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Ozone trends in the upper troposphere and lower stratosphere (UTLS) remain highly uncertain because of sharp spatial gradients and high variability caused by competing transport, chemical, and mixing processes near the upper-tropospheric jets and extratropical tropopause as well as inhomogeneous spatially and temporally limited observations of the region. Subtropical jets and the tropopause act as transport barriers, delineating boundaries between atmospheric regimes controlled by different processes; they can thus be used to separate data taken in those different regimes for numerous purposes, including trend assessment. As part of the Observed Composition Trends And Variability in the UTLS (OCTAV-UTLS) Stratosphere-troposphere Processes And their Role in Climate (SPARC) activity, we assess the effectiveness of several coordinate systems in segregating air into different atmospheric regimes. To achieve this, a comprehensive dynamical dataset is used to reference every measurement from various observing systems to the locations of jets and tropopauses in different coordinates (e.g., altitude, pressure, potential temperature, latitude, and equivalent latitude). We assess which coordinate combinations are most useful for dividing the measurements into bins such that the data in each bin are affected by the same processes, thus minimizing the variability induced when combining measurements from different dynamical regimes, each characterized by different physical processes. Such bins will be particularly suitable for combining measurements with different sampling characteristics and for assessing trends and attributing them to changing atmospheric dynamics. Overall, the use of equivalent latitude and potential temperature leads to the most substantial reduction in binned variability across the UTLS. This coordinate pairing uses potential vorticity (PV) on isentropic surfaces, thus aligning with the adiabatic transport of tracers. [ABSTRACT FROM AUTHOR]

Variations in the isotopologic composition of water vapour are fundamental for understanding the relative importance of different mechanisms of water vapour transport from the tropical upper troposphere to the lower stratosphere. Previous comparisons obtained from observations of H2O and HDO by satellite instruments showed discrepancies. In this work, newer versions of H2O and HDO retrievals from Envisat/MIPAS and SCISAT/ACE-FTS are compared. Specifically, MIPAS-IMK V5, MIPAS-ESA V8 and ACE-FTS V4.1/4.2 for the common period from February 2004 to April 2012 are compared for the first time through a profile-to-profile approach and comparison based on climatological structures. The comparison is essential for the scientific community to assess the quality of new satellite data products, a necessary procedure to validate further scientific work. Averaged stratospheric H2O profiles reveal general good agreement between 16 and 30 km. Biases derived from the profile-to-profile comparison are around zero between 16 and 30 km for MIPAS-IMK and ACE-FTS comparison. For HDO and δ D, low biases are found in the MIPAS-ESA and ACE-FTS comparison in the same range of altitudes, even if associated with a larger de-biased standard deviation. The zonally averaged cross sections of H2O and HDO exhibit the expected distribution that has been established in previous studies. For δ D the tropical depletion in MIPAS-ESA occurs at the top of the dynamical tropopause, but this minimum is found at higher altitudes in the ACE-FTS and MIPAS-IMK dataset. The tape recorder signal is present in H2O and HDO for the three databases with slight quantitative differences. The δ D annual variation for ACE-FTS data and MIPAS-ESA data is weaker compared to the MIPAS-IMK dataset, which shows a coherent tape recorder signal clearly detectable up to at least 30 km. The observed differences in the climatological δ D composites between databases could lead to different interpretations regarding the water vapour transport processes toward the stratosphere. Therefore, it is important to further improve the quality of level 2 products. [ABSTRACT FROM AUTHOR]

The Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) is currently providing the only measurements of vertically resolved chlorodifluoromethane (HCFC-22) from space. This study assesses the ACE-FTS HCFC-22 v5.2 product in the upper troposphere and lower stratosphere, as well as simulations of HCFC-22 from a 39-year specified dynamics run of the Canadian Middle Atmosphere Model (CMAM39) in the same region. In general, ACE-FTS HCFC-22 observations tend to agree with subsampled CMAM39 data to within ±5 %, except for between ∼ 15 and 25 km in the extratropical regions where ACE-FTS exhibits a negative bias of 5 %–30 % and near 6 km in the tropics where ACE-FTS exhibits a bias of - 15 %. When comparing against correlative satellite, aircraft, and balloon data, ACE-FTS typically exhibits a low bias on the order of 0 %–10 % between ∼ 5 and 15 km and is within ±15 % between ∼ 15 and 25 km. ACE-FTS, CMAM39, and surface flask measurements from the NOAA Global Monitoring Laboratory's surface air-sampling network all exhibit consistent tropospheric HCFC-22 trends ranging between 6.8 and 7.8 ppt yr -1 (within 95 % confidence) for 2004–2012 and between 3.1 and 4.7 ppt yr -1 (within 95 % confidence) for 2012–2018. Interhemispheric differences (IHDs) of HCFC-22 were also derived using ACE-FTS, NOAA, and CMAM39 data, and all three yielded consistent and correlated (r≥0.42) IHD time series, with the results indicating that surface IHD values decreased at a rate of 2.2 ± 1.1 ppt per decade between 2004 and 2018. [ABSTRACT FROM AUTHOR]

The Measurements Of Pollution In The Troposphere (MOPITT) instrument aboard NASA's Terra satellite has been measuring upwelling radiance in a nadir-viewing mode since March 2000. These radiance measurements are inverted to yield estimates of carbon monoxide (CO) profiles and total columns, providing the longest satellite record of this trace gas to date. The CO measurements from MOPITT have been used in a variety of ways, including trend analyses and the construction of CO budgets. However, their use is complicated by the influence of episodic emission events, which release large quantities of CO into the atmosphere with irregular timing, such as large sporadic wildfires of natural or anthropogenic origin. The chaotic nature of these events is a large source of variability in CO budgets and models, requiring that these events be well characterized in order to develop an improved understanding of the role they have in influencing tropospheric CO. This study describes the development of a multistep algorithm that is used to identify large episodic emission events using daily mean Level 2 (L2) MOPITT total column measurements gridded to a 0.5 by 0.5° spatial resolution. The core component of this procedure involves empirically determining the expectation density function (EDF) that describes the departure of daily-mean CO observations from the baseline behaviour of CO, as described by its periodic components and trends. The EDFs employed are not assumed to be symmetric but instead are constructed from a pair of superimposed normal distributions. Enhancement flag files are produced following this methodology, identifying the episodic events that show strong enhancement of CO outside of the range of expected CO behaviour and are now made available for the period 3 March 2000 to 31 July 2022. The distribution and frequency of these flagged measurements over this 22-year period are analyzed in order to illustrate the robustness of this method. [ABSTRACT FROM AUTHOR]

Ozone trends in the upper troposphere/lower stratosphere (UTLS) remain highly uncertain because of sharp spatial gradients and large variability caused by competing transport, chemical, and mixing processes near the upper tropospheric jets and extra-tropical tropopause, as well as inhomogeneous spatially and temporally limited observations of the region. Subtropical jets and the tropopause act as transport barriers, delineating boundaries between atmospheric regimes controlled by different processes; they can thus be used to separate data taken in those different regimes for numerous purposes, including trend assessment. As part of the Observed Composition Trends And Variability in the UTLS (OCTAV-UTLS) Stratosphere-troposphere Processes And their Role in Climate (SPARC) activity, we assess the effectiveness of several coordinate systems in segregating air into different atmospheric regimes. To achieve this, a comprehensive dynamical dataset is used to reference every measurement from various observing systems to the locations of jets and tropopauses in different coordinates (e.g., altitude, pressure, potential temperature, latitude, and equivalent latitude). We assess which coordinate combinations are most useful for dividing the measurements into bins such that the data in each bin is affected by the same processes, thus minimizing the variability induced when combining measurements from different dynamical regimes, each characterized by different physical processes. Such bins will be particularly suitable for combining measurements with different sampling characteristics and for assessing trends and attributing them to changing atmospheric dynamics. [ABSTRACT FROM AUTHOR]

The Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) is currently providing the only measurements of vertically resolved chlorodifluoromethane (HCFC-22) from space. This study assesses the ACE-FTS HCFC-22 v5.2 product in the upper troposphere – lower stratosphere, as well as the simulated concentrations of HCFC-22 from a 39-year specified dynamics run of the Canadian Middle Atmosphere Model (CMAM39) in the same region. In general, ACE-FTS HCFC-22 observations tend to agree with subsampled CMAM39 data to within ±5 %, except for between ~15 and 25 km in the extratropical regions where ACE-FTS exhibits a negative bias of 5–30 %, and near 6 km in the tropics where ACE FTS exhibits a bias of 15 %. When comparing against correlative satellite, aircraft, and balloon data, ACE-FTS typically exhibits a low bias on the order of 0–10 % between ~5–15 km and is within ±15 % between ~15–25 km. ACE-FTS, CMAM39, and surface flask measurements from the NOAA Global Monitoring Laboratory's surface air-sampling network, all exhibit consistent tropospheric HCFC-22 trends ranging between 6.8 and 7.8 pptv/year (within 95 % confidence) for 2004–2012, and between 3.1 and 4.7 pptv/year (within 95 % confidence) for 2012–2018. Interhemispheric differences (IHD) of HCFC-22 concentrations were also derived using ACE-FTS, NOAA, and CMAM39 data, and all three yielded consistent and correlated (r≥0.42) IHD timeseries, with the results indicating that surface IHD values decreased at a rate of 2.2±1.1 pptv/decade between 2004 and 2018. [ABSTRACT FROM AUTHOR]

The Measurements Of Pollution In The Troposphere (MOPITT) instrument aboard NASA's Terra satellite has been measuring upwelling radiance in a nadir-viewing mode since March 2000. These radiance measurements are inverted to yield estimates of carbon monoxide (CO) profiles and total columns, providing the longest satellite record of this trace gas to date. The CO measurements from MOPITT have been used in a variety of ways, including trend analyses and the construction of CO budgets. However, their use is complicated by the influence of episodic emission events, which release large quantities of CO into the atmosphere with irregular timing, such as large sporadic wildfires of natural or anthropogenic origin. The chaotic nature of these events is a large source of variability in CO budgets and models, requiring that these events be well characterized in order to develop an improved understanding of the role they have in influencing tropospheric CO. This study describes the development of a multi-step algorithm that is used to identify large episodic emission events using daily-mean Level 2 (L2) MOPITT total column measurements gridded to 0.5° by 0.5° spatial resolution. The core component of this procedure involves empirically determining the expectation density function (EDF) that describes the departure of daily-mean CO observations from the baseline behaviour of CO, as described by its periodic components and trends. The EDFs employed are not assumed to be symmetric, but instead are constructed from a pair of superimposed normal distributions. Enhancement flag files are produced following this methodology, identifying the episodic events that show strong enhancement of CO outside of the range of expected CO behaviour, and are now made available for the period 3 March 2000 to 31 July 2022. The distribution and frequency of these flagged measurements over this 22-year period is analyzed, to illustrate the robustness of this method. [ABSTRACT FROM AUTHOR]