James W Hannigan

and 33 more

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.

Daniele Minganti

and 11 more

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.
Australian fires are a primary driver of variability in Australian atmospheric composition and contribute significantly to regional and global carbon budgets. However, biomass burning emissions from Australia remain highly uncertain. In this work, we use surface in situ, ground-based total column and satellite total column observations to evaluate the ability of two global models (GEOS-Chem and ACCESS-UKCA) and three global biomass burning emission inventories (FINN1.5, GFED4s, and QFED2.4) to simulate carbon monoxide (CO) in the Australian atmosphere. We find that emissions from northern Australia savanna fires are substantially lower in FINN1.5 than in the other inventories. Model simulations driven by FINN1.5 are unable to reproduce either the magnitude or the variability of observed CO in northern Australia. The remaining two inventories perform similarly in reproducing the observed variability, although the larger emissions in QFED2.4 combined with an existing high bias in the southern hemisphere background lead to large CO biases. We therefore recommend GFED4s as the best option of the three for global modelling studies with focus on Australia or the southern hemisphere. Near fresh fire emissions, the higher resolution ACCESS-UKCA model is better able to simulate surface CO than GEOS-Chem, while GEOS-Chem captures more of the observed variability in the total column and remote surface air measurements. We also show that existing observations in Australia can only partially constrain global model estimates of biomass burning. Continuous measurements in fire-prone parts of Australia are needed, along with updates to global biomass burning inventories that are validated with Australian data.