scholarly journals Observations of peroxyacetyl nitrate (PAN) in the upper troposphere by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS)

2013 ◽  
Vol 13 (1) ◽  
pp. 1575-1607 ◽  
Author(s):  
K. A. Tereszchuk ◽  
D. P. Moore ◽  
J. J. Harrison ◽  
C. D. Boone ◽  
M. Park ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Biomass Burning ◽  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Fourier Transform Spectrometer ◽  
Data Set ◽  
Upper Troposphere ◽  
Volatile Organic ◽  
The Impact ◽  
Chemistry Experiment

Abstract. Peroxyacetyl nitrate (CH3CO·O2NO2, abbreviated as PAN) is a trace molecular species present in the troposphere and lower stratosphere due primarily to pollution from fuel combustion and the pyrogenic outflows from biomass burning. In the lower troposphere, PAN has a relatively short life-time and is principally destroyed within a few hours through thermolysis, but it can act as a reservoir and carrier of NOx in the colder temperatures of the upper troposphere where UV photolysis becomes the dominant loss mechanism. Pyroconvective updrafts from large biomass burning events can inject PAN into the upper troposphere and lower stratosphere (UTLS), providing a means for the long-range transport of NOx. Given the extended lifetimes at these higher altitudes, PAN is readily detectable via satellite remote sensing. A new PAN data product is now available for the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) Version 3.0 data set. We report measurements of PAN in Boreal biomass burning plumes recorded during the Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites (BORTAS) campaign. The retrieval method employed and errors analysis are described in full detail. The retrieved volume mixing ratio (VMR) profiles are compared to coincident measurements made by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument on the European Space Agency (ESA) ENVIronmental SATellite (ENVISAT). Three ACE-FTS occultations containing measurements of Boreal biomass burning outflows, recorded during BORTAS, were identified as having coincident measurements with MIPAS. In each case, the MIPAS measurements demonstrated good agreement with the ACE-FTS VMR profiles for PAN. The ACE-FTS PAN data set is used to obtain zonal mean distributions of seasonal averages from ~5 to 20 km. A strong seasonality is clearly observed for PAN concentrations in the global UTLS. Since the principal source of PAN in the UTLS is due to lofted biomass burning emissions from the pyroconvective updrafts created by large fires, the observed seasonality in enhanced PAN coincides with fire activity in different geographical regions throughout the year. This work is part of an in-depth investigation that is being conducted in an effort to study the aging and chemical evolution of biomass burning emissions in the UTLS by remote, space-borne measurements made by ACE-FTS to further our understanding of the impact of pyrogenic emissions on atmospheric chemistry. Included in this study will be the addition of new, pyrogenic, volatile organic hydrocarbons (VOCs) and oxygenated volatile organic compounds (OVOCs) to expand upon the already extensive suite of molecules retrieved by ACE-FTS to aid in elucidating biomass burning plume chemistry in the free troposphere.

scholarly journals Observations of peroxyacetyl nitrate (PAN) in the upper troposphere by the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS)

2013 ◽  
Vol 13 (11) ◽  
pp. 5601-5613 ◽  
Author(s):  
K. A. Tereszchuk ◽  
D. P. Moore ◽  
J. J. Harrison ◽  
C. D. Boone ◽  
M. Park ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Biomass Burning ◽  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Full Detail ◽  
Fourier Transform Spectrometer ◽  
Peroxyacetyl Nitrate ◽  
Data Set ◽  
Upper Troposphere ◽  
Chemistry Experiment

Abstract. Peroxyacetyl nitrate (CH3CO·O2NO2, abbreviated as PAN) is a trace molecular species present in the troposphere and lower stratosphere due primarily to pollution from fuel combustion and the pyrogenic outflows from biomass burning. In the lower troposphere, PAN has a relatively short lifetime and is principally destroyed within a few hours through thermolysis, but it can act as a reservoir and carrier of NOx in the colder temperatures of the upper troposphere, where UV photolysis becomes the dominant loss mechanism. Pyroconvective updrafts from large biomass burning events can inject PAN into the upper troposphere and lower stratosphere (UTLS), providing a means for the long-range transport of NOx. Given the extended lifetimes at these higher altitudes, PAN is readily detectable via satellite remote sensing. A new PAN data product is now available for the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) version 3.0 data set. We report observations of PAN in boreal biomass burning plumes recorded during the BORTAS (quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) campaign (12 July to 3 August 2011). The retrieval method employed by incorporating laboratory-recorded absorption cross sections into version 3.0 of the ACE-FTS forward model and retrieval software is described in full detail. The estimated detection limit for ACE-FTS PAN is 5 pptv, and the total systematic error contribution to the ACE-FTS PAN retrieval is ~ 16%. The retrieved volume mixing ratio (VMR) profiles are compared to coincident measurements made by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument on the European Space Agency (ESA) Environmental Satellite (ENVISAT). The MIPAS measurements demonstrated good agreement with the ACE-FTS VMR profiles for PAN, where the measured VMR values are well within the associated measurement errors for both instruments and comparative measurements differ no more than 70 pptv. The ACE-FTS PAN data set is used to obtain zonal mean distributions of seasonal averages from ~ 5–20 km. A strong seasonality is clearly observed for PAN concentrations in the global UTLS. Since the principal source of PAN in the UTLS is due to lofted biomass burning emissions from the pyroconvective updrafts created by large fires, the observed seasonality in enhanced PAN coincides with fire activity in different geographical regions throughout the year.

scholarly journals Partitioning between the inorganic chlorine reservoirs HCl and ClONO<sub>2</sub> during the Arctic winter 2005 from the ACE-FTS

2006 ◽  
Vol 6 (8) ◽  
pp. 2355-2366 ◽  
Author(s):  
G. Dufour ◽  
R. Nassar ◽  
C. D. Boone ◽  
R. Skelton ◽  
K. A. Walker ◽  
...  
Keyword(s):  
Fourier Transform ◽  
High Resolution ◽  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
The Arctic ◽  
Fourier Transform Spectrometer ◽  
Cold Winter ◽  
Winter Conditions ◽  
Reservoir Species ◽  
Chemistry Experiment

Abstract. From January to March 2005, the Atmospheric Chemistry Experiment high resolution Fourier transform spectrometer (ACE-FTS) on SCISAT-1 measured many of the changes occurring in the Arctic (50–80° N) lower stratosphere under very cold winter conditions. Here we focus on the partitioning between the inorganic chlorine reservoirs HCl and ClONO2 and their activation into ClO. The simultaneous measurement of these species by the ACE-FTS provides the data needed to follow chlorine activation during the Arctic winter and the recovery of the Cl-reservoir species ClONO2 and HCl. The time evolution of HCl, ClONO2 and ClO as well as the partitioning between the two reservoir molecules agrees well with previous observations and with our current understanding of chlorine activation during Arctic winter. The results of a chemical box model are also compared with the ACE-FTS measurements and are generally consistent with the measurements.

scholarly journals Validation of ACE-FTS v2.2 methane profiles from the upper troposphere to lower mesosphere

2007 ◽  
Vol 7 (6) ◽  
pp. 17975-18014 ◽  
Author(s):  
M. De Mazière ◽  
C. Vigouroux ◽  
P. F. Bernath ◽  
P. Baron ◽  
T. Blumenstock ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Remote Sensing Data ◽  
Upper Troposphere ◽  
Solar Occultation ◽  
Systematic Uncertainties ◽  
Comparison Results ◽  
Key Species ◽  
Chemistry Experiment

Abstract. The ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) solar occultation instrument that was launched onboard the Canadian SCISAT-1 satellite in August 2003 is measuring vertical profiles from the upper troposphere to the lower mesosphere for a large number of atmospheric constituents. Methane is one of the key species. The version v2.2 data of the ACE-FTS CH4 data have been compared to correlative satellite, balloon-borne and ground-based Fourier transform infrared remote sensing data to assess their quality. The comparison results indicate that the accuracy of the data is within 10% in the upper troposphere – lower stratosphere, and within 25% in the middle and higher stratosphere up to the lower mesosphere (<60 km). The observed differences are generally consistent with reported systematic uncertainties. ACE-FTS is also shown to reproduce the variability of methane in the stratosphere and lower mesosphere.

scholarly journals Technical Note: A trace gas climatology derived from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) data set

2012 ◽  
Vol 12 (11) ◽  
pp. 5207-5220 ◽  
Author(s):  
A. Jones ◽  
K. A. Walker ◽  
J. J. Jin ◽  
J. R. Taylor ◽  
C. D. Boone ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Atmospheric Chemistry ◽  
Climate Model ◽  
Chemical Species ◽  
Technical Note ◽  
Fourier Transform Spectrometer ◽  
Monthly Basis ◽  
Data Set ◽  
Individual Profiles ◽  
Chemistry Experiment

Abstract. The Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS) aboard the Canadian satellite SCISAT (launched in August 2003) was designed to investigate the composition of the upper troposphere, stratosphere, and mesosphere. ACE-FTS utilizes solar occultation to measure temperature and pressure as well as vertical profiles of over thirty chemical species including O3, H2O, CH4, N2O, CO, NO, NO2, N2O5, HNO3, HCl, ClONO2, CCl3F, CCl2F2, and HF. Global coverage for each species is obtained approximately over a three month period and measurements are made with a vertical resolution of typically 3–4 km. A quality-controlled climatology has been created for each of these 14 baseline species, where individual profiles are averaged over the period of February 2004 to February 2009. Measurements used are from the ACE-FTS version 2.2 data set including updates for O3 and N2O5. The climatological fields are provided on a monthly and three-monthly basis (DJF, MAM, JJA, SON) at 5 degree latitude and equivalent latitude spacing and on 28 pressure surfaces (26 of which are defined by the Stratospheric Processes And their Role in Climate (SPARC) Chemistry-Climate Model Validation Activity). The ACE-FTS climatological data set is available through the ACE website.

scholarly journals Partitioning between the inorganic chlorine reservoirs HCl and ClONO<sub>2</sub> during the Arctic winter 2005 from the ACE-FTS

2006 ◽  
Vol 6 (1) ◽  
pp. 1249-1273 ◽  
Author(s):  
G. Dufour ◽  
R. Nassar ◽  
C. D. Boone ◽  
R. Skelton ◽  
K. A. Walker ◽  
...  
Keyword(s):  
Fourier Transform ◽  
High Resolution ◽  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
The Arctic ◽  
Fourier Transform Spectrometer ◽  
Cold Winter ◽  
Winter Conditions ◽  
Reservoir Species ◽  
Chemistry Experiment

Abstract. From January to March 2005, the Atmospheric Chemistry Experiment high resolution Fourier transform spectrometer (ACE-FTS) on SCISAT-1 measured many of the changes occurring in the Arctic (50–80° N) lower stratosphere under very cold winter conditions. Here we focus on the partitioning between the inorganic chlorine reservoirs HCl and ClONO2 and their activation into ClO. The simultaneous measurement of these species by the ACE-FTS provides the data needed to follow chlorine activation during the Arctic winter and the recovery of the Cl-reservoir species ClONO2 and HCl. The time evolution of HCl, ClONO2 and ClO as well as the partitioning between the two reservoir molecules agrees well with previous observations and with our current understanding of chlorine activation during Arctic winter. The results of a chemical box model are also compared with the ACE-FTS measurements and are generally consistent with the measurements.

scholarly journals Validation of ACE-FTS v2.2 methane profiles from the upper troposphere to the lower mesosphere

2008 ◽  
Vol 8 (9) ◽  
pp. 2421-2435 ◽  
Author(s):  
M. De Mazière ◽  
C. Vigouroux ◽  
P. F. Bernath ◽  
P. Baron ◽  
T. Blumenstock ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Remote Sensing Data ◽  
Upper Troposphere ◽  
Solar Occultation ◽  
Systematic Uncertainties ◽  
Comparison Results ◽  
Key Species ◽  
Chemistry Experiment

Abstract. The ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) solar occultation instrument that was launched onboard the Canadian SCISAT-1 satellite in August 2003 is measuring vertical profiles from the upper troposphere to the lower mesosphere for a large number of atmospheric constituents. Methane is one of the key species. The version v2.2 data of the ACE-FTS CH4 data have been compared to correlative satellite, balloon-borne and ground-based Fourier transform infrared remote sensing data to assess their quality. The comparison results indicate that the accuracy of the data is within 10% in the upper troposphere – lower stratosphere, and within 25% in the middle and higher stratosphere up to the lower mesosphere (<60 km). The observed differences are generally consistent with reported systematic uncertainties. ACE-FTS is also shown to reproduce the variability of methane in the stratosphere and lower mesosphere.

scholarly journals Technical Note: A trace gas climatology derived from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer dataset

2011 ◽  
Vol 11 (11) ◽  
pp. 29845-29882 ◽  
Author(s):  
A. Jones ◽  
K. A. Walker ◽  
J. J. Jin ◽  
J. R. Taylor ◽  
C. D. Boone ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Atmospheric Chemistry ◽  
Climate Model ◽  
Chemical Species ◽  
Technical Note ◽  
Fourier Transform Spectrometer ◽  
Monthly Basis ◽  
Data Set ◽  
Individual Profiles ◽  
Chemistry Experiment

Abstract. The Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS) aboard the Canadian satellite SCISAT (launched in August 2003) was designed to investigate the composition of the upper troposphere, stratosphere, and mesosphere. ACE-FTS utilizes solar occultation to measure temperature and pressure as well as vertical profiles of over thirty chemical species including O3, H2O, CH4, N2O, CO, NO, NO2, N2O5, HNO3, HCl, ClONO2, CCl3F, CCl2F2, and HF. Global coverage for each species is obtained approximately over a three month period and measurements are made with a vertical resolution of typically 3–4 km. A quality-controlled climatology has been created for each of these 14 baseline species, where individual profiles are averaged over the period of February 2004 to February 2009. Measurements used are from the ACE-FTS version 2.2 data set including updates for O3 and N2O5. The climatological fields are provided on a monthly and three-monthly basis (DJF, MAM, JJA, SON) at 5 degree latitude and equivalent latitude spacing and on 28 pressure surfaces (26 of which are defined by the Stratospheric Processes And their Role in Climate (SPARC) Chemistry Climate Model validation activity). The ACE-FTS climatological dataset is available through the ACE website.

scholarly journals Global stratospheric measurements of the isotopologues of methane from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer

2015 ◽  
Vol 8 (10) ◽  
pp. 11171-11207
Author(s):  
E. M. Buzan ◽  
C. A. Beale ◽  
C. D. Boone ◽  
P. F. Bernath
Keyword(s):  
Fourier Transform ◽  
Atmospheric Chemistry ◽  
Climate Model ◽  
Fourier Transform Spectrometer ◽  
Atmospheric Methane ◽  
Community Climate Model ◽  
Atmospheric Sinks ◽  
Chemistry Experiment ◽  
Methane Concentrations ◽  
Balloon Measurements

Abstract. This paper presents an analysis of observations of methane and its two major isotopologues, CH3D and 13CH4 from the Atmospheric Chemistry Experiment (ACE) satellite between 2004 and 2013. Additionally, atmospheric methane chemistry is modeled using the Whole Atmospheric Community Climate Model (WACCM). ACE retrievals of methane extend from 6 km for all isotopologues to 75 km for 12CH4, 35 km for CH3D, and 50 km for 13CH4. While total methane concentrations retrieved from ACE agree well with the model, values of δD–CH4 and δ13C–CH4 show a bias toward higher δ compared to the model and balloon-based measurements. Calibrating δD and δ13C from ACE using WACCM in the troposphere gives improved agreement in δD in the stratosphere with the balloon measurements, but values of δ13C still disagree. A model analysis of methane's atmospheric sinks is also performed.

scholarly journals CO measurements from the ACE-FTS satellite instrument: data analysis and validation using ground-based, airborne and spaceborne observations

2008 ◽  
Vol 8 (9) ◽  
pp. 2569-2594 ◽  
Author(s):  
C. Clerbaux ◽  
M. George ◽  
S. Turquety ◽  
K. A. Walker ◽  
B. Barret ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Atmospheric Chemistry ◽  
Measurement Data ◽  
Upper Troposphere ◽  
Remote Sensors ◽  
Key Species ◽  
Vibrational Bands ◽  
Good Tracer ◽  
Chemistry Experiment ◽  
Better Than

Abstract. The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Carbon monoxide (CO), a good tracer of pollution plumes and atmospheric dynamics, is one of the key species provided by the primary instrument, the ACE-Fourier Transform Spectrometer (ACE-FTS). This instrument performs measurements in both the CO 1-0 and 2-0 ro-vibrational bands, from which vertically resolved CO concentration profiles are retrieved, from the mid-troposphere to the thermosphere. This paper presents an updated description of the ACE-FTS version 2.2 CO data product, along with a comprehensive validation of these profiles using available observations (February 2004 to December 2006). We have compared the CO partial columns with ground-based measurements using Fourier transform infrared spectroscopy and millimeter wave radiometry, and the volume mixing ratio profiles with airborne (both high-altitude balloon flight and airplane) observations. CO satellite observations provided by nadir-looking instruments (MOPITT and TES) as well as limb-viewing remote sensors (MIPAS, SMR and MLS) were also compared with the ACE-FTS CO products. We show that the ACE-FTS measurements provide CO profiles with small retrieval errors (better than 5% from the upper troposphere to 40 km, and better than 10% above). These observations agree well with the correlative measurements, considering the rather loose coincidence criteria in some cases. Based on the validation exercise we assess the following uncertainties to the ACE-FTS measurement data: better than 15% in the upper troposphere (8–12 km), than 30% in the lower stratosphere (12–30 km), and than 25% from 30 to 100 km.

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