• Energy Research

SignificanceThe COVID-19 pandemic and associated lockdowns caused significant changes to human activity that temporarily altered our imprint on the atmosphere, providing a brief glimpse of potential future changes in atmospheric composition. This event demonstrated key feedbacks within and between air quality and the carbon cycle: Improvements in air quality increased the lifetime of methane (an important greenhouse gas), while unusually hot weather and intense wildfires in Los Angeles drove poor air quality. This shows that efforts to reduce greenhouse gas emissions and improve air quality cannot be considered separately.

Atmospheric column abundances of carbon dioxide (CO2), carbon monoxide (CO), methane (CH4) and nitrous oxide (N2O) have been measured above the South Coast air basin (SCB), a densely populated urban region of Southern California, USA, which includes Los Angeles and the surrounding suburbs. Large diurnal variations in CO and CH4 are observed which correlate well with those in CO2. Weaker correlations are seen between N2O and CO2, with large uncertainties. We compute yearly SCB emissions of CO and CH4 to be 1.4 ± 0.3 Tg CO and 0.6 ± 0.1 Tg CH4. We compare our calculated emissions to the California Air Resources Board (CARB) and the Emission Database for Global Atmospheric Research (EDGAR) estimates. Our measurements confirm that urban emissions are a significant source of CH4 and in fact may be substantially higher than currently estimated. If our emissions are typical of other urban centers, these findings suggest that urban emissions could contribute 7–15% to the global anthropogenic budget of methane.

These data are now obsolete and should be replaced by the most recent data: https://doi.org/10.22002/D1.306 The EM27/SUN GGG Interferogram processing suite (EGI) is a collection of software tools to simplify processing data collected using EM27/SUN instruments through GGG. Complete processing is simplified down to a one-line command. EM27/SUN instruments are commercial, portable, solar-viewing FT-IR spectrometers (manufactured by Bruker). GGG is open-source software used to FFT the interferograms to spectra, and then fit the spectra to obtain column averaged abundances of CO2, CH4, H2O, and in some cases CO and N2O. GGG is also used for the TCCON (https://tccon-wiki.caltech.edu/).

Abstract Changes in atmospheric CO2 variability during the twenty-first century may provide insight about ecosystem responses to climate change and have implications for the design of carbon monitoring programs. This paper describes changes in the three-dimensional structure of atmospheric CO2 for several representative concentration pathways (RCPs 4.5 and 8.5) using the Community Earth System Model–Biogeochemistry (CESM1-BGC). CO2 simulated for the historical period was first compared to surface, aircraft, and column observations. In a second step, the evolution of spatial and temporal gradients during the twenty-first century was examined. The mean annual cycle in atmospheric CO2 was underestimated for the historical period throughout the Northern Hemisphere, suggesting that the growing season net flux in the Community Land Model (the land component of CESM) was too weak. Consistent with weak summer drawdown in Northern Hemisphere high latitudes, simulated CO2 showed correspondingly weak north–south and vertical gradients during the summer. In the simulations of the twenty-first century, CESM predicted increases in the mean annual cycle of atmospheric CO2 and larger horizontal gradients. Not only did the mean north–south gradient increase due to fossil fuel emissions, but east–west contrasts in CO2 also strengthened because of changing patterns in fossil fuel emissions and terrestrial carbon exchange. In the RCP8.5 simulation, where CO2 increased to 1150 ppm by 2100, the CESM predicted increases in interannual variability in the Northern Hemisphere midlatitudes of up to 60% relative to present variability for time series filtered with a 2–10-yr bandpass. Such an increase in variability may impact detection of changing surface fluxes from atmospheric observations.

Observations of the column‐averaged dry molar mixing ratio of CO2 above both Park Falls, Wisconsin and Kitt Peak, Arizona, together with partial columns derived from aircraft profiles over Eurasia and North America are used to estimate the seasonal integral of net ecosystem exchange (NEE) between the atmosphere and the terrestrial biosphere in the Northern Hemisphere. We find that NEE is ∼25% larger than predicted by the Carnegie Ames Stanford Approach (CASA) model. We show that the estimates of NEE may have been biased low by too weak vertical mixing in the transport models used to infer seasonal changes in Northern Hemisphere CO2 mass from the surface measurements of CO2 mixing ratio.

Abstract. Nitrous oxide (N2O) is both a greenhouse gas in the troposphere and an ozone depleting substance in the stratosphere and is rapidly increasing in the atmosphere. The spatial distribution of N2O emissions and the sources leading to rising concentrations in the global atmosphere are highly uncertain. We measured the global distribution of tropospheric N2O mixing ratios during the airborne Atmospheric Tomography (ATom) mission. ATom measured mixing ratios of ~300 gas species and aerosol properties in 647 vertical profiles spanning the Pacific, Atlantic, Arctic, and much of the Southern Ocean basins, from nearly Pole to Pole, over four seasons (2016–2018). We measured N2O mixing ratios at 1 Hz using a Quantum Cascade Laser Spectrometer and a new spectral retrieval method to account for the pressure and temperature sensitivity of the instrument when deployed on aircraft. This retrieval strategy improved the precision of our N2O measurements by a factor of 3, enabling us to recover the precision to that of previous missions. Most of the variance of N2O mixing ratios in the troposphere is driven by the influence of N2O-depleted stratospheric air, especially at mid and high latitudes. We observe the downward propagation of lower N2O mixing ratios (compared to surface stations) that tracks the influence of stratosphere-troposphere exchange through the tropospheric column down to the surface, resulting in a seasonal minimum at the surface 2–3 months after the peak stratosphere-to-troposphere exchange in spring. The highest N2O mixing ratios occur close to the equator, extending through the boundary layer and free troposphere. We observed influences from a complex and diverse mixture of N2O sources, with emission source types identified using the rich suite of chemical species measured on ATom and with the geographical origin calculated using an atmospheric transport model. Although ATom flights were mostly over the oceans, the most prominent N2O enhancements were associated with anthropogenic emissions, including industry, oil and gas, urban and biomass burning, especially in the tropical Atlantic outflow from Africa. Enhanced N2O mixing ratios are mostly associated with pollution-related tracers arriving from the coastal area of Nigeria. Peaks of N2O are often well-correlated with indicators of photochemical processing, suggesting possible unexpected source processes. The difficulty of separating the mixture of different sources in the atmosphere contributes to uncertainties in the N2O global budget. The extensive data set from ATom will help improve the understanding of N2O emission processes and their representation in global models.