Human activity has increased the concentration of the earth's atmospheric carbon dioxide, which plays a direct role in contributing to global warming. Mid-tropospheric CO₂ retrieved by the Atmospheric Infrared Sounder shows a substantial spatiotemporal variability that is supported by in situ aircraft measurements. The distribution of middle tropospheric CO₂ is strongly influenced by surface sources and large-scale circulations such as the mid-latitude jet streams and by synoptic weather systems, most notably in the summer hemisphere. In addition, the effects of stratosphere-troposphere exchange are observed during a final stratospheric warming event. The results provide the means to understand the sources and sinks and the lifting of CO₂ from surface layers into the free troposphere and its subsequent transport around the globe. These processes are not adequately represented in three chemistry-transport models that have been used to study carbon budgets.

Quantifying the carbonyl sulfide (OCS) land/ocean fluxes contributes to the understanding of both the sulfur and carbon cycles. The primary sources and sinks of OCS are very likely in a steady state because there is no significant observed trend or interannual variability in atmospheric OCS measurements. However, the magnitude and spatial distribution of the dominant ocean source are highly uncertain due to the lack of observations. In particular, estimates of the oceanic fluxes range from approximately 280 Gg S yr-1 to greater than 800 Gg S yr-1, with the larger flux needed to balance a similarly sized terrestrial sink that is inferred from NOAA continental sites. Here we estimate summer tropical oceanic fluxes of OCS in 2006 using a linear flux inversion algorithm and new OCS data acquired by the Aura Tropospheric Emissions Spectrometer (TES). Modeled OCS concentrations based on these updated fluxes are consistent with HIAPER Pole-to-Pole Observations during 4th airborne campaign and improve significantly over the a priori model concentrations. The TES tropical ocean estimate of 70±16GgS in June,when extrapolated over the whole year (about 840 ± 192 Gg S yr-1), supports the hypothesis proposed by Berry et al. (2013) that the ocean flux is in the higher range of approximately 800 Gg S yr-1.

Megacities are major sources of anthropogenic fossil fuel CO2 (FFCO2) emissions. The spatial extents of these large urban systems cover areas of 10 000 km2 or more with complex topography and changing landscapes. We present a high-resolution land-atmosphere modelling system for urban CO2 emissions over the Los Angeles (LA) megacity area. The Weather Research and Forecasting (WRF)-Chem model was coupled to a very high-resolution FFCO2 emission product, Hestia-LA, to simulate atmospheric CO2 concentrations across the LA megacity at spatial resolutions as fine as ∼ 1 km. We evaluated multiple WRF configurations, selecting one that minimized errors in wind speed, wind direction, and boundary layer height as evaluated by its performance against meteorological data collected during the CalNex-LA campaign (May-June 2010). Our results show no significant difference between moderate-resolution (4 km) and high-resolution (1.3 km) simulations when evaluated against surface meteorological data, but the high-resolution configurations better resolved planetary boundary layer heights and vertical gradients in the horizontal mean winds. We coupled our WRF configuration with the Vulcan 2.2 (10 km resolution) and Hestia-LA (1.3 km resolution) fossil fuel CO2 emission products to evaluate the impact of the spatial resolution of the CO2 emission products and the meteorological transport model on the representation of spatiotemporal variability in simulated atmospheric CO2 concentrations. We find that high spatial resolution in the fossil fuel CO2 emissions is more important than in the atmospheric model to capture CO2 concentration variability across the LA megacity. Finally, we present a novel approach that employs simultaneous correlations of the simulated atmospheric CO2 fields to qualitatively evaluate the greenhouse gas measurement network over the LA megacity. Spatial correlations in the atmospheric CO2 fields reflect the coverage of individual measurement sites when a statistically significant number of sites observe emissions from a specific source or location. We conclude that elevated atmospheric CO2 concentrations over the LA megacity are composed of multiple fine-scale plumes rather than a single homogenous urban dome. Furthermore, we conclude that FFCO2 emissions monitoring in the LA megacity requires FFCO2 emissions modelling with ∼ 1 km resolution because coarser-resolution emissions modelling tends to overestimate the observational constraints on the emissions estimates.

The COVID-19 global pandemic and associated government lockdowns dramatically altered human activity, providing a window into how changes in individual behavior, enacted en masse, impact atmospheric composition. The resulting reductions in anthropogenic activity represent an unprecedented event that yields a glimpse into a future where emissions to the atmosphere are reduced. Furthermore, the abrupt reduction in emissions during the lockdown periods led to clearly observable changes in atmospheric composition, which provide direct insight into feedbacks between the Earth system and human activity. While air pollutants and greenhouse gases share many common anthropogenic sources, there is a sharp difference in the response of their atmospheric concentrations to COVID-19 emissions changes, due in large part to their different lifetimes. Here, we discuss several key takeaways from modeling and observational studies. First, despite dramatic declines in mobility and associated vehicular emissions, the atmospheric growth rates of greenhouse gases were not slowed, in part due to decreased ocean uptake of CO₂ and a likely increase in CH₄ lifetime from reduced NO _x emissions. Second, the response of O₃ to decreased NO _x emissions showed significant spatial and temporal variability, due to differing chemical regimes around the world. Finally, the overall response of atmospheric composition to emissions changes is heavily modulated by factors including carbon-cycle feedbacks to CH₄ and CO₂, background pollutant levels, the timing and location of emissions changes, and climate feedbacks on air quality, such as wildfires and the ozone climate penalty.

Recent measurements of methane (CH₄) by the Mars Science Laboratory (MSL) now confront us with robust data that demand interpretation. Thus far, the MSL data have revealed a baseline level of CH₄ (∼0.4 parts per billion by volume [ppbv]), with seasonal variations, as well as greatly enhanced spikes of CH₄ with peak abundances of ∼7 ppbv. What do these CH₄ revelations with drastically different abundances and temporal signatures represent in terms of interior geochemical processes, or is martian CH₄ a biosignature? Discerning how CH₄ generation occurs on Mars may shed light on the potential habitability of Mars. There is no evidence of life on the surface of Mars today, but microbes might reside beneath the surface. In this case, the carbon flux represented by CH₄ would serve as a link between a putative subterranean biosphere on Mars and what we can measure above the surface. Alternatively, CH₄ records modern geochemical activity. Here we ask the fundamental question: how active is Mars, geochemically and/or biologically? In this article, we examine geological, geochemical, and biogeochemical processes related to our overarching question. The martian atmosphere and surface are an overwhelmingly oxidizing environment, and life requires pairing of electron donors and electron acceptors, that is, redox gradients, as an essential source of energy. Therefore, a fundamental and critical question regarding the possibility of life on Mars is, "Where can we find redox gradients as energy sources for life on Mars?" Hence, regardless of the pathway that generates CH₄ on Mars, the presence of CH₄, a reduced species in an oxidant-rich environment, suggests the possibility of redox gradients supporting life and habitability on Mars. Recent missions such as ExoMars Trace Gas Orbiter may provide mapping of the global distribution of CH₄. To discriminate between abiotic and biotic sources of CH₄ on Mars, future studies should use a series of diagnostic geochemical analyses, preferably performed below the ground or at the ground/atmosphere interface, including measurements of CH₄ isotopes, methane/ethane ratios, H₂ gas concentration, and species such as acetic acid. Advances in the fields of Mars exploration and instrumentation will be driven, augmented, and supported by an improved understanding of atmospheric chemistry and dynamics, deep subsurface biogeochemistry, astrobiology, planetary geology, and geophysics. Future Mars exploration programs will have to expand the integration of complementary areas of expertise to generate synergistic and innovative ideas to realize breakthroughs in advancing our understanding of the potential of life and habitable conditions having existed on Mars. In this spirit, we conducted a set of interdisciplinary workshops. From this series has emerged a vision of technological, theoretical, and methodological innovations to explore the martian subsurface and to enhance spatial tracking of key volatiles, such as CH₄.