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 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 Vertical Distribution of Arctic Methane in 2009–2018 Using Ground-Based Remote Sensing

2020 ◽  
Vol 12 (6) ◽  
pp. 917
Author(s):  
Tomi Karppinen ◽  
Otto Lamminpää ◽  
Simo Tukiainen ◽  
Rigel Kivi ◽  
Pauli Heikkinen ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Vertical Distribution ◽  
Atmospheric Chemistry ◽  
Polar Vortex ◽  
The Arctic ◽  
Fourier Transform Spectrometer ◽  
Atmospheric Methane ◽  
The Vertical Distribution ◽  
Chemistry Experiment

We analyzed the vertical distribution of atmospheric methane (CH 4 ) retrieved from measurements by ground-based Fourier Transform Spectrometer (FTS) instrument in Sodankylä, Northern Finland. The retrieved dataset covers 2009–2018. We used a dimension reduction retrieval method to extract the profile information, since each measurement contains around three pieces of information about the profile shape between 0 and 40 km. We compared the retrieved profiles against Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) satellite measurements and AirCore balloon-borne profile measurements. Additional comparison at the lowest tropospheric layer was done against in-situ measurements from a 50-m-high mast. In general, the ground-based FTS and ACE-FTS profiles agreed within 10% below 20 km and within 30% in the stratosphere between 20 and 40 km. Our method was able to accurately capture reduced methane concentrations inside the polar vortex in the Arctic stratosphere. The method produced similar trend characteristics as the reference instruments even when a static prior profile was used. Finally, we analyzed the time series of the CH 4 profile datasets and estimated the trend using the dynamic linear model (DLM).

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 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 Stratospheric lifetimes of CFC-12, CCl<sub>4</sub>, CH<sub>4</sub>, CH<sub>3</sub>Cl and N<sub>2</sub>O from measurements made by the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS)

2013 ◽  
Vol 13 (14) ◽  
pp. 6921-6950 ◽  
Author(s):  
A. T. Brown ◽  
C. M. Volk ◽  
M. R. Schoeberl ◽  
C. D. Boone ◽  
P. F. Bernath
Keyword(s):  
Fourier Transform ◽  
Atmospheric Chemistry ◽  
Linear Trend ◽  
Systematic Errors ◽  
Fourier Transform Spectrometer ◽  
Atmospheric Gases ◽  
Chlorine Radicals ◽  
Using Data ◽  
Long Term Impact ◽  
Chemistry Experiment

Abstract. Long lived halogen-containing compounds are important atmospheric constituents since they can act both as a source of chlorine radicals, which go on to catalyse ozone loss, and as powerful greenhouse gases. The long-term impact of these species on the ozone layer is dependent on their stratospheric lifetimes. Using observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) we present calculations of the stratospheric lifetimes of CFC-12, CCl4, CH4, CH3Cl and N2O. The lifetimes were calculated using the slope of the tracer–tracer correlation of these species with CFC-11 at the tropopause. The correlation slopes were corrected for the changing atmospheric concentrations of each species based on age of air and CFC-11 measurements from samples taken aboard the Geophysica aircraft – along with the effective linear trend of the volume mixing ratio (VMR) from tropical ground based AGAGE (Advanced Global Atmospheric Gases Experiment) sites. Stratospheric lifetimes were calculated using a CFC-11 lifetime of 45 yr. These calculations produced values of 113 + (−) 26 (18) yr (CFC-12), 35 + (−) 11 (7) yr (CCl4), 69 + (−) 65 (23) yr (CH3Cl), 123 + (−) 53 (28) yr (N2O) and 195 + (−) 75 (42) yr (CH4). The errors on these values are the weighted 1σ non-systematic errors. Systematic errors were estimated by recalculating lifetimes using VMRs which had been modified to reflect differences between ACE-FTS retrieved VMRs and those from other instruments. The results of these calculations, including systematic errors, were as follows: 113 + (−) 32 (20) for CFC-12, 123 + (−) 83 (35) for N2O, 195 + (−) 139 (57) for CH4, 35 + (−) 14 (8) for CCl4 and 69 + (−) 2119 (34) yr for CH3Cl. For CH3Cl &amp; CH4 this represents the first calculation of the stratospheric lifetime using data from a space based instrument.

scholarly journals Global distribution of upper tropospheric formic acid from the ACE-FTS

2009 ◽  
Vol 9 (20) ◽  
pp. 8039-8047 ◽  
Author(s):  
G. González Abad ◽  
P. F. Bernath ◽  
C. D. Boone ◽  
S. D. McLeod ◽  
G. L. Manney ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Formic Acid ◽  
Atmospheric Chemistry ◽  
South American ◽  
Fourier Transform Spectrometer ◽  
Vegetation Growth ◽  
Solar Occultation ◽  
The Fourier Transform ◽  
Chemistry Experiment ◽  
Seasonal Dependence

Abstract. We present the first near global upper tropospheric distribution of formic acid (HCOOH) observed from space using solar occultation measurements from the Fourier transform spectrometer (FTS) on board the Atmospheric Chemistry Experiment (ACE) satellite. Using a new set of spectroscopic line parameters recently published for formic acid by Vander Auwera et al. (2007) and Perrin and Vander Auwera (2007), we have retrieved the concentrations of HCOOH between 5 km and the tropopause for ACE-FTS observations from February 2004 to September 2007. We observe a significant seasonal dependence for the HCOOH concentrations related to vegetation growth and biomass burning. We estimate an emission ratio of 0.0051±0.0015 for HCOOH relative to CO for tropical South American fires using a selected set of data for September 2004. Results from the balloon-borne MkIV Fourier transform spectrometer are also presented and compared with the ACE measurements.

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