequently experiences unhealthy levels of ozone (O3). In this work, measurements taken during the Korea-United States Air Quality Study (KORUS-AQ, 2016) are used to explore regional gradients in O3 and its chemical precursors, and an observationally-constrained 0-D photochemical box model is used to quantify key aspects of O3 production including its sensitivity to precursor gases. Box model performance was evaluated by comparing modeled concentrations of select secondary species to airborne measurements. These comparisons indicate that the steady state assumption used in 0-D box models cannot describe select intermediate species, highlighting the importance of having a broad suite of trace gases as model constraints. When fully constrained, aggregated statistics of modeled O3 production rates agreed with observed changes in O3, indicating that the box model was able to represent the majority of O3 chemistry. Comparison of airborne observations between urban Seoul and a downwind receptor site reveal a positive gradient in O3 coinciding with a negative gradient in NOx, no gradient in CH2O, and a slight positive gradient in modeled rates of O3 production. Together, these observations indicate a radical-limited (VOC-limited) O3 production environment in the SMA. Zero-out simulations identified C7+ aromatics as the dominant VOC contributors to O3 production, with isoprene and anthropogenic alkenes making smaller but appreciable contributions. Simulations of model sensitivity to decreases in NOx produced results that were not spatially uniform, with large increases in O3 production predicted for urban Seoul and decreases in O3 production predicted for far-outlying areas. The policy implications of this work are clear: Effective O3 mitigation strategies in the SMA must focus on reducing local emissions of C7+ aromatics, while reductions in NOx emissions may increase O3 in some areas but generally decrease the regional extent of O3 exposure

Cropland Carbon Uptake Delayed and Reduced by 2019 Midwest Floods

While large‐scale floods directly impact human lives and infrastructures, they also profoundly impact agricultural productivity. New satellite observations of vegetation activity and atmospheric CO₂ offer the opportunity to quantify the effects of such extreme events on cropland carbon sequestration. Widespread flooding during spring and early summer 2019 induced conditions that delayed crop planting across the U.S. Midwest. As a result, satellite observations of solar‐induced chlorophyll fluorescence from TROPOspheric Monitoring Instrument and Orbiting Carbon Observatory reveal a 16‐day shift in the seasonal cycle of photosynthesis relative to 2018, along with a 15% lower peak value. We estimate a reduction of 0.21 PgC in cropland gross primary productivity in June and July, partially compensated in August and September (+0.14 PgC). The extension of the 2019 growing season into late September is likely to have benefited from increased water availability and late‐season temperature. Ultimately, this change is predicted to reduce the crop productivity in the Midwest Corn/Soy belt by ~15% compared to 2018. Using an atmospheric transport model, we show that a decline of ~0.1 PgC in the net carbon uptake during June and July is consistent with observed CO₂ enhancements of up to 10 ppm in the midday boundary layer from Atmospheric Carbon and Transport‐America aircraft and over 3 ppm in column‐averaged dry‐air mole fractions from Orbiting Carbon Observatory. This study quantifies the impact of floods on cropland productivity and demonstrates the potential of combining solar‐induced chlorophyll fluorescence with atmospheric CO₂ observations to monitor regional carbon flux anomalies

Advances in the Projective Dynamics Method: A Procedure of Discretizing the Space applied to Markovian Processes

AbstractThe projection of a continuous space process to a discrete space process via the transition rates between neighboring bins allows us to relate a master equation to a solution of a stochastic differential equation. The presented method is formulated in its general form for the first time and tested with the Brownian Diffusion process of noninteracting particles with white noise in simple one-dimensional potentials. The comparison of the first passage time obtained with Projective Dynamics, Brownian motion simulations and analytical solutions show the accuracy of this method as well as a wide independence of the particular choice of the binning process