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Susan Strahan

Publications and source records attributed to Susan Strahan.

Optimized Umkehr Profile Algorithm for Ozone Trend Analyses

The long-term record of Umkehr measurements from four NOAA Dobson spectrophotometers was reprocessed after updates to the instrument calibration procedures. In addition, a new data quality-control tool was developed for the Dobson automation software (WinDobson). This paper presents a comparison of Dobson Umkehr ozone profiles from NOAA ozone network stations (Boulder, OHP, MLO, Lauder) against several satellite records, including Aura Microwave Limb Sounder (MLS; ver. 4.2), and combined SBUV and OMPS records (NASA AGG and NOAA COH). A subset of satellite data is selected to match Dobson Umkehr observations at each station spatially (distance less than 200 km) and temporally (within 24 hours). Umkehr Averaging Kernels (AKs) are applied to vertically smooth all overpass satellite profiles prior to comparisons. The station Umkehr record consists of several instrumental records, which have different optical characterizations, and thus instrument-specific stray light contributes to the data processing errors and creates step changes in the record. This work evaluates the overall quality of Umkehr long-term measurements at NOAA ground-based stations and assesses the impact of the instrumental changes on the stability of the Umkehr ozone profile record. This paper describes a method designed to correct biases and discontinuities in the retrieved Umkehr profile that originate from the Dobson calibration process, repair, or optical realignment of the instrument. The M2GMI and GMI CTM ozone profile model output matched to station location and date of observation is used to evaluate instrumental step changes in the Umkehr record. Homogenization of the Umkehr record and discussion of the apparent stray light error in retrieved ozone profiles are the focus of this paper. Homogenization of ground-based records is of great importance for studies of long-term ozone trends and climate change.

Umkehr

Tropospheric Age-of-Air: Influence of SF6 Emissions on Recent Surface Trends and Model Biases

The mean age since air was last at the Northern Hemisphere (NH) midlatitude surface is a fundamental property of tropospheric transport. Here we approximate the mean age in terms of an "SF6 age" (ΓSF6), derived from surface and aircraft measurements of SF6 that are broader in spatial scope and cover a longer time period (1997-2018) than considered previously. At the surface, ΓSF6 increases from near-zero values north of 30°N to ~1.5 years over the Southern Hemisphere (SH) extratropics, with the largest meridional gradients occurring in the tropics. By comparison, vertical gradients in ΓSF6 are weak throughout, with only slight increases/decreases with height in the NH/SH. The broader spatial coverage of the measurements reveals strong variations in the seasonal cycle of ΓSF6 within the (sub)tropics that are weaker over the Atlantic and Paci c oceans, compared to over the Indian Ocean. Observations from 2000-2018 reveal that the SF6 age at sites in the SH has been decreasing by ~0.12 yr/dec. However, this decrease is not due to changes in transport but, rather, is likely related to changes in emissions, which have increased globally and reportedly shifted from northern midlatitudes into the subtropics. Simulations, which reproduce the SF6 age trends, show no decreases in an age-of-air tracer, reinforcing the fact that ΓSF6 represents only an approximation to the mean age. Finally, the modeled SF6 ages are older than observed, by ~0.3-0.4 years throughout the southern extratropics. We show that this bias is partly related to an overestimation in simulated SF6 near emissions regions,

Mean age

COVID-19 Crisis Reduces Free Tropospheric Ozone Across the Northern Hemisphere

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 nmol/mol) below the 2000–2020 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 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 contributed less than one-quarter of the observed tropospheric anomaly. The observed anomaly is consistent with recent chemistry-climate model simulations, which assume emissions reductions similar to those caused by the COVID-19 crisis. COVID-19 related emissions reductions appear to be the major cause for the observed reduced free tropospheric ozone in 2020.

COVID-19

Validation of SAGE III/ISS Solar Ozone Data with Correlative Satellite and Ground Based Measurements

The Stratospheric Aerosol and Gas Experiment III on the International Space Station (SAGE III/ISS) was launched on February 19, 2017 and began routine operation in June 2017. The first two years of SAGE III/ISS (v5.1) solar ozone data were evaluated by using correlative satellite and ground-based measurements. Among the three (MES, AO3, and MLR) SAGE III/ISS solar ozone products, AO3 ozone shows the best accuracy and precision, with mean biases less than 5% for altitudes ~15–55 km in the mid-latitudes and ~20–55 km in the tropics. In the lower stratosphere and upper troposphere, AO3 ozone shows high biases that increase with decreasing altitudes and reach ~10% near the tropopause. Preliminary studies indicate that those high biases primarily result from the contributions of the oxygen dimer (O4) not being appropriately removed within the ozone channel. The precision of AO3 ozone is estimated to be ~3% for altitudes between 20 and 40 km. It degrades to ~10–15% in the lower mesosphere (~55 km), and ~20–30% near the tropopause. There could be an altitude registration error of ~100 meter in the SAGE III/ISS auxiliary temperature and pressure profiles. This, however, does not affect retrieved ozone profiles in native number density on geometric altitude coordinates. In the upper stratosphere and lower mesosphere (~40–55 km) the SAGE III/ISS (and SAGE II) sunset ozone values are systematically higher than sunrise data by ~5–8% which are almost twice larger than what observed by other satellites or model predictions. This feature needs further study.

H J Wang

A Machine Learning Examination of Hydroxyl Radical Differences Among Model Simulations for CCMI-1

Hydroxyl radical (OH) plays critical roles within the troposphere, such as determining the lifetime of methane (CH4), yet is challenging to model due to its fast cycling and dependence on a multitude of sources and sinks. As a result, the reasons for variations in OH and the resulting CH4 lifetime (TCH4), both between models and in time, are difficult to diagnose. We apply a neural network (NN) approach to address this issue within a group of models that participated in the Chemistry-Climate Model Initiative (CCMI). Analysis of the historical specified dynamics simulations performed for CCMI indicates that the primary drivers of TCH4 differences among ten models are the flux of UV light to the troposphere (indicated by the photolysis frequency JO1D) due mostly to clouds, mixing ratio of tropospheric ozone (O3), the abundance of nitrogen oxides (NOx≡NO+NO2), and details of the various chemical mechanisms that drive OH. Water vapor, carbon monoxide (CO), the ratio of NO:NOx, and formaldehyde (HCHO) explain moderate differences in TCH4, while isoprene, CH4, the photolysis frequency of NO2 by visible light (JNO2), overhead O3 column, and temperature account for little-to-no model variation in CH4. We also apply the NNs to analysis of temporal trends in OH from 1980 to 2015. All models that participated in the specified dynamics historical simulation for CCMI demonstrate a decline in CH4 during the analysed timeframe. The significant contributors to this trend, in order of importance, are tropospheric O3, JO1D, NOx, and H2O, with CO also causing substantial interannual variability in OH burden. Finally, the identified trends in TCH4 are compared to calculated trends in the tropospheric mean OH concentration from previous work, based on analysis of observations. The comparison reveals a robust result for the effect of rising water vapor on OH and CH4, imparting an increasing and decreasing trend of about 0.5% decade(exp -1), respectively. The responses due to NOx, O3 column, and temperature are also in reasonably good agreement between the two studies, though a discrepancy in the CH4 response highlights a need for further examination of the CH4 feedback on the abundance of OH.

Julie M Nicely

Faster Tropical Upper Stratospheric Upwelling is Driving Changes in Ozone Chemistry

Trends in N2O and the chlorofluorocarbons (CFCs) cause trends in O3 through changes in their reactive product gases, NOx and ClOx, but transport plays an important role because it controls the distribution of the long‐lived source gases that produce ozone‐destroying radicals. In this study we show that increased tropical upwelling 10‐5 hPa from 2013‐2021 has changed upper stratospheric (UpS) composition and shifted the balance of O3 loss processes. We use N2O, HNO3, NOx, temperature and O3 data from the Aura Microwave Limb Sounder (MLS) and the SCI‐Sat Atmospheric Chemistry Experiment Fourier Transport Spectrometer (ACE‐FTS) over a 16‐year period to show how changes in reactive nitrogen species affected gas phase ozone chemistry above 30 hPa between June 2013‐May 2021 compared to the previous 8 years, June 2005‐May 2013. We use 2 simulations of the Global Modeling Initiative (GMI) chemistry transport model (CTM), with and without time varying MERRA2 meteorology, to understand how dynamical changes during this 16‐yr period affected O3 through changes in loss via the NOx and ClOx cycles. We also identify the role that the quasi‐biennial oscillation (QBO) in tropical zonal winds plays in the UpS composition changes. We find large increases in tropical upwelling and poleward transport in the northern branch of the UpS transport circulation since 2013 that dramatically increased the abundance of the N2O and its odd nitrogen product gases, NOx and HNO3. O3 loss by NOx in the Arctic UpS increased due to dynamically driven composition change, explaining the observed weak O3 recovery in that region since 2005. The increased upwelling also drove decreases in tropical NOx, leading to increased tropical O3 from 12‐6 hPa.

middle atmosphere chemistry and composition