Urban areas are recognised as a significant source of greenhouse gas emissions (GHG), such as carbon dioxide (CO 2 ) and methane (CH 4 ). The total amount of urban GHG emissions, especially for CH 4 , however, is not well quantified. Here we report on airborne in situ measurements using a Picarro G1301-m analyser aboard the DLR Cessna Grand Caravan to study GHG emissions downwind of the German capital Berlin. In total, five aircraft-based mass balance experiments were conducted in July 2018 within the Urban Climate Under Change [UC] 2 project. The detection and isolation of the Berlin plume was often challenging because of comparatively small GHG signals above variable atmospheric background concentrations. However, on July 20 th enhancements of up to 4 ppm CO 2 and 21 ppb CH 4 were observed over a horizontal extent of roughly 45 to 65 km downwind of Berlin. These enhanced mixing ratios are clearly distinguishable from the background and can partly be assigned to city emissions. The estimated CO 2 emission flux of 1.39 ± 0.76 t s –1 is in agreement with current inventories, while the CH 4 emission flux of 5.20 ± 1.70 kg s –1 is almost two times larger than the highest reported value in the inventories. We localized the source area with HYSPLIT trajectory calculations and the global/regional nested chemistry climate model MECO(n) (down to ~1 km), and investigated the contribution from sewage-treatment plants and waste deposition to CH 4 , which are treated differently by the emission inventories. Our work highlights the importance of strong CH 4 sources in the vicinity of Berlin and shows, that there is limited understanding of CH 4 emissions from urban regions, even for major cities in highly developed countries like Germany. Furthermore, we show that a detailed knowledge of GHG inflow mixing ratios is necessary to suitably estimate emission rates for Berlin.

The goal of the Tropospheric Ozone Assessment Report (TOAR) is to provide the research community with an up-to-date scientific assessment of tropospheric ozone, from the surface to the tropopause. While a suite of observations provides significant information on the spatial and temporal distribution of tropospheric ozone, observational gaps make it necessary to use global atmospheric chemistry models to synthesize our understanding of the processes and variables that control tropospheric ozone abundance and its variability. Models facilitate the interpretation of the observations and allow us to make projections of future tropospheric ozone and trace gas distributions for different anthropogenic or natural perturbations. This paper assesses the skill of current-generation global atmospheric chemistry models in simulating the observed present-day tropospheric ozone distribution, variability, and trends. Drawing upon the results of recent international multi-model intercomparisons and using a range of model evaluation techniques, we demonstrate that global chemistry models are broadly skillful in capturing the spatio-temporal variations of tropospheric ozone over the seasonal cycle, for extreme pollution episodes, and changes over interannual to decadal periods. However, models are consistently biased high in the northern hemisphere and biased low in the southern hemisphere, throughout the depth of the troposphere, and are unable to replicate particular metrics that define the longer term trends in tropospheric ozone as derived from some background sites. When the models compare unfavorably against observations, we discuss the potential causes of model biases and propose directions for future developments, including improved evaluations that may be able to better diagnose the root cause of the model-observation disparity. Overall, model results should be approached critically, including determining whether the model performance is acceptable for the problem being addressed, whether biases can be tolerated or corrected, whether the model is appropriately constituted, and whether there is a way to satisfactorily quantify the uncertainty.

Gathering pipelines, which transport gas from well pads to downstream processing, are a sector of the natural gas supply chain for which little measured methane emissions data are available. This study performed leak detection and measurement on 96 km of gathering pipeline and the associated 56 pigging facilities and 39 block valves. The study found one underground leak accounting for 83% (4.0 kg CH 4 /hr) of total measured emissions. Methane emissions for the 4684 km of gathering pipeline in the study area were estimated at 402 kg CH 4 /hr [95 to 1065 kg CH 4 /hr, 95% CI], or 1% [0.2% to 2.6%] of all methane emissions measured during a prior aircraft study of the same area. Emissions estimated by this study fall within the uncertainty range of emissions estimated using emission factors from EPA’s 2015 Greenhouse Inventory and study activity estimates. While EPA’s current inventory is based upon emission factors from distribution mains measured in the 1990s, this study indicates that using emission factors from more recent distribution studies could significantly underestimate emissions from gathering pipelines. To guide broader studies of pipeline emissions, we also estimate the fraction of the pipeline length within a basin that must be measured to constrain uncertainty of pipeline emissions estimates to within 1% of total basin emissions. The study provides both substantial insight into the mix of emission sources and guidance for future gathering pipeline studies, but since measurements were made in a single basin, the results are not sufficiently representative to provide methane emission factors at the regional or national level.

We assess the detectability of city emissions via a tower-based greenhouse gas (GHG) network, as part of the Indianapolis Flux (INFLUX) experiment. By examining afternoon-averaged results from a network of carbon dioxide (CO 2 ), methane (CH 4 ), and carbon monoxide (CO) mole fraction measurements in Indianapolis, Indiana for 2011–2013, we quantify spatial and temporal patterns in urban atmospheric GHG dry mole fractions. The platform for these measurements is twelve communications towers spread across the metropolitan region, ranging in height from 39 to 136 m above ground level, and instrumented with cavity ring-down spectrometers. Nine of the sites were deployed as of January 2013 and data from these sites are the focus of this paper. A background site, chosen such that it is on the predominantly upwind side of the city, is utilized to quantify enhancements caused by urban emissions. Afternoon averaged mole fractions are studied because this is the time of day during which the height of the boundary layer is most steady in time and the area that influences the tower measurements is likely to be largest. Additionally, atmospheric transport models have better performance in simulating the daytime convective boundary layer compared to the nighttime boundary layer. Averaged from January through April of 2013, the mean urban dormant-season enhancements range from 0.3 ppm CO 2 at the site 24 km typically downwind of the edge of the city (Site 09) to 1.4 ppm at the site at the downwind edge of the city (Site 02) to 2.9 ppm at the downtown site (Site 03). When the wind is aligned such that the sites are downwind of the urban area, the enhancements are increased, to 1.6 ppm at Site 09, and 3.3 ppm at Site 02. Differences in sampling height affect the reported urban enhancement by up to 50%, but the overall spatial pattern remains similar. The time interval over which the afternoon data are averaged alters the calculated urban enhancement by an average of 0.4 ppm. The CO 2 observations are compared to CO 2 mole fractions simulated using a mesoscale atmospheric model and an emissions inventory for Indianapolis. The observed and modeled CO 2 enhancements are highly correlated (r 2 = 0.94), but the modeled enhancements prior to inversion average 53% of those measured at the towers. Following the inversion, the enhancements follow the observations closely, as expected. The CH 4 urban enhancement ranges from 5 ppb at the site 10 km predominantly downwind of the city (Site 13) to 21 ppb at the site near the landfill (Site 10), and for CO ranges from 6 ppb at the site 24 km downwind of the edge of the city (Site 09) to 29 ppb at the downtown site (Site 03). Overall, these observations show that a dense network of urban GHG measurements yield a detectable urban signal, well-suited as input to an urban inversion system given appropriate attention to sampling time, sampling altitude and quantification of background conditions.

To effectively address climate change, aggressive mitigation policies need to be implemented to reduce greenhouse gas emissions. Anthropogenic carbon emissions are mostly generated from urban environments, where human activities are spatially concentrated. Improvements in uncertainty determinations and precision of measurement techniques are critical to permit accurate and precise tracking of emissions changes relative to the reduction targets. As part of the INFLUX project, we quantified carbon dioxide (CO 2 ), carbon monoxide (CO) and methane (CH 4 ) emission rates for the city of Indianapolis by averaging results from nine aircraft-based mass balance experiments performed in November-December 2014. Our goal was to assess the achievable precision of the aircraft-based mass balance method through averaging, assuming constant CO 2 , CH 4 and CO emissions during a three-week field campaign in late fall. The averaging method leads to an emission rate of 14,600 mol/s for CO 2 , assumed to be largely fossil-derived for this period of the year, and 108 mol/s for CO. The relative standard error of the mean is 17% and 16%, for CO 2 and CO, respectively, at the 95% confidence level (CL), i.e. a more than 2-fold improvement from the previous estimate of ~40% for single-flight measurements for Indianapolis. For CH 4 , the averaged emission rate is 67 mol/s, while the standard error of the mean at 95% CL is large, i.e. ±60%. Given the results for CO 2 and CO for the same flight data, we conclude that this much larger scatter in the observed CH 4 emission rate is most likely due to variability of CH 4 emissions, suggesting that the assumption of constant daily emissions is not correct for CH 4 sources. This work shows that repeated measurements using aircraft-based mass balance methods can yield sufficient precision of the mean to inform emissions reduction efforts by detecting changes over time in urban emissions.

We present a high-resolution atmospheric inversion system combining a Lagrangian Particle Dispersion Model (LPDM) and the Weather Research and Forecasting model (WRF), and test the impact of assimilating meteorological observation on transport accuracy. A Four Dimensional Data Assimilation (FDDA) technique continuously assimilates meteorological observations from various observing systems into the transport modeling system, and is coupled to the high resolution CO 2 emission product Hestia to simulate the atmospheric mole fractions of CO 2 . For the Indianapolis Flux Experiment (INFLUX) project, we evaluated the impact of assimilating different meteorological observation systems on the linearized adjoint solutions and the CO 2 inverse fluxes estimated using observed CO 2 mole fractions from 11 out of 12 communications towers over Indianapolis for the Sep.-Nov. 2013 period. While assimilating WMO surface measurements improved the simulated wind speed and direction, their impact on the planetary boundary layer (PBL) was limited. Simulated PBL wind statistics improved significantly when assimilating upper-air observations from the commercial airline program Aircraft Communications Addressing and Reporting System (ACARS) and continuous ground-based Doppler lidar wind observations. Wind direction mean absolute error (MAE) decreased from 26 to 14 degrees and the wind speed MAE decreased from 2.0 to 1.2 m s –1 , while the bias remains small in all configurations (< 6 degrees and 0.2 m s –1 ). Wind speed MAE and ME are larger in daytime than in nighttime. PBL depth MAE is reduced by ~10%, with little bias reduction. The inverse results indicate that the spatial distribution of CO 2 inverse fluxes were affected by the model performance while the overall flux estimates changed little across WRF simulations when aggregated over the entire domain. Our results show that PBL wind observations are a potent tool for increasing the precision of urban meteorological reanalyses, but that the impact on inverse flux estimates is dependent on the specific urban environment.

Improved quantification of diverse CH 4 sources at the urban scale is needed to guide local GHG mitigation strategies in the Anthropocene. Herein, we focus on landfill CH 4 emissions in California, challenging the current IPCC methodology which focuses on a climate dependency for landfill CH 4 generation (methanogenesis), but does not explicitly consider climate or soil dependencies for emissions. Relying on a comprehensive California landfill database, a field-validated process-based model for landfill CH 4 emissions (CALMIM), and select field measurements at 10 California sites with a variety of methods, we support the contrary position: Limited climate dependency for methanogenesis, but strong climate dependency for landfill CH 4 emissions. Contrary to the historic IPCC empirical model for methanogenesis with kinetic constants related to climate, we demonstrate a simpler and more robust linear empirical relationship (r 2 = 0.85; n=128) between waste mass and landfill biogas recovery [126 × 10 -6 Nm 3 CH 4 hr -1 Mg waste -1 ]. More interestingly, there are no statistically significant relationships with climate, site age, or status (open/closed) for landfill biogas recovery. The current IPCC methodology does not consider soil or climate drivers for gaseous transport or seasonal methanotrophy in different cover soils. On the other hand, we illustrate strong climate and soil dependencies for landfill emissions—e.g., average intermediate cover emissions below 20 g CH 4 m -2 d -1 when the site’s mean annual precipitation is >500 mm y -1 . Thereby, for the California landfill CH 4 inventory, the highest-emitting sites shift from landfills containing the largest mass of waste to sites dominated by intermediate cover types having a reduced rate of soil CH 4 oxidation during the annual cycle. These differences have profound implications for developing more realistic, science-based urban and regional scale GHG inventories for landfill CH 4 while reducing uncertainties for this important anthropogenic source.