P. F. Fogal

A New Bruker IFS 125HR FTIR Spectrometer for the Polar Environment Atmospheric Research Laboratory at Eureka, Nunavut, Canada: Measurements and Comparison with the Existing Bomem DA8 Spectrometer

Abstract A new Bruker IFS 125HR Fourier transform spectrometer has been installed at the Polar Environment Atmospheric Research Laboratory at Eureka, Nunavut, Canada (80.05°N, 86.42°W). This instrument will become the Network for the Detection of Atmospheric Composition Change’s (NDACC’s) primary instrument at Eureka, replacing the existing Bomem DA8 Fourier transform spectrometer, and will operate throughout the sunlit parts of the year. This paper introduces the new instrument and describes the retrieval procedure, including a comprehensive error analysis. Total columns of O3, HCl, HF, HNO3, N2O, CH4, and CO are presented for the first full year of measurements (2007). Perturbations in the total column resulting from the presence of the Arctic polar vortex over Eureka and the chemical processes within it are visible, as are annual cycles driven by photochemistry and dynamics. Enhancements in the CO total column resulting from specific biomass burning smoke events can also be seen. An intercomparison bet...

A Remotely Operated Lidar for Aerosol, Temperature, and Water Vapor Profiling in the High Arctic

AbstractA Rayleigh–Mie–Raman lidar has been installed and is operating in the Polar Environment Atmospheric Research Laboratory at Eureka in the High Arctic (79°59′N, 85°56′W) as part of the Canadian Network for the Detection of Atmospheric Change. The lidar operates in both the visible and ultraviolet and measures aerosol backscatter and extinction coefficients, depolarization ratio, tropospheric temperature, and water vapor mixing ratio. Variable field of view, aperture, and filtering allow fine-tuning of the instrument for different atmospheric conditions. Because of the remote location, operations are carried out via a satellite link. The instrument is introduced along with the measurement techniques utilized and interference filter specifications. The temperature dependence of the water vapor signal depends on the filter specifications, and this is discussed in terms of minimizing the uncertainty of the water vapor mixing ratio product. Finally, an example measurement is presented to illustrate the p...

Toronto-area ozone: Long-term measurements and modelled sources of poor air quality events

The University of Toronto Atmospheric Observatory and Environment Canadas Centre for Atmospheric Research Experiments each has over a decade of ground-based Fourier transform infrared (FTIR) spectroscopy measurements in southern Ontario. We present the Toronto area FTIR time series from 2002 to 2013 of two tropospheric trace gases—ozone and carbon monoxide—along with surface in situ measurements taken by government monitoring programs. We interpret their variability with the GEOS-Chem chemical transport model and determine the atmospheric conditions that cause pollution events in the time series. Our analysis includes a regionally tagged O3 model of the 2004–2007 time period, which quantifies the geographical contributions to Toronto area O3. The important emission types for 15 pollution events are then determined with a high-resolution adjoint model. Toronto O3, during pollution events, is most sensitive to southern Ontario and U.S. fossil fuel NOx emissions and natural isoprene emissions. The sources of Toronto pollution events are found to be highly variable, and this is demonstrated in four case studies representing local, short-, middle-, and long-range transport scenarios. This suggests that continental-scale emission reductions could improve air quality in the Toronto region. We also find that abnormally high temperatures and high-pressure systems are common to all pollution events studied, suggesting that climate change may impact Toronto O3. Finally, we quantitatively compare the sensitivity of the surface and column measurements to anthropogenic NOx emissions and show that they are remarkably similar. This work thus demonstrates the usefulness of FTIR measurements in an urban area to assess air quality.

Understanding ozone depletion: Measurements and models

Abstract This paper provides an overview of the measurement systems available to make observations of the chemistry of the ozone layer. The characteristics and applications of the data collected are considered. Models provide insight into the physical processes taking place that determine the state of the ozone layer. The properties and uses of a number of models are examined.

Infra‐red FTS measurements of CH4, N2O, O3, HNO3, HCl, CFC‐11 and CFC‐12 from the MANTRA balloon campaign

Abstract The Middle Atmosphere Nitrogen TRend Assessment (MANTRA) campaign is intended to address the question of whether possible changes in the mid‐latitude nitrogen budget can account for discrepancies between predicted and observed ozone loss at these latitudes. In addition, MANTRA seeks to establish consistency between old and new measurement techniques. We report here the results of infra‐red spectral measurements made with a high resolution Fourier Transform Spectrometer (FTS) during the August 1998 MANTRA flight. Vertical mixing ratio profiles of methane, nitrous oxide, ozone, nitric acid, hydrogen chloride, CFC‐11 and CFC‐12 are presented. The error estimates on the retrieved values are larger than typical for this type of measurement, due mostly to instrument problems that occurred during flight. In addition, the CFC values are larger than expected. Possible reasons for this are discussed.

Ozone: From discovery to protection

Abstract Within one hundred and fifty years, ozone has gone from an unknown quantity to a protected species. This paper traces the evolution of the science of the ozone layer and follows modern research efforts to the point where the Montreal Protocol to Protect the Ozone Layer was put into place. The Montreal Protocol deserves special consideration because it is the best example of a case where science rapidly drove policy development to bring about the implementation of a global agreement to protect the environment.

Characterization of aerosol growth events over Ellesmere Island during the summers of 2015 and 2016

The occurrence of frequent aerosol nucleation and growth events in the Arctic during summertime may impact the region’s climate through increasing the number of cloud condensation nuclei in the Arctic atmosphere. Measurements of aerosol size distributions and aerosol composition were taken during the summers of 2015 and 2016 at Eureka and Alert on 15 Ellesmere Island in Nunavut, Canada. The corresponding results provide a better understanding of the frequency and spatial extent of these nucleation and growth events as well as of the composition and sources of aerosol mass during particle growth. These events are observed beginning in June with the melting of the sea ice rather than with polar sunrise, which strongly suggests emissions from marine sources are the primary cause of the events. Frequent particle nucleation followed by growth occurs throughout the summer. Correlated particle growths events at the two sites, separated by 480 km, indicate 20 conditions existing over such large scales play a key role in determining the timing and the characteristics of the events. In addition, aerosol mass spectrometry measurements are used to analyze the size-resolved chemical composition of aerosols during two selected growth events. It is found that particles with diameters smaller than 100 nm are predominately organic with only a small sulphate contribution. The oxidation of the organic fraction also changes with particle size with larger particles containing a greater fraction of organic acids relative to other non-acid oxygenates (e.g. alcohols or 25 aldehydes). It is also observed that the relative amount of m/z 44 in the measured mass spectra increases during the growth events suggesting increases in organic acid concentrations in the particle phase. The nucleation and growth events at Eureka are observed most often when the temperature inversion between the sea and the measurement site (at 610 m ASL) is non-existent or weak allowing presumably fresh marine emissions to be mixed upward to the observatory altitude. While the nature of the gaseous precursors responsible for the growth events are 30 poorly understood, oxidation of dimethyl sulphide alone to produce particle phase sulphate or methanesulphonic acid is not consistent with the measured aerosol composition, suggesting the importance of condensation of other gas phase organic compounds for particle growth. 1 Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-428 Manuscript under review for journal Atmos. Chem. Phys. Discussion started: 8 May 2018 c

Multi-year comparisons of ground-based and space-borne Fourier Transform Spectrometers in the high Arctic between 2006 and 2013

This paper presents 8 years (2006–2013) of measurements obtained from Fourier transform spectrometers (FTSs) in the high Arctic at the Polar Environment Atmospheric Research Laboratory (PEARL; 80.05 N, 86.42W). These measurements were taken as part of the Canadian Arctic ACE (Atmospheric Chemistry Experiment) validation campaigns that have been carried out since 2004 during the polar sunrise period (from mid-February to mid-April). Each spring, two ground-based FTSs were used to measure total and partial columns of HF, O3, and trace gases that impact O3 depletion, namely, HCl and HNO3. Additionally, some tropospheric greenhouse gases and pollutant species were measured, namely CH4, N2O, CO, and C2H6. During the same time period, the satellite-based ACE-FTS made measurements near Eureka and provided profiles of the same trace gases. Comparisons have been carried out between the measurements from the Portable Atmospheric Research Interferometric Spectrometer for the InfraRed (PARIS-IR) and the co-located high-resolution Bruker 125HR FTS, as well as with the latest version of the ACE-FTS retrievals (v3.5). The total column comparison between the two colocated ground-based FTSs, PARIS-IR and Bruker 125HR, found very good agreement for most of these species (except HF), with differences well below the estimated uncertainties (≤ 6%) and with high correlations (R ≥ 0.8). Partial columns have been used for the ground-based to space-borne comparison, with coincident measurements selected based on time, distance, and scaled potential vorticity (sPV). The comparisons of the ground-based measurements with ACEFTS show good agreement in the partial columns for most species within 6 % (except for C2H6 and PARIS-IR HF), which is consistent with the total retrieval uncertainty of the ground-based instruments. The correlation coefficients (R) of the partial column comparisons for all eight species range from approximately 0.75 to 0.95. The comparisons show no notable increases of the mean differences over these 8 years, indicating the consistency of these datasets and suggesting that the space-borne ACE-FTS measurements have been stable over this period. In addition, changes in the amounts of these trace gases during springtime between 2006 and 2013 are presented and discussed. Increased O3 (0.9%yr−1), HCl (1.7%yr−1), HF (3.8%yr−1), CH4 (0.5 % yr−1), and C2H6 (2.3%yr−1, 2009–2013) have been found with the PARIS-IR dataset, the longer of the two ground-based records. Published by Copernicus Publications on behalf of the European Geosciences Union. 3274 D. Griffin et al.: Ground-based and space-borne FTS comparisons in the high Arctic (2006–2013)

Infrared Measurements Throughout Polar Night using Two AERIs in the Arctic

The Extended-range Atmospheric Emitted Radiance Interferometer (E-AERI) is a moderate resolution (1 cm−1) Fourier transform infrared spectrometer for measuring the absolute downwelling infrared spectral radiance from the atmosphere between 400 and 3000 cm−1. The extended spectral range of the instrument permits monitoring of the 400–550 cm−1 (20–25 μm) region, where much of the infrared surface cooling currently occurs in the dry air of the Arctic. The E-AERI provides information about radiative balance, trace gases, and cloud properties in the Canadian high Arctic. The instrument was installed at the Polar Environment Atmospheric Research Laboratory (PEARL) Ridge Lab at Eureka, Nunavut, in October 2008. Measurements are taken every seven minutes year-round (precipitation permitting), including polar night when the solar-viewing spectrometers are not operated. A similar instrument, the University of Idaho’s Polar AERI (P-AERI), was installed at the Zero-altitude PEARL Auxiliary Laboratory (0PAL), 15 km away from the Ridge Lab, from March 2006 to June 2009. During the period of overlap, these two instruments provided calibrated radiance measurements from two different altitudes. Retrievals of total columns of various trace gases are being evaluated using a prototype version of the retrieval algorithm SFIT2 modified to analyze emission features. In contrast to solar absorption measurements of atmospheric trace gases, which depend on sunlit clear-sky conditions, the use of emission spectra allows measurements year-round (except during precipitation events or when clouds are present). This capability allows the E-AERI to provide temporal coverage throughout the four months of polar night and to measure the radiative budget throughout the entire year. This presentation will describe the new E-AERI instrument, its performance evaluations, and clear sky vs. cloudy measurements.