Top-down estimates of CO2 fluxes are typically constrained by either surface-based or space-based CO2 observations. Both of these measurement types have spatial and temporal gaps in observational coverage that can lead to biases in inferred fluxes. Assimilating both surface-based and space-based measurements concurrently in a flux inversion framework improves observational coverage and reduces sampling biases. This study examines the consistency of flux constraints provided by these different observations and the potential to combine them by performing a series of six-year (2010–2015) CO2 flux inversions. Flux inversions are performed assimilating surface-based measurements from the in situ and flask network, measurements from the Total Carbon Column Observing Network (TCCON), and space-based measurements from the Greenhouse Gases Observing Satellite (GOSAT), or all three datasets combined. Combining the datasets results in more precise flux estimates for sub-continental regions relative to any of the datasets alone. Combining the datasets also improves the accuracy of the posterior fluxes, based on reduced root-mean-square differences between posterior-flux-simulated CO2 and aircraft-based CO2 over midlatitude regions (0.35–0.50~ppm) in comparison to GOSAT (0.39–0.57~ppm), TCCON (0.52–0.63~ppm), or in situ and flask measurements (0.45–0.53~ppm) alone. These results suggest that surface-based and GOSAT measurements give complementary constraints on CO2 fluxes in the northern extratropics and can be combined in flux inversions to improve observational coverage. This stands in contrast with many earlier attempts to combine these datasets and suggests that improvements in the NASA Atmospheric CO2 Observations from Space (ACOS) retrieval algorithm have significantly improved the consistency of space-based and surface-based flux constraints.

In the winter and spring of 2019/2020, the unusually cold, strong, and stable polar vortex created favorable conditions for ozone depletion in the Arctic. Chemical ozone loss started earlier than in any previous year in the satellite era, and continued until the end of March, resulting in the unprecedented reduction of the ozone column. The vortex was located above the Polar Environment Atmospheric Research Laboratory in Eureka, Canada (80 °N, 86 °W) from late February to the end of April, presenting an excellent opportunity to examine ozone loss from a single ground station. Measurements from a suite of instruments show that total column ozone in 2020 was at an all-time low in the 20-year dataset, 22 to 102 DU below previous records set in 2011. Ozone minima (<200 DU), enhanced OClO and BrO slant columns, and unusually low HCl, ClONO2 , and HNO3 columns were observed in March. Polar stratospheric clouds were present as late as 20 March, and ozonesondes show unprecedented depletion in the March and April ozone profiles (to <0.2 ppmv). While both chemical and dynamical factors lead to reduced ozone when the vortex is cold, the contribution of chemical depletion was exceptional in spring 2020 when compared to typical Arctic winters. The mean chemical ozone loss over Eureka was estimated to be 111-127 DU (27-31%) using April measurements and passive ozone from the SLIMCAT chemical transport model. While absolute ozone loss was generally smaller in 2020 than in 2011, percentage ozone loss was greater in 2020.

Throughout spring and summer 2020, ozone stations in the northern extratropics recorded unusually low ozone in the free troposphere. From April to August, and from 1 to 8 kilometers altitude, ozone was on average 7% (~4 ppbv) below the 2000 to 2020 climatological mean. Such low ozone, over several months, and at so many stations, has not been observed in any previous year since at least 2000. Atmospheric composition re-analyses from the Copernicus Atmosphere Monitoring Service and simulations from the NASA GMI model indicate that the large 2020 springtime ozone depletion in the Arctic stratosphere has contributed less than one quarter to the observed tropospheric anomaly. The observed anomaly is consistent with two recent model simulations, which assume emission reductions similar to those caused by the COVID-19 crisis. COVID-19 related emission reductions appear to be the major cause for the observed low free tropospheric ozone in 2020.

During the global COVID-19 pandemic, anthropogenic emissions of air pollutants and greenhouse gases, especially traffic emissions in urban areas, have declined significantly. Long-term measurements of trace gas concentrations in urban areas can be used to quantify the impact of emission reductions on local air quality. Open-path Fourier transform infrared (OP-FTIR) spectroscopy is a non-intrusive technique that can be used to simultaneously measure multiple atmospheric trace gases in the boundary layer. This study investigates the reduction of surface CO, CO2 , and CH4 mole fractions during the lockdown in downtown Toronto, Canada, which is the fourth largest city in North America. The mean daily CO mole fraction anomaly (ΔCO) for the period from March 14 to May 18, 2020 declined by 46 ± 16% compared to the period before lockdown from January 13 to March 13, 2020. The mean daily ΔCO during the lockdown also declined relative to the same period in previous years: by 50 ± 20% relative to 2019 and by 44 ± 25% relative to 2018. Changes in the diurnal variations of CO, CO2 and CH4 during the lockdown are also investigated and compared to 2019 and 2018. Both CO and CO2 show early morning maxima on weekdays corresponding to rush hour. The change of the amplitude of the diurnal variation in CO during the lockdown is significant, compared to the period before lockdown. The differences in the diurnal variation in CO during the same two periods in 2019 and 2018 are not significant. Ratios of CO/CO2 anomalies show seasonal variations, which are also likely due to seasonal changes of emissions from local sources. These results show that the COVID-19 lockdown in Toronto modified surface mole fractions, diurnal variations, and ratios of air pollutants monitored by OP-FTIR. In addition, measured CO mole fractions are compared with simulated CO mole fractions by WRF-STILT to assess the relationship between atmospheric measurements and urban emissions from Toronto.

Carbonyl sulfide (OCS) is a non-hygroscopic trace species in the free troposphere and the primary sulfur reservoir maintained by direct oceanic, geologic, biogenic and anthropogenic emissions and the oxidation of other sulfur-containing source species. It’s the largest source of sulfur transported to the stratosphere during volcanically quiescent periods. Data from 22 ground-based globally dispersed stations are used to derive trends in total and partial column OCS. Middle infrared spectral data are recorded by solar-viewing Fourier transform interferometers that are operated as part of the Network for the Detection of Atmospheric Composition Change between 1986 and 2020. Vertical information in the retrieved profiles provides analysis of discreet altitudinal regions. Trends are found to have well-defined inflection points. In two linear trend time periods ~2002 - 2008 and ~2008 - 2016, tropospheric trends range from ~0.0 to (1.55 ± 0.30 %/y) in contrast to the prior period where all tropospheric trends are negative. Regression analyses show strongest correlation in the free troposphere with anthropogenic emissions. Stratospheric trends in the period ~2008 - 2016 are positive up to (1.93 ± 0.26 %/y) except notably low latitude stations that have negative stratospheric trends. Since ~2016, all stations show a free tropospheric decrease to 2020. Stratospheric OCS is regressed with simultaneously measured N$_2$O to derive a trend accounting for dynamical variability. Stratospheric lifetimes are derived and range from (54.1 ± 9.7)y in the sub-tropics to (103.4 ± 18.3)y in Antarctica. These unique long-term measurements provide new and critical constraints on the global OCS budget.

Experimental measurements of collision-induced absorption (CIA) cross-sections for CO2-H2 and CO2-CH4 complexes were performed using Fourier transform spectroscopy over a spectral range of 100-500 cm and a temperature range of 200-300 K. These experimentally derived CIA cross-sections agree with the spectral range and temperature dependence of the calculation by \citeA{Robin}, however the amplitude is half of what was predicted. Furthermore, the CIA cross-sections reported here agree with those measured by \citeA{Turbet}. The CIA cross-sections can be applied to planetary systems with CO$_{2}$-rich atmospheres, such as Mars and Venus, and will be useful to terrestrial spectroscopists. Additionally, radiative transfer calculations of the early Mars atmosphere were performed and showed that CO2$-CH4 CIA would require surface pressure greater than 3 bar for a 10% methane atmosphere to achieve 273 K at the surface. CO2-H2, however, liquid water is possible with 5% hydrogen and less than 2 bar of surface pressure.

Experimental measurements of collision-induced absorption (CIA) cross-sections for CO-H2 and CO2-CH4 complexes were performed using Fourier transform spectroscopy over a spectral range of 100-500 cm and a temperature range of 200-300 K. These experimentally derived CIA cross-sections agree with the spectral range and temperature dependence of the calculation by Wordsworth (2017), however the amplitude is half of what was predicted. Furthermore, the CIA cross-sections reported here agree with those measured by Turbet (2019). The CIA cross-sections can be applied to planetary systems with CO2-rich atmospheres, such as Mars and Venus, and will be useful to terrestrial spectroscopists. Additionally, radiative transfer calculations of the early Mars atmosphere were performed and showed that CO2-CH4 CIA would require surface pressure greater than 3 bar for a 10% methane atmosphere to achieve 273 K at the surface. CO2-H2, however, liquid water is possible with 5\% hydrogen and less than 2 bar of surface pressure.

In this study, we examine the ability of the data assimilation of global satellite-based carbon monoxide (CO) observations to constrain high-latitude boreal wildfire emissions. We compare the optimized emissions from inversions using CO measurements from the Measurement of Pollution in the Troposphere (MOPITT) and Infrared Atmospheric Sounding Interferometer (IASI). We found that both inversions yield generally consistent posterior CO emissions globally; however, distinct differences are observed for the episodic 2017 Canadian wildfires. The 3-day global coverage of MOPITT limits its ability to accurately optimize emissions, while the daily global coverage of IASI provides a moderate improvement despite its lower surface sensitivity. Through a series of observing system simulation experiments (OSSEs), we show that the temporal coverage of IASI most strongly influenced the posterior estimates, while the differences in vertical sensitivities of MOPITT and IASI have a minor contribution.

An unanswered question in planetary science is how could the early Martian atmosphere have maintained a greenhouse effect sufficient to allow for liquid water on the surface? A recent study by Wordsworth et al. (DOI:10.1002/2016GL071766) suggested that previously unaccounted-for collision-induced absorption (CIA) by carbon dioxide (CO2) and hydrogen gas (H2), and by CO2 and methane (CH4) could provide the additional atmospheric absorption needed to trap enough radiation to raise the Martian surface temperature above freezing. However, as CIA cross-sections for CO2-H2 and CO2-CH4 complexes do not exist in the literature, the authors could only use computational methods to simulate the CIA absorption cross-sections that they themselves identify in the study as needing experimental validation. Preliminary results will be presented from experimental measurements of the CIA cross-sections for CO2-H2 and CO2-CH4 complexes performed using Fourier Transform Spectroscopy. We have obtained Beam-time at the Canadian Light Source Far-IR beamline in late October and early November which will allow us to derive Cross-sections over a spectral range of 0-3000 cm-1 and a temperature range of 200-350 K. In addition to allowing us to experimentally validate the hypothesis of Wordsworth, the cross-sections so obtained can also be applied to other planetary systems with CO2-rich atmospheres, such as Venus, and will be useful to terrestrial spectroscopists.