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 ◽  
...  

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).

2015 ◽  
Vol 8 (10) ◽  
pp. 11171-11207
Author(s):  
E. M. Buzan ◽  
C. A. Beale ◽  
C. D. Boone ◽  
P. F. Bernath

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.


2006 ◽  
Vol 6 (8) ◽  
pp. 2355-2366 ◽  
Author(s):  
G. Dufour ◽  
R. Nassar ◽  
C. D. Boone ◽  
R. Skelton ◽  
K. A. Walker ◽  
...  

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.


2010 ◽  
Vol 3 (1) ◽  
pp. 51-66 ◽  
Author(s):  
R. L. Batchelor ◽  
F. Kolonjari ◽  
R. Lindenmaier ◽  
R. L. Mittermeier ◽  
W. Daffer ◽  
...  

Abstract. The Canadian Arctic Atmospheric Chemistry Experiment Validation Campaigns have been carried out at Eureka, Nunavut (80.05° N, 86.42° W) during the polar sunrise period since 2004. During the International Polar Year (IPY) springs of 2007 and 2008, three ground-based Fourier transform infrared (FTIR) spectrometers were operated simultaneously. This paper presents a comparison of trace gas measurements of stratospherically important species involved in ozone depletion, namely O3, HCl, ClONO2, HNO3 and HF, recorded with these three spectrometers. Total column densities of the gases measured with the new Canadian Network for the Detection of Atmospheric Change (CANDAC) Bruker 125HR are shown to agree to within 3.5% with the existing Environment Canada Bomem DA8 measurements. After smoothing both of these sets of measurements to account for the lower spectral resolution of the University of Waterloo Portable Atmospheric Research Interferometric Spectrometer for the Infrared (PARIS-IR), the measurements were likewise shown to agree with PARIS-IR to within 7%. Concurrent measurements of these gases were also made with the satellite-based Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) during overpasses of Eureka during these time periods. While one of the mandates of the ACE satellite mission is to study ozone depletion in the polar spring, previous validation exercises have identified the highly variable polar vortex conditions of the spring period to be a challenge for validation efforts. In this work, comparisons between the CANDAC Bruker 125HR and ACE-FTS have been used to develop strict criteria that allow the ground- and satellite-based instruments to be confidently compared. When these criteria are taken into consideration, the observed biases between the ACE-FTS and ground-based FTIR spectrometer are not persistent for both years and are generally insignificant, though small positive biases of ~5%, comparable in magnitude to those seen in previous validation exercises, are observed for HCl and HF in 2007, and negative biases of −15.3%, −4.8% and −1.5% are seen for ClONO2, HNO3 and O3 in 2008.


2006 ◽  
Vol 6 (1) ◽  
pp. 1249-1273 ◽  
Author(s):  
G. Dufour ◽  
R. Nassar ◽  
C. D. Boone ◽  
R. Skelton ◽  
K. A. Walker ◽  
...  

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.


2009 ◽  
Vol 2 (6) ◽  
pp. 2881-2917 ◽  
Author(s):  
R. L. Batchelor ◽  
F. Kolonjari ◽  
R. Lindenmaier ◽  
R. L. Mittermeier ◽  
W. Daffer ◽  
...  

Abstract. The Canadian Arctic Atmospheric Chemistry Experiment Validation Campaigns have been carried out at Eureka, Nunavut (80.05° N, 86.42° W) during the polar sunrise period since 2004. During the International Polar Year (IPY) springs of 2007 and 2008, three ground-based Fourier transform infrared (FTIR) spectrometers were operated simultaneously. This paper presents a comparison of trace gas measurements of stratospherically important species involved in ozone depletion, namely O3, HCl, ClONO2, HNO3 and HF, recorded with these three spectrometers. Total column densities of the gases measured with the new Canadian Network for the Detection of Atmospheric Change (CANDAC) Bruker 125HR are shown to agree to within 3.5% with the existing Environment Canada Bomem DA8 measurements. After smoothing both of these sets of measurements to account for the lower spectral resolution of the University of Waterloo Portable Atmospheric Research Interferometric Spectrometer for the Infrared (PARIS-IR), the measurements were likewise shown to agree with PARIS-IR to within 7%. Concurrent measurements of these gases were also made with the satellite-based Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) during overpasses of Eureka during these time periods. While one of the mandates of the ACE satellite mission is to study ozone depletion in the polar spring, previous validation exercises have identified the highly variable polar vortex conditions of the spring period to be a challenge for validation efforts. In this work, comparisons between the CANDAC Bruker 125HR and ACE-FTS have been used to develop strict criteria that allow the ground- and satellite-based instruments to be confidently compared. When these criteria are taken into consideration, there is shown to be no significant bias between the ACE-FTS and ground-based FTIR spectrometer for any of these gases.


2013 ◽  
Vol 13 (14) ◽  
pp. 6921-6950 ◽  
Author(s):  
A. T. Brown ◽  
C. M. Volk ◽  
M. R. Schoeberl ◽  
C. D. Boone ◽  
P. F. Bernath

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 & CH4 this represents the first calculation of the stratospheric lifetime using data from a space based instrument.


2009 ◽  
Vol 9 (20) ◽  
pp. 8039-8047 ◽  
Author(s):  
G. González Abad ◽  
P. F. Bernath ◽  
C. D. Boone ◽  
S. D. McLeod ◽  
G. L. Manney ◽  
...  

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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