Accounting for Transport Error in Inversions: An Urban Synthetic Data Experiment.

We present and discuss the use of a high-dimensional computational method for atmospheric inversions that incorporates the space-time structure of transport and dispersion errors. In urban environments, transport and dispersion errors are largely the result of our inability to capture the true underlying transport of greenhouse gas (GHG) emissions to observational sites. Motivated by the impact of transport model error on estimates of fluxes of GHGs using in situ tower-based mole-fraction observations, we specifically address the need to characterize transport error structures in high-resolution large-scale inversion models. We do this using parametric covariance functions combined with shrinkage-based regularization methods within an Ensemble Transform Kalman Filter inversion setup. We devise a synthetic data experiment to compare the impact of transport and dispersion error component of the model-data mismatch covariance choices on flux retrievals and study the robustness of the method with respect to fewer observational constraints. We demonstrate the analysis in the context of inferring CO2 fluxes starting with a hypothesized prior in the Washington D.C. /Baltimore area constrained by a synthetic set of tower-based CO2 measurements within an observing system simulation experiment framework. This study demonstrates the ability of these simple covariance structures to substantially improve the estimation of fluxes over standard covariance models in flux estimation from urban regions.

Wintertime CO2, CH4, and CO Emissions Estimation for the Washington, DC-Baltimore Metropolitan Area Using an Inverse Modeling Technique.

Since greenhouse gas mitigation efforts are mostly being implemented in cities, the ability to quantify emission trends for urban environments is of paramount importance. However, previous aircraft work has indicated large daily variability in the results. Here we use measurements of CO2, CH4, and CO from aircraft over 5 days within an inverse model to estimate emissions from the DC-Baltimore region. Results show good agreement with previous estimates in the area for all three gases. However, aliasing caused by irregular spatiotemporal sampling of emissions is shown to significantly impact both the emissions estimates and their variability. Extensive sensitivity tests allow us to quantify the contributions of different sources of variability and indicate that daily variability in posterior emissions estimates is larger than the uncertainty attributed to the method itself (i.e., 17% for CO2, 24% for CH4, and 13% for CO). Analysis of hourly reported emissions from power plants and traffic counts shows that 97% of the daily variability in posterior emissions estimates is explained by accounting for the sampling in time and space of sources that have large hourly variability and, thus, caution must be taken in properly interpreting variability that is caused by irregular spatiotemporal sampling conditions.

Assessment of Planetary Boundary Layer parametrizations and urban heat island comparison: Impacts and implications for tracer transport.

Accurate simulation of planetary boundary layer height (PBLH) is key to greenhouse gas emission estimation, air quality prediction and weather forecasting. This manuscript describes an extensive performance assessment of several Weather Research and Forecasting (WRF) model configurations where novel observations from ceilometers, surface stations and a flux tower were used to study their ability to reproduce planetary boundary layer heights (PBLH) and the impact that the urban heat island (UHI) has on the modeled PBLHs in the greater Washington, D.C. area. In addition, CO2 measurements at two urban towers were compared to tracer transport simulations. The ensemble of models used 4 PBL parameterizations, 2 sources of initial and boundary conditions and 1 configuration including the building energy parameterization (BEP) urban canopy model. Results have shown low biases over the whole domain and period for wind speed, wind direction and temperature with no drastic differences between meteorological drivers. We find that PBLH errors are mostly positively correlated with sensible heat flux errors, and that modeled positive UHI intensities are associated with deeper modeled PBLs over the urban areas. In addition, we find that modeled PBLHs are typically biased low during nighttime for most of the configurations with the exception of those using the MYNN parametrization and that these biases directly translate to tracer biases. Overall, the configurations using MYNN scheme performed the best, reproducing the PBLH and CO2 molar fractions reasonably well during all hours, thus opening the door to future nighttime inverse modeling.

Single-Blind Quantification of Natural Gas Leaks from 1 km Distance Using Frequency Combs.

A new method is tested in a single-blind study for detection, attribution, and quantification of methane emissions from the natural gas supply chain, which contribute substantially to annual U.S. emissions. The monitoring approach couples atmospheric methane concentration measurements from an open-path dual frequency comb laser spectrometer with meteorological data in an inversion to characterize emissions. During single-blind testing, the spectrometer is placed >1 km from decommissioned natural gas equipment configured with intentional leaks of controllable rate. Single, steady emissions ranging from 0 to 10.7 g min-1 (0-34.7 scfh) are detected, located, and quantified at three gas pads of varying size and complexity. The system detects 100% of leaks, including leaks as small as 0.96 g min-1 (3.1 scfh). It attributes leaks to the correct pad or equipment group (tank battery, separator battery, wellhead battery) 100% of the time and to the correct equipment (specific separator, tank, or wellhead) 67% of the time. All leaks are quantified to within 3.7 g min-1 (12 scfh); 94% are quantified to within 2.8 g min-1 (9 scfh). These tests are an important initial demonstration of the methodology's viability for continuous monitoring of large regions, with extension to other trace gases and industries.

Tower-Based Greenhouse Gas Measurement Network Design---The National Institute of Standards and Technology North East Corridor Testbed.

The North-East Corridor (NEC) Testbed project is the 3rd of three NIST (National Institute of Standards and Technology) greenhouse gas emissions testbeds designed to advance greenhouse gas measurements capabilities. A design approach for a dense observing network combined with atmospheric inversion methodologies is described. The Advanced Research Weather Research and Forecasting Model with the Stochastic Time-Inverted Lagrangian Transport model were used to derive the sensitivity of hypothetical observations to surface greenhouse gas emissions (footprints). Unlike other network design algorithms, an iterative selection algorithm, based on a k-means clustering method, was applied to minimize the similarities between the temporal response of each site and maximize sensitivity to the urban emissions contribution. Once a network was selected, a synthetic inversion Bayesian Kalman filter was used to evaluate observing system performance. We present the performances of various measurement network configurations consisting of differing numbers of towers and tower locations. Results show that an overly spatially compact network has decreased spatial coverage, as the spatial information added per site is then suboptimal as to cover the largest possible area, whilst networks dispersed too broadly lose capabilities of constraining flux uncertainties. In addition, we explore the possibility of using a very high density network of lower cost and performance sensors characterized by larger uncertainties and temporal drift. Analysis convergence is faster with a large number of observing locations, reducing the response time of the filter. Larger uncertainties in the observations implies lower values of uncertainty reduction. On the other hand, the drift is a bias in nature, which is added to the observations and, therefore, biasing the retrieved fluxes.

Direct and Indirect Measurements and Modeling of Methane Emissions in Indianapolis, Indiana.

This paper describes process-based estimation of CH4 emissions from sources in Indianapolis, IN and compares these with atmospheric inferences of whole city emissions. Emissions from the natural gas distribution system were estimated from measurements at metering and regulating stations and from pipeline leaks. Tracer methods and inverse plume modeling were used to estimate emissions from the major landfill and wastewater treatment plant. These direct source measurements informed the compilation of a methane emission inventory for the city equal to 29 Gg/yr (5% to 95% confidence limits, 15 to 54 Gg/yr). Emission estimates for the whole city based on an aircraft mass balance method and from inverse modeling of CH4 tower observations were 41 ± 12 Gg/yr and 81 ± 11 Gg/yr, respectively. Footprint modeling using 11 days of ethane/methane tower data indicated that landfills, wastewater treatment, wetlands, and other biological sources contribute 48% while natural gas usage and other fossil fuel sources contribute 52% of the city total. With the biogenic CH4 emissions omitted, the top-down estimates are 3.5-6.9 times the nonbiogenic city inventory. Mobile mapping of CH4 concentrations showed low level enhancement of CH4 throughout the city reflecting diffuse natural gas leakage and downstream usage as possible sources for the missing residual in the inventory.