Carbonyl sulfide (OCS) is a non-hygroscopic trace species in the free troposphere and a large sulfur reservoir maintained by both direct oceanic, geologic, biogenic, and anthropogenic emissions and the oxidation of other sulfur-containing source species. It is 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 to 2008 and ∼2008 to 2016 tropospheric trends range from ∼0.0 to (1.55 ± 0.30%/yr) 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 to 2016 are positive up to (1.93 ± 0.26%/yr) 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)yr in the sub-tropics to (103.4 ± 18.3)yr in Antarctica. These unique long-term measurements provide new and critical constraints on the global OCS budget.Plain Language Summary Carbonyl sulfide (OCS) is the most abundant sulfur containing gas in the atmosphere. There are many sources and sinks of OCS and other sulfur species in the atmosphere but most other short lived sulfur species eventually are converted to OCS. It is important to quantify and understand OCS as it can be used to understand CO 2 and the carbon cycle and also since it eventually is transported into the stratosphere where it maintains the sulfate aerosol layer at about 20 km into the atmosphere. This layer is very important for earth's energy balance and climate change. In contrast with earlier and less comprehensive reports, this global study from 22 observation stations worldwide, shows stratospheric OCS to be increasing HANNIGAN ET AL.

Abstract. Understanding variations in atmospheric ozone in the Arctic is difficult because there are only a few long-term records of vertical ozone profiles in this region. We present 12 years of ozone profiles from February 2005 to February 2017 at four sites: Summit Station, Greenland; Ny-Ålesund, Svalbard, Norway; and Alert and Eureka, Nunavut, Canada. These profiles are created by combining ozonesonde measurements with ozone profile retrievals using data from the Microwave Limb Sounder (MLS). This combination creates a high-quality dataset with low uncertainty values by relying on in situ measurements of the maximum altitude of the ozonesondes (∼30 km) and satellite retrievals in the upper atmosphere (up to 60 km). For each station, the total column ozone (TCO) and the partial column ozone (PCO) in four atmospheric layers (troposphere to upper stratosphere) are analyzed. Overall, the seasonal cycles are similar at these sites. However, the TCO over Ny-Ålesund starts to decline 2 months later than at the other sites. In summer, the PCO in the upper stratosphere over Summit Station is slightly higher than at the other sites and exhibits a higher standard deviation. The decrease in PCO in the middle and upper stratosphere during fall is also lower over Summit Station. The maximum value of the lower- and middle-stratospheric PCO is reached earlier in the year over Eureka. Trend analysis over the 12-year period shows significant trends in most of the layers over Summit and Ny-Ålesund during summer and fall. To understand deseasonalized ozone variations, we identify the most important dynamical drivers of Arctic ozone at each level. These drivers are chosen based on mutual selected proxies at the four sites using stepwise multiple regression (SMR) analysis of various dynamical parameters with deseasonalized data. The final regression model is able to explain more than 80 % of the TCO and more than 70 % of the PCO in almost all of the layers. The regression model provides the greatest explanatory value in the middle stratosphere. The important proxies of the deseasonalized ozone time series at the four sites are tropopause pressure (TP) and equivalent latitude (EQL) at 370 K in the troposphere, the quasi-biennial oscillation (QBO) in the troposphere and lower stratosphere, the equivalent latitude at 550 K in the middle and upper stratosphere, and the eddy heat flux (EHF) and volume of polar stratospheric clouds throughout the stratosphere.

Abstract. Stratospheric circulation is a critical part of the Arctic ozone cycle. Sudden stratospheric warming events (SSWs) manifest the strongest alteration of stratospheric dynamics. During SSWs, changes in planetary wave propagation vigorously influence zonal mean zonal wind, temperature, and tracer concentrations in the stratosphere over the high latitudes. In this study, we examine six persistent major SSWs from 2004 to 2020 using the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2). Using the unique density of observations around the Greenland sector at high latitudes, we perform comprehensive comparisons of high-latitude observations with the MERRA-2 ozone dataset during the six major SSWs. Our results show that MERRA-2 captures the high variability of mid-stratospheric ozone fluctuations during SSWs over high latitudes. However, larger uncertainties are observed in the lower stratosphere and troposphere. The zonally averaged stratospheric ozone shows a dramatic increase of 9 %–29 % in total column ozone (TCO) near the time of each SSW, which lasts up to 2 months. This study shows that the average shape of the Arctic polar vortex before SSWs influences the geographical extent, timing, and magnitude of ozone changes. The SSWs exhibit a more significant impact on ozone over high northern latitudes when the average polar vortex is mostly elongated as seen in 2009 and 2018 compared to the events in which the polar vortex is displaced towards Europe. Strong correlation (R2=90  %) is observed between the magnitude of change in average equivalent potential vorticity before and after SSWs and the associated averaged total column ozone changes over high latitudes. This paper investigates the different terms of the ozone continuity equation using MERRA-2 circulation, which emphasizes the key role of vertical advection in mid-stratospheric ozone during the SSWs and the magnified vertical advection in elongated vortex shape as seen in 2009 and 2018.

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