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Satellites monitoring air pollutants (e.g., nitrogen oxides; NOx = NO + NO2) or greenhouse gases (GHGs) are widely utilized to understand the spatiotemporal variability in and evolution of emission characteristics, chemical transformations, and atmospheric transport over anthropogenic hotspots. Recently, the joint use of space-based long-lived GHGs (e.g., carbon dioxide; CO2) and short-lived pollutants has made it possible to improve our understanding of emission characteristics. Some previous studies, however, lack consideration of the non-linear NOx chemistry or complex atmospheric transport. Considering the increase in satellite data volume and the demand for emission monitoring at higher spatiotemporal scales, it is crucial to construct a local-scale emission optimization system that can handle both long-lived GHGs and short-lived pollutants in a coupled and effective manner. This need motivates us to develop a Lagrangian chemical transport model that accounts for NOx chemistry and fine-scale atmospheric transport (STILT–NOx) and to investigate how physical and chemical processes, anthropogenic emissions, and background may affect the interpretation of tropospheric NO2 columns (tNO2). Interpreting emission signals from tNO2 commonly involves either an efficient statistical model or a sophisticated chemical transport model. To balance computational expenses and chemical complexity, we describe a simplified representation of the NOx chemistry that bypasses an explicit solution of individual chemical reactions while preserving the essential non-linearity that links NOx emissions to its concentrations. This NOx chemical parameterization is then incorporated into an existing Lagrangian modeling framework that is widely applied in the GHG community. We further quantify uncertainties associated with the wind field and chemical parameterization and evaluate modeled columns against retrieved columns from the TROPOspheric Monitoring Instrument (TROPOMI v2.1). Specifically, simulations with alternative model configurations of emissions, meteorology, chemistry, and inter-parcel mixing are carried out over three United States (US) power plants and two urban areas across seasons. Using the U.S. Environmental Protection Agency (EPA)-reported emissions for power plants with non-linear NOx chemistry improves the model–data alignment in tNO2 (a high bias of ≤ 10 % on an annual basis), compared to simulations using either the Emissions Database for Global Atmospheric Research (EDGAR) model or without chemistry (bias approaching 100 %). The largest model–data mismatches are associated with substantial biases in wind directions or conditions of slower atmospheric mixing and photochemistry. More importantly, our model development illustrates (1) how NOx chemistry affects the relationship between NOx and CO2 in terms of the spatial and seasonal variability and (2) how assimilating tNO2 can quantify systematic biases in modeled wind directions and emission distribution in prior inventories of NOx and CO2, which laid a foundation for a local-scale multi-tracer emission optimization system.

When estimating fossil fuel carbon dioxide (FFCO2) emissions from observed CO2 concentrations, the accuracy can be hampered by biogenic carbon exchanges during the growing season, even for urban areas where strong fossil fuel emissions are found. While biogenic carbon fluxes have been studied extensively across natural vegetation types, biogenic carbon fluxes within an urban area have been challenging to quantify due to limited observations and differences between urban and rural regions. Here we developed a simple model representation, i.e., Solar-Induced Fluorescence (SIF) for Modeling Urban biogenic Fluxes (“SMUrF”), that estimates the gross primary production (GPP) and ecosystem respiration (Reco) over cities around the globe. Specifically, we leveraged space-based SIF, machine learning, eddy-covariance (EC) flux data, and ancillary remote-sensing-based products, and we developed algorithms to gap-fill fluxes for urban areas. Grid-level hourly mean net ecosystem exchange (NEE) fluxes are extracted from SMUrF and evaluated against (1) non-gap-filled measurements at 67 EC sites from FLUXNET during 2010–2014 (r>0.7 for most data-rich biomes), (2) independent observations at two urban vegetation and two crop EC sites over Indianapolis from August 2017 to December 2018 (r=0.75), and (3) an urban biospheric model based on fine-grained land cover classification in Los Angeles (r=0.83). Moreover, we compared SMUrF-based NEE with inventory-based FFCO2 emissions over 40 cities and addressed the urban–rural contrast in both the magnitude and timing of CO2 fluxes. To illustrate the application of SMUrF, we used it to interpret a few summertime satellite tracks over four cities and compared the urban–rural gradient in column CO2 (XCO2) anomalies due to NEE against XCO2 enhancements due to FFCO2 emissions. With rapid advances in space-based measurements and increased sampling of SIF and CO2 measurements over urban areas, SMUrF can be useful to inform the biogenic CO2 fluxes over highly vegetated regions during the growing season.

Urban regions are responsible for emitting significant amounts of fossil fuel carbon dioxide (FFCO2), and emissions at the finer, city scales are more uncertain than those aggregated at the global scale. Carbon-observing satellites may provide independent top-down emission evaluations and compensate for the sparseness of surface CO2 observing networks in urban areas. Although some previous studies have attempted to derive urban CO2 signals from satellite column-averaged CO2 data (XCO2) using simple statistical measures, less work has been carried out to link upwind emission sources to downwind atmospheric columns using atmospheric models. In addition to Eulerian atmospheric models that have been customized for emission estimates over specific cities, the Lagrangian modeling approach – in particular, the Lagrangian particle dispersion model (LPDM) approach – has the potential to efficiently determine the sensitivity of downwind concentration changes to upwind sources. However, when applying LPDMs to interpret satellite XCO2, several issues have yet to be addressed, including quantifying uncertainties in urban XCO2 signals due to receptor configurations and errors in atmospheric transport and background XCO2.In this study, we present a modified version of the Stochastic Time-Inverted Lagrangian Transport (STILT) model, X-STILT, for extracting urban XCO2 signals from NASA's Orbiting Carbon Observatory 2 (OCO-2) XCO2 data. X-STILT incorporates satellite profiles and provides comprehensive uncertainty estimates of urban XCO2 enhancements on a per sounding basis. Several methods to initialize receptor/particle setups and determine background XCO2 are presented and discussed via sensitivity analyses and comparisons. To illustrate X-STILT's utilities and applications, we examined five OCO-2 overpasses over Riyadh, Saudi Arabia, during a 2-year time period and performed a simple scaling factor-based inverse analysis. As a result, the model is able to reproduce most observed XCO2 enhancements. Error estimates show that the 68 % confidence limit of XCO2 uncertainties due to transport (horizontal wind plus vertical mixing) and emission uncertainties contribute to ∼ 33 % and ∼ 20 % of the mean latitudinally integrated urban signals, respectively, over the five overpasses, using meteorological fields from the Global Data Assimilation System (GDAS). In addition, a sizeable mean difference of −0.55 ppm in background derived from a previous study employing simple statistics (regional daily median) leads to a ∼ 39 % higher mean observed urban signal and a larger posterior scaling factor. Based on our signal estimates and associated error impacts, we foresee X-STILT serving as a tool for interpreting column measurements, estimating urban enhancement signals, and carrying out inverse modeling to improve quantification of urban emissions.

The Stochastic Time-Inverted Lagrangian Transport (STILT) model is comprised of a compiled Fortran executable that carries out advection and dispersion calculations as well as a higher-level code layer for simulation control and user interaction, written in the open-source data analysis language R. We introduce modifications to the STILT-R code base with the aim to improve the model's applicability to fine-scale (

We introduce the Polar Vegetation Photosynthesis and Respiration Model (PolarVPRM), a remote-sensing-based approach for generating accurate, high-resolution (≥ 1 km2, 3 hourly) estimates of net ecosystem CO2 exchange (NEE). PolarVPRM simulates NEE using polar-specific vegetation classes, and by representing high-latitude influences on NEE, such as the influence of soil temperature on subnivean respiration. We present a description, validation and error analysis (first-order Taylor expansion) of PolarVPRM, followed by an examination of per-pixel trends (2001–2012) in model output for the North American terrestrial region north of 55° N. PolarVPRM was validated against eddy covariance (EC) observations from nine North American sites, of which three were used in model calibration. Comparisons of EC NEE to NEE from three models indicated that PolarVPRM displayed similar or better statistical agreement with eddy covariance observations than existing models showed. Trend analysis (2001–2012) indicated that warming air temperatures and drought stress in forests increased growing season rates of respiration, and decreased rates of net carbon uptake by vegetation when air temperatures exceeded optimal temperatures for photosynthesis. Concurrent increases in growing season length at Arctic tundra sites allowed for increases in photosynthetic uptake over time by tundra vegetation. PolarVPRM estimated that the North American high-latitude region changed from a carbon source (2001–2004) to a carbon sink (2005–2010) to again a source (2011–2012) in response to changing environmental conditions.

A bidirectional air–surface exchange scheme for atmospheric ammonia was incorporated into the Stochastic Time-Inverted Lagrangian Transport air quality model (STILT-Chem v0.8). STILT-Chem v0.8 was then applied to simulate atmospheric ammonia concentrations at 53 measurement sites in the province of Ontario, Canada for a six-month period from 1 June to 30 November 2006. In addition to the bidirectional scheme, two unidirectional dry deposition schemes were tested. Comparisons of modeled ammonia concentrations against observations show that all three schemes can reasonably predict observations. For sites with low observed ammonia concentrations, the bidirectional scheme clearly overestimated ammonia concentrations during crop-growing season. Although all three schemes tended to underestimate ammonia concentrations after mid-October and for sites with elevated observed concentrations, mainly due to underestimated NH3 emission inventory after mid-October and/or underestimated emission potentials for those sites, the bidirectional scheme performed better because of its introduction of compensation points into the flux calculation parameterization. In addition to uncertainties in the emission inventory, the results of additional sensitivity tests suggest that uncertainties in the input values of emission potentials in the bidirectional scheme greatly affect the accuracy of modeled ammonia concentrations. The use of much larger emission potentials in the bidirectional scheme and larger anthropogenic NH3 emission after mid-October than provided in the model emissions files is needed for accurate prediction of elevated ammonia concentrations at intensive agricultural locations.

A new chemistry module that simulates atmospheric ammonia (NH3) and ammonium (NH+4) was incorporated into a backward-in-time stochastic Lagrangian air quality model (STILT-Chem) that was originally developed to simulate the concentrations of a variety of gas-phase species at receptors. STILT-Chem simulates the transport of air parcels backward in time using ensembles of fictitious particles with stochastic motions, while accounting for emissions, deposition and chemical transformation forward in time along trajectories identified by the backward-in-time simulations. The incorporation of the new chemistry module allows the model to simulate not only gaseous species, but also multi-phase species involving NH3 and NH+4. The model was applied to simulate concentrations of NH3 and particulate NH+4 at six sites in the Canadian province of Ontario for a six-month period in 2006. The model-predicted concentrations of NH3 and particulate NH+4 were compared with observations, which show broad agreement between simulated concentrations and observations. Since the model is based on back trajectories, the influence of each major process such as emission, deposition and chemical conversion on the concentration of a modeled species at a receptor can be determined for every upstream location at each time step. This makes it possible to quantitatively investigate the upstream processes affecting receptor concentrations. The modeled results suggest that the concentrations of NH3 at those sites were significantly and frequently affected by Ohio, Iowa, Minnesota, Michigan, Wisconsin, southwestern Ontario and nearby areas. NH3 is mainly contributed by emission sources whereas particulate NH+4 is mainly contributed by the gas-to-aerosol chemical conversion of NH3. Dry deposition is the largest removal process for both NH3 and particulate NH+4. This study revealed the contrast between agricultural versus forest sites. Not only were emissions of NH3 higher, but removal mechanisms (especially chemical loss for NH3 and dry deposition for NH+4) were less efficient for agricultural sites. This combination explains the significantly higher concentrations of NH3 and particulate NH+4 observed at agricultural sites.