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See detailAtmospheric implications of large C2-C5 alkane emissions from the U.S. oil and gas industry
Tzompa-Sosa, Z; Henderson, B H; Keller, C A et al

in Journal of Geophysical Research. Atmospheres (2019), (2013), 1--22

Emissions of C2-C5 alkanes from the U.S. oil and gas sector have changed rapidly over the last decade. We use a nested GEOS-Chem simulation driven by updated 2011NEI emissions with aircraft, surface and ... [more ▼]

Emissions of C2-C5 alkanes from the U.S. oil and gas sector have changed rapidly over the last decade. We use a nested GEOS-Chem simulation driven by updated 2011NEI emissions with aircraft, surface and column observations to 1) examine spatial patterns in the emissions and observed atmospheric abundances of C2-C5 alkanes over the U.S., and 2) estimate the contribution of emissions from the U.S. oil and gas industry to these patterns. The oil and gas sector in the updated 2011NEI contributes over 80% of the total U.S. emissions of ethane (C2H6) and propane (C3H8), and emissions of these species are largest in the central U.S. Observed mixing ratios of C2-C5 alkanes show enhancements over the central U.S. below 2 km. A nested GEOS-Chem simulation underpredicts observed C3H8 mixing ratios in the boundary layer over several U.S. regions and the relative underprediction is not consistent, suggesting C3H8 emissions should receive more attention moving forward. Our decision to consider only C4-C5 alkane emissions as a single lumped species produces a geographic distribution similar to observations. Due to the increasing importance of oil and gas emissions in the U.S., we recommend continued support of existing long-term measurements of C2-C5 alkanes. We suggest additional monitoring of C2-C5 alkanes downwind of northeastern Colorado, Wyoming and western North Dakota to capture changes in these regions. The atmospheric chemistry modeling community should also evaluate whether chemical mechanisms that lump larger alkanes are sufficient to understand air quality issues in regions with large emissions of these species. [less ▲]

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See detailThe influence of biomass burning on the Arctic: Pan-Arctic FTIR observations and model results
Strong, K; Lutsch, E; Conway, S et al

Poster (2018, September)

Transport of biomass burning emissions into the Arctic can cause episodic enhancements of multiple trace gas species. We present a multi-year time series of the total columns of carbon monoxide (CO ... [more ▼]

Transport of biomass burning emissions into the Arctic can cause episodic enhancements of multiple trace gas species. We present a multi-year time series of the total columns of carbon monoxide (CO), hydrogen cyanide (HCN), and ethane (C2H6) measured using Fourier Transform Infrared (FTIR) solar absorption spectroscopy at six high-latitude sites: Eureka, Nunavut; Ny Alesund, Norway; Thule, Greenland; Kiruna, Sweden; Poker Flat, Alaska; and St. Petersburg, Russia, and at three mid-latitude sites; Zugspitze, Germany; Jungfraujoch, Switzerland; and Toronto, Ontario. For each site, the inter-annual trends and seasonal variabilities of the CO total column time series are determined and enhancements above ambient levels are used to identify possible wildfire pollution events. Correlations of HCN and C2H6 with CO, back-trajectories from HYSPLIT and FLEXPART, and fire locations from the Moderate Resolution Spectroradiometer (MODIS) confirm the detections and identify the source regions. The GEOS-Chem chemical transport model is run in tagged mode to determine the relative contributions to the observed enhancements from continental-scale biomass burning source regions. Exceptional emissions of CO, HCN, C2H6, and ammonia (NH3) from the 2017 North American wildfires were measured at Eureka and Thule, indicating that wildfires may be a major source of NH3 in the summertime high Arctic. The enhancement ratios of the long-lived species HCN and C2H6 are found to be comparable between sites, but for NH3, the enhancement ratios are strongly dependent on the transport patterns of the smoke plumes. Satellite measurements of NH3 from the Infrared Atmospheric Sounding Instrument (IASI) and Cross-track Infrared Sounder (CrIS) are used to examine the spatial and temporal variabilities of NH3. Comparisons to a high-resolution (0.25° x 0.3125°) nested run of GEOS-Chem using emissions from the Global Fire Assimilation System (GFAS) are performed to evaluate the emission inventories and assess the long-range transport of NH3 to the high Arctic. [less ▲]

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See detailDetection of the long-range transport of wildfire pollution to the Arctic using a network of ground-based FTIR spectrometers, satellite observations and model results
Lutsch, E; Conway, S; Strong, K et al

Conference (2017, December 14)

We present a multi-year time series of the total columns of carbon monoxide (CO), hydrogen cyanide (HCN) and ethane (C2H6) obtained by Fourier Transform Infrared (FTIR) spectrometer measurements at nine ... [more ▼]

We present a multi-year time series of the total columns of carbon monoxide (CO), hydrogen cyanide (HCN) and ethane (C2H6) obtained by Fourier Transform Infrared (FTIR) spectrometer measurements at nine sites. Six are high-latitude sites: Eureka, Nunavut; Ny Alesund, Norway; Thule, Greenland; Kiruna, Sweden; Poker Flat, Alaska and St. Petersburg, Russia and three are mid-latitude sites; Zugspitze, Germany; Jungfraujoch, Switzerland and Toronto, Ontario. For each site, the inter-annual trends and seasonal variabilities of the CO total column time series are accounted for allowing for ambient concentrations to be determined. Enhancements above ambient levels are then used to identify possible wildfire pollution events. Since the abundance of each trace gas species emitted in a wildfire event is specific to the type of vegetation burned and the burning phase, correlations of CO to the other long-lived wildfire tracers HCN and C2H6 allow for further confirmation of the detection of wildfire pollution. Back-trajectories from HYSPLIT and FLEXPART as well as fire detections from the Moderate Resolution Spectroradiometer (MODIS) allow the source regions of the detected enhancements to be determined while satellite observations of CO from the Measurement of Pollution in the Troposphere (MOPITT) and Infrared Atmospheric Sounding Interferometer (IASI) instruments can be used to track the transport of the smoke plume. Differences in travel times between sites allows ageing of biomass burning plumes to be determined, providing a means to infer the physical and chemical processes affecting the loss of each species during transport. Comparisons of ground-based FTIR measurements to GEOS-Chem chemical transport model results are used to investigate these processes, evaluate wildfire emission inventories and infer the influence of wildfire emissions on the Arctic. [less ▲]

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See detailValidation of MOPITT carbon monoxide using ground-based Fourier transform infrared spectrometer data from NDACC
Buchholz, R. R.; Deeter, M. N.; Worden, H. M. et al

in Atmospheric Measurement Techniques (2017), 10(5), 1927--1956

The Measurements of Pollution in the Troposphere (MOPITT) satellite instrument provides the longest continuous dataset of carbon monoxide (CO) from space. We perform the first validation of MOPITT version ... [more ▼]

The Measurements of Pollution in the Troposphere (MOPITT) satellite instrument provides the longest continuous dataset of carbon monoxide (CO) from space. We perform the first validation of MOPITT version 6 retrievals using total column CO measurements from ground-based remote-sensing Fourier transform infrared spectrometers (FTSs). Validation uses data recorded at 14 stations, that span a wide range of latitudes (80°N to 78°S), in the Network for the Detection of Atmospheric Composition Change (NDACC). MOPITT measurements are spatially co-located with each station, and different vertical sensitivities between instruments are accounted for by using MOPITT averaging kernels (AKs). All three MOPITT retrieval types are analyzed: thermal infrared (TIR-only), joint thermal and near infrared (TIR–NIR), and near infrared (NIR-only). Generally, MOPITT measurements overestimate CO relative to FTS measurements, but the bias is typically less than 10%. Mean bias is 2.4% for TIR-only, 5.1% for TIR–NIR, and 6.5% for NIR-only. The TIR–NIR and NIR-only products consistently produce a larger bias and lower correlation than the TIR-only. Validation performance of MOPITT for TIR-only and TIR–NIR retrievals over land or water scenes is equivalent. The four MOPITT detector element pixels are validated separately to account for their different uncertainty characteristics. Pixel 1 produces the highest standard deviation and lowest correlation for all three MOPITT products. However, for TIR-only and TIR–NIR, the error-weighted average that includes all four pixels often provides the best correlation, indicating compensating pixel biases and well-captured error characteristics. We find that MOPITT bias does not depend on latitude but rather is influenced by the proximity to rapidly changing atmospheric CO. MOPITT bias drift has been bound geographically to within ±0.5%/yr or lower at almost all locations. [less ▲]

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See detailIdentifying long-range transport of wildfire emissions to the Arctic by a network of groundbased FTIR spectrometers, satellite observations and transport models
Lutsch, E; Conway, S; Strong, K et al

Conference (2017, June)

We present a multi-year time series of the total column amounts of carbon monoxide (CO), hydrogen cyanide (HCN) and ethane (C2H6) obtained by Fourier Transform Infrared (FTIR) spectrometer measurements at ... [more ▼]

We present a multi-year time series of the total column amounts of carbon monoxide (CO), hydrogen cyanide (HCN) and ethane (C2H6) obtained by Fourier Transform Infrared (FTIR) spectrometer measurements at ten sites. Six high-latitude sites: Eureka, Nunavut (80.02°N, 86.42°W); Ny Alesund, Norway (78.92°N, 11.93°E); Thule, Greenland (76.53°N, 68.74°W); Kiruna, Sweden (67.84°N, 20.41°E); Poker Flat, Alaska (65.11°N, 147.42°W); St. Petersburg, Russia (59.88°N, 29.83°E) and four mid-latitude sites: Bremen, Germany (53.1°N, 8.8°E); Zugspitze, Germany (47.42°N, 10.98°E); Jungfraujoch, Switzerland (46.55°N, 7.98°E) and Toronto, Ontario (43.66°N, 79.40°W). For each site, enhancements of total column amounts above seasonal means are identified and attributed to wildfire events by HYSPLIT and FLEXPART back-trajectories. Wildfire source locations are identified by the MODIS fire hot spot dataset while satellite measurements of CO total columns from IASI illustrate transport of the smoke plume and allow for further confirmation of the observed enhancement. Using the multi-year time series, inter-annual variability of wildfire events is observed. Differences in travel times of the smoke plume between sites allow for ageing of the plume to be determined providing a means to infer the physical and chemical processes affecting the loss of each species during transport. The varying lifetimes of the species and independent measurements at all sites, along with sensitivities to various source regions given by FLEXPART allow for the transport pathways to the Arctic to be investigated. By accounting for the effect of the ageing of the smoke plumes, the measured FTIR enhancement ratios are corrected to obtain emission ratios and emission factors, which are needed to improve the simulation of fire emissions in chemical transport models. [less ▲]

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See detailObservation and simulation of ethane at 22 FTIR sites
Mahieu, Emmanuel ULiege; Franco, Bruno ULiege; Pozzer, Andrea et al

Conference (2017, May 30)

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See detailRevisiting global fossil fuel and biofuel emissions of ethane
Tzompa-Sosa, Z. A.; Mahieu, Emmanuel ULiege; Franco, Bruno ULiege et al

in Journal of Geophysical Research. Atmospheres (2017), 122(4), 2493--2512

Recent measurements over the Northern Hemisphere indicate that the long-term decline in the atmospheric burden of ethane (C2H6) has ended and the abundance increased dramatically between 2010 and 2014 ... [more ▼]

Recent measurements over the Northern Hemisphere indicate that the long-term decline in the atmospheric burden of ethane (C2H6) has ended and the abundance increased dramatically between 2010 and 2014. The rise in C2H6 atmospheric abundances has been attributed to oil and natural gas extraction in North America. Existing global C2H6 emission inventories are based on outdated activity maps that do not account for current oil and natural gas exploitation regions. We present an updated global C2H6 emission inventory based on 2010 satellite-derived CH4 fluxes with adjusted C2H6 emissions over the U.S. from the National Emission Inventory (NEI 2011). We contrast our global 2010 C2H6 emission inventory with one developed for 2001. The C2H6 difference between global anthropogenic emissions is subtle (7.9 versus 7.2 Tg yr−1), but the spatial distribution of the emissions is distinct. In the 2010 C2H6 inventory, fossil fuel sources in the Northern Hemisphere represent half of global C2H6 emissions and 95% of global fossil fuel emissions. Over the U.S., unadjusted NEI 2011 C2H6 emissions produce mixing ratios that are 14–50% of those observed by aircraft observations (2008–2014). When the NEI 2011 C2H6 emission totals are scaled by a factor of 1.4, the Goddard Earth Observing System Chem model largely reproduces a regional suite of observations, with the exception of the central U.S., where it continues to underpredict observed mixing ratios in the lower troposphere. We estimate monthly mean contributions of fossil fuel C2H6 emissions to ozone and peroxyacetyl nitrate surface mixing ratios over North America of ~1% and ~8%, respectively. [less ▲]

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See detailUsing NDACC column measurements of carbonyl sulfide to estimate its sources and sinks
Wang; Marshall, J; Palm, Mathias et al

in Geophysical Research Abstracts (2016, April 19), 18

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See detailEvaluating ethane and methane emissions associated with the development of oil and natural gas extraction in North America
Franco, Bruno ULiege; Mahieu, Emmanuel ULiege; Emmons, L. K. et al

in Environmental Research Letters (2016), 11(4), 044010

Sharp rises in the atmospheric abundance of ethane (C2H6) have been detected from 2009 onwards in the Northern Hemisphere as a result of the unprecedented growth in the exploitation of shale gas and tight ... [more ▼]

Sharp rises in the atmospheric abundance of ethane (C2H6) have been detected from 2009 onwards in the Northern Hemisphere as a result of the unprecedented growth in the exploitation of shale gas and tight oil reservoirs in North America. Using time series of C2H6 total columns derived from ground-based FTIR observations made at five selected NDACC sites, we characterize the recent C2H6 evolution and determine growth rates of ~5%/yr at mid-latitudes and of ~3%/yr at remote sites. Results from CAM-chem simulations with the HTAP2 bottom-up inventory for anthropogenic emissions are found to greatly underestimate the current C2H6 abundances. Doubling global emissions is required to reconcile the simulations and the observations prior to 2009. We further estimate that North American anthropogenic C2H6 emissions have increased from 1.6 Tg/yr in 2008 to 2.8 Tg/yr in 2014, i.e. by 75% over these six years. We also completed a second simulation with new top-down emissions of C2H6 from North American oil and gas activities, biofuel consumption and biomass burning, inferred from space-borne observations of methane (CH4) from GOSAT. In this simulation, GEOS-Chem is able to reproduce FTIR measurements at the mid-latitudinal sites, underscoring the impact of the North American oil and gas development on the current C2H6 abundance. Finally we estimate that the North American oil and gas emissions of CH4, a major greenhouse gas, grew from 20 to 35 Tg/yr over the period 2008 to 2014, in association with the recent C2H6 rise. [less ▲]

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See detailTowards understanding the variability in biospheric CO2 fluxes: using FTIR spectrometry and a chemical transport model to investigate the sources and sinks of carbonyl sulfide and its link to CO2
Wang, Y.; Deutscher, N. M.; Palm, Mathias et al

in Atmospheric Chemistry and Physics (2016), 16

Understanding carbon dioxide (CO2) biospheric processes is of great importance because the terrestrial exchange drives the seasonal and interannual variability of CO2 in the atmosphere. Atmospheric ... [more ▼]

Understanding carbon dioxide (CO2) biospheric processes is of great importance because the terrestrial exchange drives the seasonal and interannual variability of CO2 in the atmosphere. Atmospheric inversions based on CO2 concentration measurements alone can only determine net biosphere fluxes, but not differentiate between photosynthesis (uptake) and respiration (production). Carbonyl sulfide (OCS) could provide an important additional constraint: it is also taken up by plants during photosynthesis but not emitted during respiration, and therefore is a potential means to differentiate between these processes. Solar absorption Fourier Transform InfraRed (FTIR) spectrometry allows for the retrievals of the atmospheric concentrations of both CO2 and OCS from measured solar absorption spectra. Here, we investigate co-located and quasi-simultaneous FTIR measurements of OCS and CO2 performed at five selected sites located in the Northern Hemisphere. These measurements are compared to simulations of OCS and CO2 using a chemical transport model (GEOS-Chem). The coupled biospheric fluxes of OCS and CO2 from the simple biosphere model (SiB) are used in the study. The CO2 simulation with SiB fluxes agrees with the measurements well, while the OCS simulation reproduced a weaker drawdown than FTIR measurements at selected sites, and a smaller latitudinal gradient in the Northern Hemisphere during growing season when comparing with HIPPO (HIAPER Pole-to-Pole Observations) data spanning both hemispheres. An offset in the timing of the seasonal cycle minimum between SiB simulation and measurements is also seen. Using OCS as a photosynthesis proxy can help to understand how the biospheric processes are reproduced in models and to further understand the carbon cycle in the real world. [less ▲]

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See detailCurrent trend in carbon tetrachloride from several NDACC FTIR stations
Hannigan, J.; Palm, Mathias; Conway, S. et al

Conference (2015, October 05)

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See detailRecent ethane increase above North America: comparison between FTIR measurements and model simulations
Franco, Bruno ULiege; Bader, Whitney ULiege; Mahieu, Emmanuel ULiege et al

Conference (2015, June 11)

Ethane (C2H6) has a large impact on tropospheric composition and air quality because of its involvement in the global VOC (volatile organic compound) – HOx – NOx chemistry responsible for generating and ... [more ▼]

Ethane (C2H6) has a large impact on tropospheric composition and air quality because of its involvement in the global VOC (volatile organic compound) – HOx – NOx chemistry responsible for generating and destroying tropospheric ozone. By acting as a major sink for tropospheric OH radicals, the abundance of C2H6 influences the atmospheric content of carbon monoxide and impacts the lifetime of methane. Moreover, it is an important source of PAN, a thermally unstable reservoir for NOx radicals. On a global scale, the main sources of C2H6 are leakage from the production, transport of natural gas loss, biofuel consumption and biomass burning, mainly located in the Northern Hemisphere. Due to its relatively long lifetime of approximately two months, C2H6 is a sensitive indicator of tropospheric pollution and transport. Using an optimized retrieval strategy (see Franco et al., 2014), we present here a 20-year long-term time series of C2H6 column abundance retrieved from ground-based Fourier Transform InfraRed (FTIR) solar spectra recorded from 1994 onwards at the high-altitude station of Jungfraujoch (Swiss Alps, 46.5° N, 3580 m a.s.l.), part of the Network for the Detection of Atmospheric Composition Change (NDACC, see http://www.ndacc.org). After a regular 1994 – 2008 decrease of the C2H6 amounts, which is very consistent with prior major studies (e.g., Aydin et al., 2011; Simpson et al., 2012) and our understanding of global C2H6 emissions, trend analysis using a bootstrap resampling tool reveals a C2H6 upturn and a statistically-significant sharp burden increase from 2009 onwards (Franco et al., 2014). We hypothesize that this observed recent increase in C2H6 could affect the whole Northern Hemisphere and may be related to the recent massive growth in the exploitation of shale gas and tight oil reservoirs. This hypothesis is supported by measurements derived from solar occultation observations performed since 2004 by the Atmospheric Chemistry Experiment – Fourier Transform Spectrometer (ACE-FTS) instrument and at other NDACC sites, namely Toronto (44° N) and Thule (77° N). Indeed, the recent rates of changes characterizing these data sets are consistent in magnitude and sign with the one derived from the FTIR measurements at Jungfraujoch. In contrast, the ethane time series form Lauder (45° S) shows a monotonic decrease over the last two decades. Investigating both the cause and impact on air quality of the C2H6 upturn should be a high priority for the atmospheric chemistry community. [less ▲]

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See detailUse of GEOS-Chem for the interpretation of long-term FTIR measurements at the Jungfraujoch and other NDACC sites
Mahieu, Emmanuel ULiege; Bovy, Benoît ULiege; Bader, Whitney ULiege et al

Poster (2015, May 04)

We present recent and ongoing investigations using 3D CTM GEOS-Chem model simulations for the interpretation of long-term FTIR measurements performed at selected NDACC sites.

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See detailRecent increase of ethane detected in the remote atmosphere of the Northern Hemisphere
Franco, Bruno ULiege; Bader, Whitney ULiege; Bovy, Benoît ULiege et al

Conference (2015, April 13)

Ethane (C2H6) has a large impact on tropospheric composition and air quality because of its involvement in the global VOC (volatile organic compound) – HOx – NOx chemistry responsible for generating and ... [more ▼]

Ethane (C2H6) has a large impact on tropospheric composition and air quality because of its involvement in the global VOC (volatile organic compound) – HOx – NOx chemistry responsible for generating and destroying tropospheric ozone. By acting as a major sink for tropospheric OH radicals, the abundance of C2H6 influences the atmospheric content of carbon monoxide and impacts the lifetime of methane. Moreover, it is an important source of PAN, a thermally unstable reservoir for NOx radicals. On a global scale, the main sources of C2H6 are leakage from the production, transport of natural gas loss, biofuel consumption and biomass burning, mainly located in the Northern Hemisphere. Due to its relatively long lifetime of approximately two months, C2H6 is a sensitive indicator of tropospheric pollution and transport. Using an optimized retrieval strategy (see Franco et al., 2014), we present here a 20-year long-term time series of C2H6 column abundance retrieved from ground-based Fourier Transform InfraRed (FTIR) solar spectra recorded from 1994 onwards at the high-altitude station of Jungfraujoch (Swiss Alps, 46.5° N, 3580 m a.s.l.), part of the Network for the Detection of Atmospheric Composition Change (NDACC, see http://www.ndacc.org). After a regular 1994 – 2008 decrease of the C2H6 amounts, which is very consistent with prior major studies (e.g., Aydin et al., 2011; Simpson et al., 2012) and our understanding of global C2H6 emissions, trend analysis using a bootstrap resampling tool reveals a C2H6 upturn and a statistically-significant sharp burden increase from 2009 onwards (Franco et al., 2014). We hypothesize that this observed recent increase in C2H6 could affect the whole Northern Hemisphere and may be related to the recent massive growth in the exploitation of shale gas and tight oil reservoirs. This hypothesis is supported by measurements derived from solar occultation observations performed since 2004 by the Atmospheric Chemistry Experiment – Fourier Transform Spectrometer (ACE-FTS) instrument and at other NDACC sites, namely Toronto (44° N) and Thule (77° N). Indeed, the recent rates of changes characterizing these data sets are consistent in magnitude and sign with the one derived from the FTIR measurements at Jungfraujoch. In contrast, the ethane time series form Lauder (45° S) shows a monotonic decrease over the last two decades. Investigating both the cause and impact on air quality of the C2H6 upturn should be a high priority for the atmospheric chemistry community. [less ▲]

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See detailValidation of ACE-FTS measurements of CFC-11, CFC-12 and HCFC-22 using ground-based FTIRs
Kolonjari, F; Walker, K A; Mahieu, Emmanuel ULiege et al

Poster (2013, December 10)

Satellite data can be an effective global monitoring tool for long-lived compounds in the atmosphere. The Atmospheric Chemistry Experiment (ACE) is a mission onboard the Canadian satellite SCISAT. The ... [more ▼]

Satellite data can be an effective global monitoring tool for long-lived compounds in the atmosphere. The Atmospheric Chemistry Experiment (ACE) is a mission onboard the Canadian satellite SCISAT. The primary instrument on SCISAT is a high-resolution infrared Fourier transform spectrometer (ACE-FTS) which is capable of measuring a range of gases including key chlorofluorocarbon (CFC) and hydrochlorofluorocarbon (HCFC) species. These families of species are of interest because of their significant contribution to anthropogenic ozone depletion and to global warming. To assess the quality of data derived from satellite measurements, validation using other data sources is critical. Ground-based Fourier transform infrared spectrometers (FTIRs) are particularly useful for this purpose. In this study, five FTIRs located at four sites around the world are used to validate the CFC-11 (CCl3F), CFC-12 (CCl2F2), and HCFC-22 (CHClF2) retrieved profiles from ACE-FTS measurements. These species are related because HCFC-22 was the primary replacement for CFC-11 and CFC-12 in refrigerant and propellant applications. The FTIRs used in this study record solar absorption spectra at Eureka (Canada), Jungfraujoch (Switzerland), Poker Flat (USA), and Toronto (Canada). The retrieval of CFC-11, CFC-12, and HCFC-22 are not standard products for many of these FTIRs, and as such, a harmonization of retrieval parameters between the sites has been conducted. The retrievals of these species from the FTIR spectra are sensitive from the surface to approximately 20 km, while the ACE-FTS profiles extend from 6 to 30 km. For each site, partial column comparisons between coincident measurements of the three species and a validation of the observed trends will be discussed. [less ▲]

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