This study presents the Ozone Monitoring Instrument (OMI) Collection 4 formaldehyde (HCHO) retrieval developed with the Smithsonian Astrophysical Observatory’s (SAO) Making Earth System Data Records for Use in Research Environments (MEaSUREs) algorithm. The retrieval algorithm updates and makes improvements to the NASA operational OMI HCHO (OMI Collection 3 HCHO) algorithm, and has been transitioned to use OMI Collection 4 Level-1B radiances. This paper describes the updated retrieval algorithm and compares Collection 3 and Collection 4 data products. The OMI Collection 4 HCHO exhibits remarkably improved stability over time in comparison to the OMI Collection 3 HCHO product, with better precision and the elimination of artificial trends present in the Collection 3 during the later years of the mission. We validate the OMI Collection 4 HCHO data product using Fourier-Transform Infrared (FTIR) ground-based HCHO measurements. The climatological monthly averaged OMI Collection 4 HCHO vertical column densities (VCDs) agree well with the FTIR VCDs, with a correlation coefficient of 0.83, root-mean-square error (RMSE) of 2.98 × 1015 molecules cm-2, regression slope of 0.79, and intercept of 8.21 × 1014 molecules cm-2. Additionally, we compare the monthly averaged OMI Collection 4 HCHO VCDs to OMPS Suomi NPP, OMPS NOAA-20, and TROPOMI HCHO VCDs in overlapping years for twelve geographic regions. This comparison demonstrates high correlation coefficients of 0.98 (OMPS Suomi NPP), 0.97 (OMPS NOAA-20), and 0.90 (TROPOMI).

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.

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.

The Brewer-Dobson Circulation (BDC) determines the distribution of long-lived trac- ers in the stratosphere; therefore, their changes can be used to diagnose changes in the BDC. We evaluate decadal (2005-2018) trends of nitrous oxide (N2O) in two versions of the Whole Atmosphere Chemistry-Climate Model (WACCM) by comparing them with measurements from four Fourier transform infrared (FTIR) ground-based instruments, the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), and with a chemistry-transport model (CTM) driven by four different reanalyses. The limited sensitivity of the FTIR instruments can hide negative N2O trends in the mid-stratosphere because of the large increase in the lowermost stratosphere. When applying ACE-FTS measurement sampling on model datasets, the reanalyses from the European Centre for Medium Range Weather Forecast (ECMWF) compare best with ACE-FTS, but the N2O trends are consistently exaggerated. The N2O trends obtained with WACCM disagree with those obtained from ACE-FTS, but the new WACCM version performs better than the previous above the Southern Hemisphere in the stratosphere. Model sensitivity tests show that the decadal N2O trends reflect changes in the stratospheric transport. We further investigate the N2 O Transformed Eulerian Mean (TEM) budget in WACCM and in the CTM simulation driven by the latest ECMWF reanalysis. The TEM analysis shows that enhanced advection affects the stratospheric N2O trends in the Tropics. While no ideal observational dataset currently exists, this model study of N2O trends still provides new insights about the BDC and its changes because of the contribution from relevant sensitivity tests and the TEM analysis.