ALBERT

Description: An intercomparison of ozone total column measurements derived from various platforms is presented in this work. Satellite data from Infrared Atmospheric Sounding Interferometer (IASI), Ozone Monitoring Instrument (OMI) and Global Ozone Monitoring Experiment (GOME-2) are compared with data from two ground-based spectrometers (Fourier Transform Infrared spectrometer FTIR and Brewer), located at the Network for Detection of Atmospheric Composition Change (NDACC) super-site of Izaña (Tenerife), measured during a campaign from March to June 2009. These ground-based observing systems have already been demonstrated to perform consistent, precise and accurate ozone total column measurements. An excellent agreement between ground-based and OMI/GOME-2 data is observed. Results from two different algorithms for deriving IASI ozone total column are also compared: the European Organisation for the Exploitation of Meteorological Satellites (EUMETSAT/ESA) operational algorithm and the LISA (Laboratoire Interuniversitaire des Systèmes Atmosphériques) algorithm. A better agreement was found with LISA's analytical approach based on an altitude-dependent Tikhonov-Philips regularization: correlations are 0.94 and 0.89 compared to FTIR and Brewer, respectively; while the operational IASI ozone columns (based on neural network analysis) show correlations of 0.90 and 0.85, respectively, compared to the O3 columns obtained from FTIR and Brewer.

Description: Ground-based Fourier-transform infrared (FTIR) solar absorption spectroscopy is a powerful remote sensing technique providing information on the vertical distribution of various atmospheric constituents. This work presents the first evaluation of a mid-resolution ground-based FTIR to measure tropospheric ozone, independently of stratospheric ozone. This is demonstrated using a new atmospheric observatory (named OASIS for "Observations of the Atmosphere by Solar absorption Infrared Spectroscopy"), installed in Créteil (France). Indeed, the information content of OASIS ozone retrievals is clearly sufficient to monitor separately tropospheric (from the surface up to 8 km) and stratospheric ozone. Daily mean tropospheric ozone columns derived from the Infrared Atmospheric Sounding Interferometer (IASI) and from OASIS measurements have been compared for summer 2009 and a good agreement of −5.6 (±16.1) % is observed. Also, a qualitative comparison between in-situ surface ozone measurements and OASIS data clearly shows OASIS's capacity to monitor seasonal tropospheric ozone variations, as well as ozone pollution episodes in summer 2009 around Paris. Two extreme pollution events were identified (on the 1 July and 6 August 2009) for which ozone partial columns from OASIS and predictions from a regional air-quality model (CHIMERE) were compared by respecting temporal and spatial coincidence criteria. Quantitatively, an average bias of 0.2 %, a mean square error deviation of 7.6 %, and a correlation coefficient of 0.91 was found between CHIMERE and OASIS. This demonstrates that a mid-resolution FTIR instrument in ground-based solar absorption geometry is a promising technique for monitoring tropospheric ozone.

Description: We investigate Arctic tropospheric composition using ground-based Fourier Transform Infrared (FTIR) solar absorption spectra, recorded at the Polar Environment Atmospheric Research Laboratory (PEARL, Eureka, Nunavut, Canada, 80°5' N, 86°42' W) and at Thule (Greenland, 76°53' N, −68°74' W) from 2008 to 2012. The target species: carbon monoxide (CO), hydrogen cyanide (HCN), ethane (C2H6), acetylene (C2H2), formic acid (HCOOH), and formaldehyde (H2CO) are emitted by biomass burning and can be transported from mid-latitudes to the Arctic. By detecting simultaneous enhancements of three biomass burning tracers (HCN, CO, and C2H6), ten and eight fire events are identified at Eureka and Thule, respectively, within the five-year FTIR timeseries. Analyses of Hybrid Single Particle Lagrangian Integrated Trajectory Model (HYSPLIT) back-trajectories coupled with Moderate Resolution Imaging Spectroradiometer (MODIS) fire hot spot data, Stochastic Time-Inverted Lagrangian Transport model (STILT) footprints, and Ozone Monitoring Instrument (OMI) UV aerosol index maps are used to attribute burning source regions and travel time durations of the plumes. By taking into account the effect of aging of the smoke plumes, measured FTIR enhancement ratios were corrected to obtain emission ratios and equivalent emission factors. The means of emission factors for extratropical forest estimated with the two FTIR datasets are 0.39 ± 0.15 g kg−1 for HCN, 1.23 ± 0.49 g kg−1 for C2H6, 0.34 ± 0.16 g kg−1 for C2H2, 2.13 ± 0.92 g kg−1 for HCOOH, and 3.14 ± 1.28 g kg−1 for CH3OH. To improve our knowledge concerning the dynamical and chemical processes associated with Arctic pollution from fires, the two sets of FTIR measurements were compared to the Model for Ozone and Related chemical Tracers, version 4 (MOZART-4). Seasonal cycles and day-to-day variabilities were compared to assess the ability of the model to reproduce emissions from fires and their transport. Good agreement in winter confirms that transport is well implemented in the model. For C2H6, however, the lower wintertime concentration estimated by the model as compared to the FTIR observations highlight an underestimation of its emission. Results show that modelled and measured total columns are correlated (linear correlation coefficient r 〉 0.6 for all gases except for H2CO at Eureka and HCOOH at Thule), but suggest a~general underestimation of the concentrations in the model for all seven tropospheric species in the high Arctic.

Description: We present a five-year timeseries of seven tropospheric species measured using a ground-based Fourier Transform InfraRed (FTIR) spectrometer at the Polar Environment Atmospheric Research Laboratory (PEARL, Eureka, Nunavut, Canada, 80°05' N, 86°42' W) from 2007 to 2011. Total columns and temporal variabilities of carbon monoxide (CO), hydrogen cyanide (HCN), and ethane (C2H6), as well as the first derived total columns at Eureka of acetylene (C2H2), methanol (CH3OH), formic acid (HCOOH), and formaldehyde (H2CO) are investigated, providing a new dataset in the sparsely sampled high latitudes. Total columns are obtained using the SFIT2 retrieval algorithm based on the Optimal Estimation Method. The microwindows, as well as the a priori profiles and variabilities are selected to optimize the information content of the retrievals, and error analyses are performed for all seven species. Our retrievals show good sensitivities in the troposphere. The seasonal amplitudes of the timeseries, ranging from 34 to 104%, are captured while using a single a priori profile for each species. The timeseries of the CO, C2H6 and C2H2 total columns at PEARL exhibit strong seasonal cycles with maxima in winter and minima in summer, in opposite phase to the HCN, CH3OH, HCOOH and H2CO timeseries. These cycles result from the relative contributions of the photochemistry, oxidation, and transport, as well as biogenic and biomass burning emissions. Comparisons of the FTIR partial columns with coincident satellite measurements by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) show good agreement. The correlation coefficients and the slopes range from 0.56 to 0.97, and 0.50 to 3.35, respectively, for the seven target species. Our new dataset is compared with previous measurements found in the literature to assess atmospheric budgets of these tropospheric species in the high Arctic. The CO and C2H6 concentrations are consistent with negative trends observed over the Northern Hemisphere, attributed to fossil fuel emission decrease. The importance of poleward transport on the atmospheric budgets of HCN and C2H2 is highlighted. Columns and variabilities of CH3OH, and HCOOH at PEARL are comparable to previous measurements performed at other remote sites. However, the small columns of H2CO in early May might reflect its large atmospheric variability, and/or the effect of the updated spectroscopic parameters used in our retrievals. Overall, emissions from biomass burning contribute to the day-to-day variabilities of the seven tropospheric species observed at Eureka.

Description: An intercomparison of ozone total column measurements derived from various platforms is presented in this work. Satellite data from Infrared Atmospheric Sounding Interferometer (IASI), Ozone Monitoring Instrument (OMI) and Global Ozone Monitoring Experiment (GOME-2) are compared with data from two ground-based spectrometers (Fourier Transform Infrared spectrometer FTIR and Brewer), located at the Network for Detection of Atmospheric Composition Change (NDACC) super-site of Izaña (Tenerife), measured during a campaign from March to June 2009. These ground-based observing systems have already been demonstrated to perform consistent, precise and accurate ozone total column measurements. An excellent agreement between ground-based and OMI/GOME-2 data is observed. Results from two different algorithms for deriving IASI ozone total column are also compared: the European Organisation for the Exploitation of Meteorological Satellites (EUMETSAT/ESA) operational algorithm and the LISA (Laboratoire Inter-universitaire des Systèmes Atmosphériques) algorithm. A better agreement was found with LISA's analytical approach based on an altitude-dependent Tikhonov-Philips regularization: correlations are 0.94 and 0.89 compared to FTIR and Brewer, respectively; while the operational IASI ozone columns (based on neural network analysis) show correlations of 0.90 and 0.85, respectively, compared to the O3 columns obtained from FTIR and Brewer.

Description: Ground-based Fourier-transform infrared (FTIR) solar absorption spectroscopy is a powerful remote sensing technique providing information on the vertical distribution of various atmospheric constituents. This work presents the first evaluation of a mid-resolution ground-based FTIR to measure tropospheric ozone, independently of stratospheric ozone. This is demonstrated using a new atmospheric observatory (named OASIS for "Observations of the Atmosphere by Solar absorption Infrared Spectroscopy"), installed in Créteil (France). The capacity of the technique to separate stratospheric and tropospheric ozone is demonstrated. Daily mean tropospheric ozone columns derived from the Infrared Atmospheric Sounding Interferometer (IASI) and from OASIS measurements are compared for summer 2009 and a good agreement of −5.6 (±16.1) % is observed. Also, a qualitative comparison between in-situ surface ozone measurements and OASIS data reveals OASIS's capacity to monitor seasonal tropospheric ozone variations, as well as ozone pollution episodes in summer 2009 around Paris. Two extreme pollution events are identified (on the 1 July and 6 August 2009) for which ozone partial columns from OASIS and predictions from a regional air-quality model (CHIMERE) are compared following strict criteria of temporal and spatial coincidence. An average bias of 0.2%, a mean square error deviation of 7.6%, and a correlation coefficient of 0.91 is found between CHIMERE and OASIS, demonstrating the potential of a mid-resolution FTIR instrument in ground-based solar absorption geometry for tropospheric ozone monitoring.

Description: We present a five-year time series of seven tropospheric species measured using a ground-based Fourier transform infrared (FTIR) spectrometer at the Polar Environment Atmospheric Research Laboratory (PEARL; Eureka, Nunavut, Canada; 80°05' N, 86°42' W) from 2007 to 2011. Total columns and temporal variabilities of carbon monoxide (CO), hydrogen cyanide (HCN) and ethane (C2H6) as well as the first derived total columns at Eureka of acetylene (C2H2), methanol (CH3OH), formic acid (HCOOH) and formaldehyde (H2CO) are investigated, providing a new data set in the sparsely sampled high latitudes. Total columns are obtained using the SFIT2 retrieval algorithm based on the optimal estimation method. The microwindows as well as the a priori profiles and variabilities are selected to optimize the information content of the retrievals, and error analyses are performed for all seven species. Our retrievals show good sensitivities in the troposphere. The seasonal amplitudes of the time series, ranging from 34 to 104%, are captured while using a single a priori profile for each species. The time series of the CO, C2H6 and C2H2 total columns at PEARL exhibit strong seasonal cycles with maxima in winter and minima in summer, in opposite phase to the HCN, CH3OH, HCOOH and H2CO time series. These cycles result from the relative contributions of the photochemistry, oxidation and transport as well as biogenic and biomass burning emissions. Comparisons of the FTIR partial columns with coincident satellite measurements by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) show good agreement. The correlation coefficients and the slopes range from 0.56 to 0.97 and 0.50 to 3.35, respectively, for the seven target species. Our new data set is compared to previous measurements found in the literature to assess atmospheric budgets of these tropospheric species in the high Arctic. The CO and C2H6concentrations are consistent with negative trends observed over the Northern Hemisphere, attributed to fossil fuel emission decrease. The importance of poleward transport for the atmospheric budgets of HCN and C2H2 is highlighted. Columns and variabilities of CH3OH and HCOOH at PEARL are comparable to previous measurements performed at other remote sites. However, the small columns of H2CO in early May might reflect its large atmospheric variability and/or the effect of the updated spectroscopic parameters used in our retrievals. Overall, emissions from biomass burning contribute to the day-to-day variabilities of the seven tropospheric species observed at Eureka.

Description: We investigate Arctic tropospheric composition using ground-based Fourier transform infrared (FTIR) solar absorption spectra, recorded at the Polar Environment Atmospheric Research Laboratory (PEARL, Eureka, Nunavut, Canada, 80°05' N, 86°42' W) and at Thule (Greenland, 76°53' N, −68°74' W) from 2008 to 2012. The target species, carbon monoxide (CO), hydrogen cyanide (HCN), ethane (C2H6), acetylene (C2H2), formic acid (HCOOH), and formaldehyde (H2CO) are emitted by biomass burning and can be transported from mid-latitudes to the Arctic. By detecting simultaneous enhancements of three biomass burning tracers (HCN, CO, and C2H6), ten and eight fire events are identified at Eureka and Thule, respectively, within the 5-year FTIR time series. Analyses of Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model back-trajectories coupled with Moderate Resolution Imaging Spectroradiometer (MODIS) fire hotspot data, Stochastic Time-Inverted Lagrangian Transport (STILT) model footprints, and Ozone Monitoring Instrument (OMI) UV aerosol index maps, are used to attribute burning source regions and travel time durations of the plumes. By taking into account the effect of aging of the smoke plumes, measured FTIR enhancement ratios were corrected to obtain emission ratios and equivalent emission factors. The means of emission factors for extratropical forest estimated with the two FTIR data sets are 0.40 ± 0.21 g kg−1 for HCN, 1.24 ± 0.71 g kg−1 for C2H6, 0.34 ± 0.21 g kg−1 for C2H2, and 2.92 ± 1.30 g kg−1 for HCOOH. The emission factor for CH3OH estimated at Eureka is 3.44 ± 1.68 g kg−1. To improve our knowledge concerning the dynamical and chemical processes associated with Arctic pollution from fires, the two sets of FTIR measurements were compared to the Model for OZone And Related chemical Tracers, version 4 (MOZART-4). Seasonal cycles and day-to-day variabilities were compared to assess the ability of the model to reproduce emissions from fires and their transport. Good agreement in winter confirms that transport is well implemented in the model. For C2H6, however, the lower wintertime concentration estimated by the model as compared to the FTIR observations highlights an underestimation of its emission. Results show that modeled and measured total columns are correlated (linear correlation coefficient r 〉 0.6 for all gases except for H2CO at Eureka and HCOOH at Thule), but suggest a general underestimation of the concentrations in the model for all seven tropospheric species in the high Arctic.