Document Type

Article

Publication Date

2025

DOI

10.1029/2024JD042298

Publication Title

Journal of Geophysical Research: Atmospheres

Volume

130

Issue

15

Pages

e2024JD042298 (1-19)

Abstract

We present fluorine inventories calculated for twenty years (2004–2023) and five latitude bands (82°–60°N, 60°–30°N, 30°N–30°S, 30°–60°S, and 60°–82°S) at altitudes from the surface up to 55 km. The inventories were calculated using the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE‐FTS) version 5.2 retrievals of the volume mixing ratios (VMRs) of 15 fluorine‐containing species. Of these 15 species, 3 are product gases: HF, COF₂, COCIF, and 12 are source gases: SF₆, PFC-14 (CF₄), CFC-11 (CCl₃F), CFC-12 (CCl₂F₂), CFC-113 (CCIF₂CCl₂F), HCFC-22 (CHF₂CL), HCFC-141b(C₂H₃Cl₂F), HCFC-142b (C₂H₃CIF₂), HFC-23 (CHF₃), HFC-32 (CH₂F₂) HFC-125 (C₂HF₅) and HFC-134a (C₂H₂F₄). As necessary, ACE-FTS data were supplemented with data from the TOMCAT 3-D chemical transport model and ground-based measurements from the National Oceanic and Atmopsheric Administration (NOAA) and the Advanced Global Atmospheric Gases Experiment (AGAGE). The total fluorine (Ftot) profiles are dominated by source gas contributions in the troposphere and lower stratosphere up to 35 km in the tropics 30°N-30°S), 30 km in midlatitudes (60°-30°N/30°-60°S) and 24 km near the poles (82°-60°N/60°-82°S). In this atmospheric region, the primary contributions come from CFCs, HCFCs, carbon tetrafluoride (CF₄), and increasingly in recent years HFCs. Above these altitudes HF increasingly dominates the Ftot profile reaching as much as 79% of Ftot at 55 km. The 2004-2023 time series of the mean Ftot inventories shows a global increase of 48.9 ± 0.7 ppt/year or 1.68 ± 0.02%/year resulting in a mean Ftot approaching 3.5 ppb in 2023.

Rights

© 2025 The Authors.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International (CC BY 4.0) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.

Data Availability

Article states: "ACE-FTS version 5.2 retrieval results and ACE-imager extinction profiles are freely available from the ACE web portal: https://databace.scisat.ca/level2/ace_v5.2/display_data.php (ACE-SOC, 2024). Initial registration is required at https://databace.scisat.ca/l2signup.php. Version 5.2 is also available at https://doi.org/10.20383/103.01245 (Bernath et al., 2025). NOAA data were obtained from their GML, publicly available online: https://gml.noaa.gov/dv/data/ (NOAA-GML, 2024), or https://gml.noaa.gov/hats/data.html (NOAA-LOGOS, 2024). Files for each species were downloaded individually, such as the CFC-11 HATS combined file at https://gml.noaa.gov/aftp/data/hats/cfcs/cfc11/combined/HATS_global_F11.txt (Dutton et al., 2024). AGAGE data were originally obtained from AGAGE-data (2024) but can also be found in Prinn et al. (2023). All measurements from AGAGE were obtained in a single file."

Original Publication Citation

Raymond, N., Bernath, P., Boone, C., & Chipperfield, M. (2025). Twenty years of global stratospheric fluorine inventories from Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE‐FTS) measurements. Journal of Geophysical Research: Atmospheres, 130(15), 1-19, Article e2024JD042298. https://doi.org/10.1029/2024JD042298

ORCID

0000-0002-1255-396X (Bernath)

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