Tha Canadian High altitude Aerosol Water vapour and Cloud (HAWC) mission is built upon innovative Canadian optical remote sensing technology and will provide important information related to water vapour, aerosols and cloud microphysics in the upper troposphere and lower stratopshere. HAWC is made up of three Canadian passive optical instruments, the Spatial Hetrodyne Observations of Water (SHOW), the Aerosol Limb Imager (ALI) and the Thin Ice Cloud and Far infraRed Emissions (TICFIRE) where the first two look at scattered sunlight in the atmospheric limb from low earth orbit and the latter instrument measures thermal emission in the nadir, also from low earth orbit. This presentation will outline the technology, the measurements and the expected scientific return of the HAWC mission that is expected to launch in the first part of the next decade.
The Changing-Atmosphere Infra-Red Tomography Explorer (CAIRT) is currently in Phase A as one of two final candidates for ESA’s Earth Explorer 11. As a Fourier transform infrared limb imager, CAIRT will observe simultaneously from the middle troposphere to the lower thermosphere at high spectral resolution and with unprecedented horizontal and vertical resolution. With this, CAIRT will provide critical information on (a) atmospheric gravity waves, circulation and mixing, (b) coupling with the upper atmosphere, solar variability and space weather and, (c) aerosols and pollutants in the upper troposphere and lower stratosphere. In this presentation we will give an overview of CAIRT’s science goals and the expected mission performance, based on latest results from feasibility studies performed during Phase 0.
Many stratospheric trace gases, including O3, HCl, and NOy, have had opposing trends in the Southern Hemisphere (SH) compared to the Northern Hemisphere (NH) during the last 2 decades. Some of this difference is due to hemispherically asymmetric changes in the rate of transport by the Brewer–Dobson circulation (BDC), and some is due to ozone depletion and recovery. The mean age of air (AoA) is a common proxy for the transport rate by the BDC in models; however it cannot be directly measured. We use observations from the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) along with results from the Chemical Lagrangian Model of the Stratosphere (CLaMS) to derive AoA anomalies and AoA trends. The AoA is derived using observations of N2O, CH4, and CFC-12, all long-lived trace gases with tropospheric sources. We also consider CLaMS simulations driven with four different reanalyses (ERA5, ERA-Interim, JRA-55, MERRA-2). We find that, irrespective of which trace gas or reanalysis is used, air in the NH aged by up to 0.3 years per decade relative to the SH over 2004–2017. The maximum hemispheric difference in aging occurs in the middle stratosphere, near 30 hPa (∼ 24 km). We also show that the aging rate in the NH becomes smaller when the analysis is extended to 2021. The observed aging in the NH middle stratosphere contradicts model predictions of a decrease in stratospheric AoA in response to rising atmospheric greenhouse gas levels. However, the smaller aging rate during 2004–2021 compared to 2004–2017 provides some evidence that the NH aging is impacted by decadal variability and the limited length of the observation period.
Launched aboard the Canadian SCISAT satellite in August 2003, the Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (MAESTRO) instrument has been measuring solar absorption spectra in the ultraviolet (UV) and visible part of the spectrum for more than 20 years. The UV-channel measurements from MAESTRO are used to retrieve profiles of ozone from the short-wavelength end of the Chappuis band (UV-ozone) and NO2, while measurements made in the visible part of the spectrum are used to retrieve a separate ozone (Vis-ozone) product. The latest ozone and NO2 profile products, version 4.5, have been released, and they initially cover the period from February 2004 to December 2023, although they will continue to be updated. The version 4.5 retrieval algorithm represents an improvement from previous versions, with changes including updated pressure and temperature input information, an improved algorithm for high-Sun reference spectrum calculation, improved Rayleigh scattering modelling, and the change to a Twomey–Tikhonov inversion algorithm from a Chahine relaxation technique. Due to the buildup of an unknown contaminant, the UV-ozone and NO2 products are only viable up to June 2009 for NO2 and December 2009 for UV-ozone. This study presents comparisons of the version 4.5 MAESTRO ozone and NO2 measurements with coincident (both spatially and temporally) measurements from an ensemble of 11 other satellite limb-viewing instruments. In the stratosphere, the Vis-ozone product was found to possess a small high bias, with stratosphere-averaged relative differences between 2.3 % and 8.2 %, although good agreement with the comparison datasets was found overall. A similar bias, albeit with slightly poorer agreement, is found for the UV-ozone product in the stratosphere, with the average stratospheric agreement between MAESTRO and the other datasets ranging from 2.8 % to 11.9 %. For NO2, general agreement with the comparison datasets is only found in the range from 20 to 40 km. Within this range, MAESTRO is found to have a low bias for NO2, and most of the datasets agree to within 27.2 %, although the average agreement ranges from 8.5 % to 43.4 %.
Field evidence has confirmed a new sea salt aerosol (SSA) source on sea ice, which may significantly affect polar boundary layer chemistry and polar winter climate. While the SSA production rate from blowing snow has been previously parameterised (Yang et al., 2008) and then validated by measurements at both Poles, some key parameters involved are not yet fully constrained, leading to uncertainties when using numerical models to compare with field measurements and assess their environmental and climate impacts. In this presentation, we focus on two key parameters: blowing snow size distribution and snow salinity, which determine SSA production in number and size, respectively. We aim to constrain these factors using the latest field data, supported by remote sensing BrO data and modelling. Blowing snow particles typically follow a two-parameter gamma distribution function with shape factor (alpha) and scaling factor (beta) varying over a large range. However, our recent work focusing on the Arctic Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition data showed that at a given height, beta values increase with wind speeds, while alpha gradually approach a constant value of 1.9 at higher wind speeds (e.g. larger than 10 m/s). This is the first time that we derive such a relationship for blowing snow, which further affirms the aerosol production mechanism from blowing snow and helps elucidate the underlying processes involved. Accordingly, we parameterised the blowing snow particle size distribution as a function of wind speed, accounting for variable wind speeds during storms. In addition, supported by a chemistry transport model (p-TOMCAT), we examined the sensitivities of SSA mass and reactive bromine release rate (in association with the SSA production) to representative snow salinities derived from observations in the central Arctic and coastal regions (at Eureka, Canada). Mean winter/springtime snow salinities that best represent the Arctic were derived by comparing the modelled BrO with ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) and air-based satellite-based GOME-2 BrO data at Svalbard and Eureka.
According to satellite measurements from multiple instruments, water vapour (H2O) concentrations, in most regions of the stratosphere, have been increasing at a statistically significant rate of ∼1 %–5 % per decade since the early 2000s. Previous studies have estimated stratospheric H2O trends, but none have simultaneously quantified the contributions from all main sources (temperature variations in the tropical tropopause region, changes in the Brewer–Dobson circulation, and changes in methane (CH4) concentrations and oxidation) at all latitudes. Atmospheric Chemistry Experiment–Fourier Transform Spectrometer (ACE-FTS) measurements are used to estimate altitude-/latitude-dependent stratospheric H2O trends from 2004–2021 due to these sources. Results indicate that rising temperatures in the tropical tropopause region play a significant role in the increases, accounting for ∼1 %–4 % per decade in the tropical lower mid-stratosphere and in the mid-latitudes below ∼20 km. By regressing to ACE-FTS N2O concentrations, it is found that, in the lower mid-stratosphere, general circulation changes have led to both significant H2O increases and significant H2O decreases on the order of 1 %–2 % per decade depending on the altitude/latitude region. Making use of measured and modelled CH4 concentrations, the increase in H2O due to CH4 oxidation is calculated to be ∼1 %–2 % per decade above ∼30 km in the Northern Hemisphere and throughout the stratosphere in the Southern Hemisphere. After accounting for these sources, there are still regions of the mid-latitude lower mid-stratosphere that exhibit significant residual H2O trends increasing at 1 %–2 % per decade. Results indicate that these unaccounted-for increases could potentially be explained by increases in upper-tropospheric molecular hydrogen.
The Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (MAESTRO) instrument on the SCISAT satellite provides aerosol extinction measurements in multiple solar wavelength bands. In this study, we evaluate the quality and utility of MAESTRO version 3.13 stratospheric aerosol extinction retrievals, from February 2004-February 2021, through comparison with measurements from other satellite instruments. Despite significant scatter in the MAESTRO data, we find that gridded median MAESTRO aerosol extinctions and stratospheric aerosol optical depth (SAOD) values are generally in good agreement with those from other instruments during volcanically quiescent periods. After volcanic eruptions and wildfire injections, gridded median MAESTRO extinction and SAOD are well correlated with other measurement sets but generally biased low by 40 %-80 %. The & Aring;ngstr & ouml;m exponent (AE), which can provide information on aerosol particle size, is derived from the MAESTRO spectral extinction measurements in the lowermost stratosphere, showing perturbations after volcanic eruptions qualitatively similar to those from the Stratospheric Aerosol and Gas Experiment on the International Space Station (SAGE III/ISS) for the eruptions of Ambae (2018) and Ulawun (2019). Differences in AE anomalies after the 2019 extratropical Raikoke eruption may be due to the different spatiotemporal sampling of the two instruments. Furthermore, we introduce a method to adjust MAESTRO extinction data based on comparison with extinction measurements from SAGE III/ISS during the period from June 2017-February 2021, resulting in improved comparison during volcanically active periods. Our work suggests that empirical bias correction may enhance the utility of MAESTRO aerosol extinction data, which can make it a useful complement to existing satellite records, especially when multi-wavelength solar occultation data from other instruments are unavailable.
To determine the long-term effect of Australian bushfires on the upper tropospheric composition in the South Pacific, we investigated the variation in CO and hydrocarbon species in the South Pacific according to the extent of Australian bushfires (2004–2020). We conducted analyses using satellite data on hydrocarbon and CO from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), and on fire (fire count, burned area, and fire radiative power) from the Moderate Resolution Imaging Spectroradiometer (MODIS). Additionally, we compared the effects of bushfires between Northern and Southeastern Australia (N_Aus and SE_Aus, respectively). Our analyses show that Australian bushfires in austral spring (September to November) result in the largest increase in CO and hydrocarbon species in the South Pacific and even in the west of South America, indicating the trans-Pacific transport of smoke plumes. In addition to HCN (a well-known wildfire indicator), CO and other hydrocarbon species (C2H2, C2H6, CH3OH, HCOOH) are also considerably increased by Australian bushfires. A unique finding in this study is that the hydrocarbon increase in the South Pacific mostly relates to the bushfires in N_Aus, implying that we need to be more vigilant of bushfires in N_Aus, although the severe Australian bushfire in 2019–2020 occurred in SE_Aus. Due to the surface conditions in springtime, bushfires on grassland in N_Aus during this time account for most Australian bushfires. All results show that satellite data enables us to assess the long-term effect of bushfires on the air composition over remote areas not having surface monitoring platforms.
Over the past few decades, a reduction in chlorinated long-lived ozone-depleting substance emissions due to the regulations imposed by the Montreal Protocol has led to a global decrease in stratospheric chlorine. At the same time, emissions of chlorinated Very Short-Lived Substances, which are unregulated, have increased. Here we show that observed changes of inorganic stratospheric chlorine are inconsistent with changes in the tropospheric abundances of long-lived ozone-depleting substances. Satellite observations of stratospheric chlorine species from the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer during 2004-2020 reveal that the observed decrease in inorganic stratospheric chlorine is 25%-30% smaller than expected based on trends of long-lived ozone-depleting substances alone. At mid-latitudes in the lower stratosphere, this can be explained by the chlorinated Very Short-Lived Substances increase, which offsets the long-term reduction of stratospheric chlorine by up to 30%.
The High-Altitude Aerosols, Water Vapor, and Clouds (HAWC) mission is an observing system, with a planned launch around 2031, that is being developed by the Canadian Space Agency to provide collocated global measurements of aerosols, water vapor, and thin ice clouds in the upper troposphere and lower stratosphere with vertical coverage that extends into the troposphere in the polar regions. The mission is the Canadian contribution to NASA's Atmospheric Observing System (AOS), a satellite constellation will include multiple instruments to monitor aerosols, clouds, and precipitation as part of Earth System Observatory (ESO). The HAWC mission includes three innovative Canadian instruments: the Aerosol Limb Imager (ALI), the Thin Ice Clouds and Far Infrared Emissions (TICFIRE) instrument, and the Spatial Heterodyne Observations of Water (SHOW) instrument. ALI and SHOW will provide limb profiles of aerosol and water vapor with high spatial resolution (vertical and along track) and high sensitivity to fine aerosols and dry conditions. TICFIRE will provide nadir measurements of infrared radiation, thin ice cloud content, and cloud microphysical properties. These coordinated measurements will help build a more comprehensive picture of high-altitude aerosols, clouds, and water vapor in the atmosphere. In this paper, we present the HAWC concept and discuss the primary science objectives and requirements of the mission. The instrument payloads and data products are introduced, and synergies between HAWC and other AOS instruments are identified.
The Brewer-Dobson Circulation (BDC) is one of the main determinants of trace gas distributions in the atmosphere. Climate models predict that atmospheric warming will cause the BDC to accelerate, modifying where greenhouse gases are most active and impacting the radiative properties of the atmosphere, resulting in a feedback effect. This acceleration is difficult to verify with observations because the speed of the BDC cannot be measured directly. However, changes in stratospheric transport can be identified using the stratospheric age of air, defined as the time since an air parcel entered the stratosphere from the troposphere. A decrease in age of air at higher latitudes would suggest a reduction in transit times, signifying an acceleration of the BDC. Age of air can be calculated using long-lived “clock tracers” such as sulfur hexafluoride (SF6), an industrial gas that is produced in the troposphere, has a negligible seasonal cycle, and has no stratospheric sinks. Due to its small concentrations, measurements have been historically limited, but detecting changes in age of air derived from SF6 requires a long-term, and ideally consistent (i.e., measured by the same instrument), time series. The Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) provides the longest available vertically-resolved record of SF6, spanning 2004 to the present. This study presents a new age of air product derived from the ACE-FTS SF6 dataset using an updated version of the method used for the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) SF6 dataset, which spans the 2002-2012 period. In this presentation, the method for age of air calculation will be presented along with comparisons with other age of air profile datasets derived from MIPAS and balloon measurements. The long-term trend in age of air will be estimated using this new product with the goal of corroborating the predictions made by climate models.
The Changing-Atmosphere Infra-Red Tomography (CAIRT) mission was proposed as ESA's Earth Explorer 11 candidate to address critical gaps in understanding the middle atmosphere and its role in climate forcing and feedbacks. Using an innovative imaging Fourier Transform Spectrometer, CAIRT combines limb sounding with high-resolution infrared spectroscopy to deliver unprecedented 3D observations of atmospheric composition, temperature, aerosols, and optically thin clouds. These measurements are needed to improve understanding of processes such as gravity wave dynamics, tracer transport, and long-term circulation trends. This paper provides an overview of the mission's scientific objectives, the observation concept, and key technical requirements, followed by a detailed account of the system architecture developed during the Phase 0 and Phase A studies. Two payload concepts were defined and matured, sharing the same measurement technique but differing in implementation details. Extensive pre-development activities were conducted to de-risk critical subsystems including the interferometer, detector assemblies, cryogenic cooling, and pointing mechanisms. At the end of Phase A, the mission was deemed to have reached the required scientific and technical readiness level and demonstrated strong scientific relevance.
Two decades of ACE-FTS, the Atmospheric Chemistry Experiment - Fourier Transform Spectrometer, version 5.2 (v5.2) ozone data (2004-2023) are evaluated with ozonesonde data from across the globe. The biases between the ACE-FTS and ozonesonde measurements are first estimated by analyzing coincident data pairs. A second approach is taken for the validation by comparing the ACE-FTS and ozonesonde monthly mean time series, with the former generated by sampling the ACE-FTS data within latitude/longitude boxes (i.e., +/- 5 degrees/+/- 30 degrees) surrounding the stations and calculating the monthly averages. The biases, correlations, variation patterns, and the mean states of the two time series are compared. The biases estimated in this way exhibit more consistent and smoother features than using the coincident pair method. The ACE-FTS and ozonesonde monthly mean time series are highly correlated and exhibit similar variation patterns in the lower stratosphere at all latitudes. The ACE-FTS instrument drifts for each station are assessed in terms of the long-term linear trends relative to ozonesondes, which, although highly stable, may have their own minor changes with time. The ACE-FTS ozone profiles exhibit in general high biases in the stratosphere for altitudes above similar to 20 km, increasing with altitude up to similar to 10 % at around 30 km. For altitudes between 20 km and the tropopause, biases of up to +/- 10 % are found, depending on altitude and latitude with the largest biases found in the tropics and southern mid-latitudes. The ACE-FTS instrument drifts are generally non-significant overall in the stratosphere with high variation between the stations. Averaging the individual station instrument drifts within several latitude bands results in small non-significant drifts of within +/- 1 %-2 % per decade in the northern mid-latitudes to high latitudes and the southern high latitudes. It also results in a positive but non-significant drift of up to 5 % per decade in the tropics and southern mid-latitudes, with overall uncertainties in this region ranging up to 5 %-10 % per decade (2 sigma level) in the low stratosphere. As part of this assessment, an analysis of ozonesonde measurement stability using ACE-FTS as a transfer standard is conducted and finds small step changes in ozonesonde response at some stations. These results are in general agreement with recent findings using other satellite data sources.
This study evaluates tropospheric columns of methane, carbon monoxide, and ozone in the Arctic simulated by 11 models. The Arctic is warming at nearly 4 times the global average rate, and with changing emissions in and near the region, it is important to understand Arctic atmospheric composition and how it is changing. Both measurements and modelling of air pollution in the Arctic are difficult, making model validation with local measurements valuable. Evaluations are performed using data from five high-latitude ground-based Fourier transform infrared (FTIR) spectrometers in the Network for the Detection of Atmospheric Composition Change (NDACC). The models were selected as part of the 2021 Arctic Monitoring and Assessment Programme (AMAP) report on short-lived climate forcers. This work augments the model–measurement comparisons presented in that report by including a new data source: column-integrated FTIR measurements, whose spatial and temporal footprint is more representative of the free troposphere than in situ and satellite measurements. Mixing ratios of trace gases are modelled at 3-hourly intervals by CESM, CMAM, DEHM, EMEP MSC-W, GEM-MACH, GEOS-Chem, MATCH, MATCH-SALSA, MRI-ESM2, UKESM1, and WRF-Chem for the years 2008, 2009, 2014, and 2015. The comparisons focus on the troposphere (0–7 km partial columns) at Eureka, Canada; Thule, Greenland; Ny Ålesund, Norway; Kiruna, Sweden; and Harestua, Norway. Overall, the models are biased low in the tropospheric column, on average by −9.7 % for CH4, −21 % for CO, and −18 % for O3. Results for CH4 are relatively consistent across the 4 years, whereas CO has a maximum negative bias in the spring and minimum in the summer and O3 has a maximum difference centered around the summer. The average differences for the models are within the FTIR uncertainties for approximately 15 % of the model–location comparisons.
HCFC-22 is an ozone-depleting substance with a greenhouse effect. The atmospheric mole fractions of HCFC-22 have been increasing since the 1950s. Within the NDACC-IRWG network, HCFC-22 mol fractions can be retrieved from solar absorption spectra measured by ground-based FTIR. However, only a few sites have provided HCFC-22 data sets. Here, we demonstrate a harmonized FTIR HCFC-22 retrieval strategy and generate a new global NDACC-IRWG HCFC-22 data set at 16 FTIR sites. The systematic and random uncertainties are 5.3%-8.7% and 3.2%-8.0%, respectively. A maximum HCFC-22 column annual growth rate was observed in 2009 with a mean of 7.65 +/- 1.39 ppt/year, and the HCFC-22 annual growth rate decreased to 3.57 +/- 1.39 ppt/year (2016-2020) and 2.15 +/- 2.09 ppt/year (2021-2023). The annual growth rates derived from the FTIR measurements are compared to the ones derived from NOAA surface flask samplings and ACE-FTS satellite measurements, and the three independent data sets show a good agreement.
This study explores the role of snowpack in polar boundary layer chemistry, especially as a direct source of reactive bromine (BrOx = BrO + Br) and nitrogen (NOx = NO + NO2) in the Arctic springtime. Surface snow samples were collected daily from a Canadian high Arctic location at Eureka, Nunavut (80° N, 86° W) from the end of February to the end of March in 2018 and 2019. The snow was sampled at several sites representing distinct environments: sea ice, inland close to sea level, and a hilltop ∼ 600 m above sea level (a.s.l.). At the inland sites, surface snow salinity has a double-peak distribution with the first and lowest peak at 0.001–0.002 practical salinity unit (psu), which corresponds to the precipitation effect, and the second peak at 0.01–0.04 psu, which is likely related to the salt accumulation effect (due to loss of water vapour by sublimation). Snow salinity on sea ice has a triple-peak distribution; its first and second peaks overlap with the inland peaks, and the third peak at 0.2–0.4 psu is likely due to the sea water effect (a result of upward migration of brine). At all sites, snow sodium and chloride concentrations increase by almost 10-fold from the top 0.2 to ∼ 1.5 cm. Surface snow bromide at sea level is significantly enriched, indicating a net sink of atmospheric bromine. Moreover, surface snow bromide at sea level has an increasing trend over the measurement period, with mean slopes of 0.024 µM d−1 in the 0–0.2 cm layer and 0.016 µM d−1 in the 0.2–0.5 cm layer. Surface snow nitrate at sea level also shows a significant increasing trend, with mean slopes of 0.27, 0.20, and 0.07 µM d−1 in the top 0.2, 0.2–0.5, and 0.5–1.5 cm layers, respectively. Using these trends, an integrated net deposition flux of bromide of (1.01 ± 0.48) × 107 molec.cm-2s-1 and an integrated net deposition flux of nitrate of (2.6 ± 0.37) × 108 molec.cm-2s-1 were derived. In addition, the surface snow nitrate and bromide at inland sites were found to be significantly correlated (R = 0.48–0.76) with the [NO3-]/[Br-] ratio of 4–7 indicating a possible acceleration effect of reactive bromine in atmospheric NOx-to-nitrate conversion. This is the first time such an effect has been seen in snow chemistry data obtained with a sampling frequency as short as 1 d. BrO partial column (0–4 km) data measured by MAX-DOAS show a decreasing trend in early spring, which generally agrees with the derived surface snow bromide deposition flux indicating that bromine in Eureka atmosphere and surface snow did not reach a photochemical equilibrium state. Through mass balance analysis, we conclude that the average release flux of reactive bromine from snow over the campaign period must be smaller than the derived bromide deposition flux of ∼ 1 × 107 molec.cm-2s-1. Note that the net mean fluxes observed do not completely rule out larger bidirectional fluxes over shorter timescales.
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 δD, 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 δD 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 δD 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 δD 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.
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.
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.