Using machine learning to construct TOMCAT model and occultation measurement-based stratospheric methane (TCOM-CH4) and nitrous oxide (TCOM-N2O) profile data sets

oai:publications.copernicus.org:essd109417Monitoring the atmospheric concentrations of greenhouse gases (GHGs) is crucial to improve our understanding of their climate impact. However, there are no long-term profile data sets of important GHGs that can be used to gain a better insight into the processes controlling their variations in the atmosphere. In this study, we apply corrections to chemical transport model (CTM) output based on profile measurements from two solar occultation instruments: the HALogen Occultation Experiment (HALOE) and the Atmospheric Chemistry Experiment – Fourier Transform Spectrometer (ACE-FTS). The goal is to construct long-term (1991–2021), gap-free stratospheric profile data sets, hereafter referred to as TCOM, for two important GHGs. To estimate the corrections that need to be applied to the CTM profiles, we use the extreme gradient boosting (XGBoost) regression model. For methane (TCOM-CH4), we utilize both HALOE and ACE satellite profile measurements from 1992 to 2018 to train the XGBoost model, while profiles from 2019 to 2021 serve as an independent evaluation data set. As there are no nitrous oxide (N2O) profile measurements for earlier years, we derive XGBoost-derived correction terms to construct TCOM-N2O profiles using only ACE-FTS profiles from the 2004–2018 time period, with profiles from 2019–2021 used for the independent evaluation. Overall, both TCOM-CH4 and TCOM-N2O profiles exhibit excellent agreement with the available satellite-measurement-based data sets. We find that compared to evaluation profiles, biases in TCOM-CH4 and TCOM-N2O are generally less than 10 % and 50 %, respectively, throughout the stratosphere. The daily zonal mean profile data sets, covering altitude (15–60 km) and pressure (300–0.1 hPa) levels, are publicly available via the following links: https://doi.org/10.5281/zenodo.7293740 for TCOM-CH4 (Dhomse, 2022a) and https://doi.org/10.5281/zenodo.7386001 for TCOM-N2O (Dhomse, 2022b).</p

Three-dimensional modelling of trace species in the Arctic lower stratosphere

A three-dimensional radiative-dynamical-chemical model has been developed and used to study some aspects of modeling the polar lower stratosphere. The model includes a comprehensive gas-phase chemistry scheme as well as a treatment of heterogeneous reactions occurring on the surface of polar stratospheric clouds. Tracer transport is treated by an accurate, nondispersive scheme with little diffusion suited to the representation of strong gradients. Results from a model simulation of early February 1990 are presented and used to illustrate the importance of the model transport scheme. The model simulation is also used to examine the potential for Arctic ozone destruction and the relative contributions of the chemical cycles responsible

On the regional and seasonal ozone depletion potential of chlorinated very short-lived substances

Chloroform (CHCl3), dichloromethane (CH2Cl2), perchloroethylene (C2Cl4) and 1,2-dichloroethane (C2H4Cl2) are chlorinated Very Short-Lived Substances (Cl-VSLS) with a range of commercial/industrial applications. Recent studies highlight the increasing influence of Cl-VSLS on the stratospheric chlorine budget and therefore their possible role in ozone depletion. Here, we evaluate the ozone depletion potential (ODP) of these Cl-VSLS using a three-dimensional chemical transport model and investigate sensitivity to emission location/season. The seasonal dependence of the ODPs is small but ODPs vary by a factor of 2-3 depending on the continent of emission: 0.0143-0.0264 (CHCl3), 0.0097-0.0208 (CH2Cl2), 0.0057-0.0198 (C2Cl4) and 0.0029-0.0119 (C2H4Cl2). Asian emissions produce the largest ODPs owing to proximity to the tropics and efficient troposphere-to-stratosphere transport of air originating from industrialised East Asia. The Cl-VSLS ODPs are generally small but the upper ends of the CHCl3 and CH2Cl2 ranges are comparable to the mean ODP of methyl chloride (0.02), a longer-lived ozone-depleting substance

The increasing threat to stratospheric ozone from dichloromethane.

It is well established that anthropogenic chlorine-containing chemicals contribute to ozone layer depletion. The successful implementation of the Montreal Protocol has led to reductions in the atmospheric concentration of many ozone-depleting gases, such as chlorofluorocarbons. As a consequence, stratospheric chlorine levels are declining and ozone is projected to return to levels observed pre-1980 later this century. However, recent observations show the atmospheric concentration of dichloromethane-an ozone-depleting gas not controlled by the Montreal Protocol-is increasing rapidly. Using atmospheric model simulations, we show that although currently modest, the impact of dichloromethane on ozone has increased markedly in recent years and if these increases continue into the future, the return of Antarctic ozone to pre-1980 levels could be substantially delayed. Sustained growth in dichloromethane would therefore offset some of the gains achieved by the Montreal Protocol, further delaying recovery of Earth's ozone layer

Satellite Observations of Stratospheric Hydrogen Flouride and Comparisons with SLIMCAT Calculations

The vast majority of emissions of fluorine-containing molecules are anthropogenic in nature, e.g. chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs), and hydrofluorocarbons (HFCs). Many of these fluorine-containing species deplete stratospheric ozone and are regulated by the Montreal Protocol. Once in the atmosphere they slowly degrade, ultimately leading to the formation of hydrogen fluoride (HF), the dominant reservoir of stratospheric fluorine due to its extreme stability. Monitoring the growth of stratospheric HF is therefore an important marker for the success of the Montreal Protocol. We report the comparison of global distributions and trends of HF measured in the Earth\u27s atmosphere by the satellite remote-sensing instruments ACE-FTS (Atmospheric Chemistry Experiment Fourier transform spectrometer), which has been recording atmospheric spectra since 2004, and HALOE (HALogen Occultation Experiment), which recorded atmospheric spectra between 1991 and 2005, with the output of SLIMCAT, a state-of-the-art three-dimensional chemical transport model. In general the agreement between observation and model is good, although the ACE-FTS measurements are biased high by  ∼  10 % relative to HALOE. The observed global HF trends reveal a substantial slowing down in the rate of increase of HF since the 1990s: 4.97 ± 0.12 % year−1 (1991–1997; HALOE), 1.12 ± 0.08 % year−1 (1998–2005; HALOE), and 0.52 ± 0.03 % year−1 (2004–2012; ACE-FTS). In comparison, SLIMCAT calculates trends of 4.01, 1.10, and 0.48 % year−1, respectively, for the same periods; the agreement is very good for all but the earlier of the two HALOE periods. Furthermore, the observations reveal variations in the HF trends with latitude and altitude; for example, between 2004 and 2012 HF actually decreased in the Southern Hemisphere below  ∼  35 km. An additional SLIMCAT simulation with repeating meteorology for the year 2000 produces much cleaner trends in HF with minimal variations with latitude and altitude. Therefore, the variations with latitude and altitude in the observed HF trends are due to variability in stratospheric dynamics on the timescale of a few years. Overall, the agreement between observation and model points towards the ongoing success of the Montreal Protocol and the usefulness of HF as a metric for stratospheric fluorine

Effects of stratosphere-troposphere chemistry coupling on tropospheric ozone

A new, computationally efficient coupled stratosphere-troposphere chemistry-climate model (S/T-CCM) has been developed based on three well-documented components: a 64-level general circulation model from the UK Met Office Unified Model, the tropospheric chemistry transport model (STOCHEM), and the UMSLIMCAT stratospheric chemistry module. This newly developed S/T-CCM has been evaluated with various observations, and it shows good performance in simulating important chemical species and their interdependence in both the troposphere and stratosphere. The modeled total column ozone agrees well with Total Ozone Mapping Spectrometer observations. Modeled ozone profiles in the upper troposphere and lower stratosphere are significantly improved compared to runs with the stratospheric chemistry and tropospheric chemistry models alone, and they are in good agreement with Michelson Interferometer for Passive Atmospheric Sounding satellite ozone profiles. The observed CO tape recorder is also successfully captured by the new CCM, and ozone-CO correlations are in accordance with Atmospheric Chemistry Experiment observations. However, because of limitations in vertical resolution, intrusion of CO-rich air in the stratosphere from the mesosphere could not be simulated in the current version of S/T-CCM. Additionally, the simulated stratosphere-to-troposphere ozone flux, which controls upper tropospheric OH and O3 concentrations, is found to be more realistic in the new coupled model compared to STOCHEM. © 2010 by the American Geophysical Union

Three-dimensional model study of the Arctic ozone loss in 2002/2003 and comparison with 1999/2000 and 2003/2004

We have used the SLIMCAT 3-D off-line chemical transport model (CTM) to quantify the Arctic chemical ozone loss in the year 2002/2003 and compare it with similar calculations for the winters 1999/2000 and 2003/2004. Recent changes to the CTM have improved the model's ability to reproduce polar chemical and dynamical processes. The updated CTM uses σ-θ as a vertical coordinate which allows it to extend down to the surface. The CTM has a detailed stratospheric chemistry scheme and now includes a simple NAT-based denitrification scheme in the stratosphere. In the model runs presented here the model was forced by ECMWF ERA40 and operational analyses. The model used 24 levels extending from the surface to ~55km and a horizontal resolution of either 7.5° x 7.5° or 2.8° x 2.8°. Two different radiation schemes, MIDRAD and the CCM scheme, were used to diagnose the vertical motion in the stratosphere. Based on tracer observations from balloons and aircraft, the more sophisticated CCM scheme gives a better representation of the vertical transport in this model which includes the troposphere. The higher resolution model generally produces larger chemical O3 depletion, which agrees better with observations. The CTM results show that very early chemical ozone loss occurred in December 2002 due to extremely low temperatures and early chlorine activation in the lower stratosphere. Thus, chemical loss in this winter started earlier than in the other two winters studied here. In 2002/2003 the local polar ozone loss in the lower stratosphere was ~40% before the stratospheric final warming. Larger ozone loss occurred in the cold year 1999/2000 which had a persistently cold and stable vortex during most of the winter. For this winter the current model, at a resolution of 2.8° x 2.8°, can reproduce the observed loss of over 70% locally. In the warm and more disturbed winter 2003/2004 the chemical O3 loss was generally much smaller, except above 620K where large losses occurred due to a period of very low minimum temperatures at these altitudes

Influence of the Arctic Oscillation on the Vertical Distribution of Wintertime Ozone in the Stratosphere and Upper Troposphere over Northern Hemisphere

The influence of the Arctic Oscillation (AO) on the vertical distribution of stratospheric ozone in the Northern Hemisphere in winter is analyzed using observations and an offline chemical transport model. Positive ozone anomalies are found at low latitudes (0–30°N) and there are three negative anomaly centers in the northern mid- and high latitudes during positive AO phases. The negative anomalies are located in the Arctic middle stratosphere (~30 hPa, 70–90°N), Arctic upper troposphere/lower stratosphere (UTLS, 150–300 hPa, 70–90°N), and mid-latitude UTLS (70–300 hPa, 30–60°N). Further analysis shows that anomalous dynamical transport related to AO variability primarily controls these ozone changes. During positive AO events, positive ozone anomalies between 0–30°N at 50–150 hPa are related to the weakened meridional transport of the Brewer–Dobson circulation (BDC) and enhanced eddy transport. The negative ozone anomalies in the Arctic middle stratosphere are also caused by the weakened BDC, while the negative ozone anomalies in the Arctic UTLS are caused by the increased tropopause height, weakened BDC vertical transport, weaker exchange between the mid-latitudes and the Arctic, and enhanced ozone depletion via heterogeneous chemistry. The negative ozone anomalies in the mid-latitude UTLS are due mainly to enhanced eddy transport from the mid-latitudes to the equatorward of 30°N, while the transport of ozone-poor air from the Arctic to the mid-latitudes makes a minor contribution. Interpreting AO-related variability of stratospheric ozone, especially in the UTLS, would be helpful for the prediction of tropospheric ozone variability caused by AO