Remote sensing datasets of water vapor isotopic composition are used along with objective measures of convective aggregation to better understand the impact of convective aggregation on the atmospheric hydrologic cycle in the global tropics ($30^{\circ}$N to $30^{\circ}$S) for the period 2015-2020. When convection is unaggregated, vertical velocity profiles are top-heavy, mixing ratios increase and water vapor $\delta D$ decreases as the mean precipitation rate increases, consistent with partial hydrometeor evaporation below anvils into a relatively humid atmospheric column. Aggregated convection is associated with bottom-heavy vertical velocity profiles and a positive correlation between mixing ratio and $\delta D$, a result that is consistent with isotopic enrichment from detrainment of shallow convection near the observation level. Intermediate degrees of aggregation do not display significant variation in $\delta D$ with mixing ratio or precipitation rate. Convective aggregation provides a useful paradigm for understanding the relationships between mixing ratio and isotopic composition across a range of convective settings. The results presented here may have utility for a variety of applications including the interpretation of paleoclimate archives and the evaluation of numerical simulations of convection.

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.

We present a Lagrangian framework for identifying mechanisms that control the isotopic composition of mid-tropospheric water vapor in the Sahel region during the West African Monsoon 2016. In this region mixing between contrasting air masses, strong convective activity, as well as surface and rain evaporation lead to high variability in the distribution of stable water isotopologues. Using backward trajectories based on high-resolution isotope-enabled model data, we obtain information not only about the source regions of Sahelian air masses, but also about the evolution of H2O and its isotopologue HDO (expressed as δD) along the pathways of individual air parcels. We sort the full trajectory ensemble into groups with similar transport pathways and hydro-meteorological properties, such as precipitation and relative humidity, and investigate the evolution of the corresponding paired {H2O, δD} distributions. The use of idealized process curves in the {H2O, δD} phase space allows us to attribute isotopic changes to contributions from (1) air mass mixing, (2) Rayleigh condensation during convection, and (3) microphysical processes depleting the vapor beyond the Rayleigh prediction, i.e., partial rain evaporation in unsaturated and isotopic equilibration δin saturated conditions. Different combinations of these processes along the trajectory ensembles are found to determine the final isotopic composition in the Sahelian troposphere during the monsoon. The presented Lagrangian framework is a powerful tool for interpreting tropospheric water vapor distributions. In the future, it will be applied to satellite observations of H2O, δD} over Africa and other regions in order to better quantify characteristics of the hydrological cycle.