K. A. Walker

University of Toronto, Toronto, Ontario, Canada

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Publications (274)549.07 Total impact

  • Niall J. Ryan, Kaley A. Walker
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    ABSTRACT: A preparatory performance and error characterization was carried out for a ground-based millimeter wave instrument designed for high Arctic atmospheric research. The instrument is a radiometer to measure rotational emission spectra of O3, ClO, HNO3, and N2O, between 265 and 280 GHz, using a sensitive superconductor–insulator–superconductor detector. Forward and inverse modeling tests have been performed to assess the instrument/inversion system and to determine the sources of the most significant errors in the retrieval of each trace gas. The altitude ranges over which retrievals of concentrations can be made were found to be ~13–62 km for O3, ~12.5–39 km for N2O, ~12–36 km for HNO3, and ~18–46 km for ClO. For each target species the measurement and smoothing errors calculated with an optimal estimation method (OEM) were compared to the errors calculated from inversions of 500 simulated spectra. The absolute error from these inversions agreed well the OEM results, but there were systematic differences that are attributed to nonlinearities in the forward model. The results of these nonlinearities can cause biases of the order of 5–10% of the a priori profile if they are not accounted for when averaging concentration profiles or when analyzing trends in concentration. The techniques used here can be applied to any ground-based remote sounder.
    Journal of Quantitative Spectroscopy and Radiative Transfer 01/2015; 151:26–37. · 2.38 Impact Factor
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    ABSTRACT: The abundance of chlorine in the Earth's atmosphere increased considerably during the 1970s to 1990s, following large emissions of anthropogenic long-lived chlorine-containing source gases, notably the chlorofluorocarbons. The chemical inertness of chlorofluorocarbons allows their transport and mixing throughout the troposphere on a global scale, before they reach the stratosphere where they release chlorine atoms that cause ozone depletion. The large ozone loss over Antarctica was the key observation that stimulated the definition and signing in 1987 of the Montreal Protocol, an international treaty establishing a schedule to reduce the production of the major chlorine- and bromine-containing halocarbons. Owing to its implementation, the near-surface total chlorine concentration showed a maximum in 1993, followed by a decrease of half a per cent to one per cent per year, in line with expectations. Remote-sensing data have revealed a peak in stratospheric chlorine after 1996, then a decrease of close to one per cent per year, in agreement with the surface observations of the chlorine source gases and model calculations. Here we present ground-based and satellite data that show a recent and significant increase, at the 2σ level, in hydrogen chloride (HCl), the main stratospheric chlorine reservoir, starting around 2007 in the lower stratosphere of the Northern Hemisphere, in contrast with the ongoing monotonic decrease of near-surface source gases. Using model simulations, we attribute this trend anomaly to a slowdown in the Northern Hemisphere atmospheric circulation, occurring over several consecutive years, transporting more aged air to the lower stratosphere, and characterized by a larger relative conversion of source gases to HCl. This short-term dynamical variability will also affect other stratospheric tracers and needs to be accounted for when studying the evolution of the stratospheric ozone layer.
    Nature 11/2014; 515(7525):104-107. · 38.60 Impact Factor
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    ABSTRACT: We present measurements of a long-range smoke transport event recorded on 20–21 July 2011 over Halifax, Nova Scotia, Canada, during the Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites (BORTAS-B) campaign. Ground-based Fourier transform spectrometers and photometers detected air masses associated with large wild-land fires burning in eastern Manitoba and western Ontario. We investigate a plume with high trace gas amounts but low amounts of particles that preceded and overlapped at the Halifax site with a second plume with high trace gas loadings and significant amounts of particulate material. We show that the first plume experienced a meteorological scavenging event, but the second plume had not been similarly scavenged. This points to the necessity to account carefully for the plume history when considering long-range transport since simultaneous or near-simultaneous times of arrival are not necessarily indicative of either similar trajectories or meteorological history. We investigate the origin of the scavenged plume, and the possibility of an aerosol wet deposition event occurring in the plume ∼ 24 h prior to the measurements over Halifax. The region of lofting and scavenging is only monitored on an intermittent basis by the present ob-serving network, and thus we must consider many different pieces of evidence in an effort to understand the early dynamics of the plume. Through this discussion we also demonstrate the value of having many simultaneous remote-sensing measurements in order to understand the physical and chemical behaviour of biomass burning plumes.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 08/2014; 14:8449-8460. · 5.51 Impact Factor
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    ABSTRACT: We present the first comprehensive intercomparison of currently available satellite ozone climatologies in the upper troposphere / lower stratosphere (UTLS) (300-70 hPa) as part of the Stratosphere-troposphere Processes and their Role in Climate (SPARC) Data Initiative. The Tropospheric Emission Spectrometer (TES) instrument is the only nadir-viewing instrument in this initiative, as well as the only instrument with a focus on tropospheric composition. We apply the TES observational operator to ozone climatologies from the more highly vertically resolved limb-viewing instruments. This minimizes the impact of differences in vertical resolution among the instruments and allows identification of systematic differences in the large-scale structure and variability of UTLS ozone. We find that the climatologies from most of the limb-viewing instruments show positive differences (ranging from 5 to 75%) with respect to TES in the tropical UTLS, and comparison to a “zonal mean” ozonesonde climatology indicates that these differences likely represent a positive bias for p ≤ 100 hPa. In the extratropics, there is good agreement among the climatologies regarding the timing and magnitude of the ozone seasonal cycle (differences in the peak-to-peak amplitude of <15%) when the TES observational operator is applied, as well as very consistent midlatitude interannual variability. The discrepancies in ozone temporal variability are larger in the tropics, with differences between the datasets of up to 55% in the seasonal cycle amplitude. However, the differences among the climatologies are everywhere much smaller than the range produced by current chemistry-climate models, indicating that the multiple-instrument ensemble is useful for quantitatively evaluating these models.
    Journal of Geophysical Research: Atmospheres. 05/2014;
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    ABSTRACT: Drifts, trends and periodic variations were calculated from monthly zonally averaged ozone profiles. The ozone profiles were derived from level-1b data of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) by means of the scientific level-2 processor run by the Karlsruhe Institute of Technology (KIT), Institute for Meteorology and Climate Research (IMK). All trend and drift analyses were performed using a multilinear parametric trend model which includes a linear term, several harmonics with period lengths from 3 to 24 months and the quasi-biennial oscillation (QBO). Drifts at 2-sigma significance level were mainly negative for ozone relative to Aura MLS and Odin OSIRIS and negative or near zero for most of the comparisons to lidar measurements. Lidar stations used here include those at Hohenpeissenberg (47.8° N, 11.0° E), Lauder (45.0° S, 169.7° E), Mauna Loa (19.5° N, 155.6° W), Observatoire Haute Provence (43.9° N, 5.7° E) and Table Mountain (34.4° N, 117.7° W). Drifts against the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) were found to be mostly insignificant. The assessed MIPAS ozone trends cover the time period of July 2002 to April 2012 and range from -0.56 ppmv decade-1 to +0.48 ppmv decade-1 (-0.52 ppmv decade-1 to +0.47 ppmv decade-1 when displayed on pressure coordinates) depending on altitude/pressure and latitude. From the empirical drift analyses we conclude that the real ozone trends might be slightly more positive/less negative than those calculated from the MIPAS data, by conceding the possibility of MIPAS having a very small (approximately within -0.3 ppmv decade-1) negative drift for ozone. This leads to drift-corrected trends of -0.41 ppmv decade-1 to +0.55 ppmv decade-1 (-0.38 ppmv decade-1 to +0.53 ppmv decade-1 when displayed on pressure coordinates) for the time period covered by MIPAS Envisat measurements, with very few negative and large areas of positive trends at mid-latitudes for both hemispheres around and above 30 km (~10 hPa). Negative trends are found in the tropics around 25 and 35 km (~25 and 5 hPa), while an area of positive trends is located right above the tropical tropopause. These findings are in good agreement with the recent literature. Differences of the trends compared with the recent literature could be explained by a possible shift of the subtropical mixing barriers. Results for the altitude-latitude distribution of amplitudes of the quasi-biennial, annual and the semi-annual oscillation are overall in very good agreement with recent findings.
    Atmospheric Chemistry and Physics 02/2014; 14(5). · 4.88 Impact Factor
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    ABSTRACT: We present measurements of a long range smoke transport event recorded on 20–21 July 2011 over Halifax, Nova Scotia, Canada, during the Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites (BORTAS-B) campaign. Ground-based Fourier transform spectrometers and photometers detected air masses associated with large wildland fires burning in eastern Manitoba and western Ontario. We investigate a plume with high trace gas amounts but low amounts of particles that preceded and overlapped at the Halifax site with a second plume with high trace gas loadings and significant amounts of particulate material. We show that the first plume experienced a meteorological scavenging event but the second plume had not been similarly scavenged. This points to the necessity to account carefully for the plume history when considering long range transport since simultaneous or near-simultaneous times of arrival are not necessarily indicative of either similar trajectories or meteorological history. We investigate the origin of the scavenged plume, and the possibility of an aerosol wet deposition event occurring in the plume ~24 h prior to the measurements over Halifax. The region of lofting and scavenging is only monitored on an intermittent basis by the present observing network, and thus we must consider many different pieces of evidence in an effort to understand the early dynamics of the plume. Through this discussion we also demonstrate the value of having many simultaneous remote-sensing measurements in order to understand the physical and chemical behaviour of biomass burning plumes.
    ATMOSPHERIC CHEMISTRY AND PHYSICS DISCUSSIONS. 02/2014; 14:3395-3426.
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    ABSTRACT: An algorithm is developed to retrieve the vertical profile of carbon dioxide in the 5 to 25 km altitude range using mid-infrared solar occultation spectra from the main instrument of the ACE (Atmospheric Chemistry Experiment) mission, namely the Fourier Transform Spectrometer (FTS). The main challenge is to find an atmospheric phenomenon which can be used for accurate tangent height determination in the lower atmosphere, where the tangent heights (THs) calculated from geometric and timing information is not of sufficient accuracy. Error budgets for the retrieval of CO2 from ACE-FTS and the FTS on a potential follow-on mission named CASS (Chemical and Aerosol Sounding Satellite) are calculated and contrasted. Retrieved THs are typically within 60 m of those retrieved using the ACE version 3.x software after revisiting the temperature dependence of the N2 CIA (Collision-Induced Absorption) laboratory measurements and accounting for sulfate aerosol extinction. After correcting for the known residual high bias of ACE version 3.x THs expected from CO2 spectroscopic/isotopic inconsistencies, the remaining bias for tangent heights determined with the N2 CIA is -20m. CO2 in the 5-13 km range in the 2009-2011 time frame is validated against aircraft measurements from CARIBIC, CONTRAIL and HIPPO, yielding typical biases of -1.7 ppm in the 5-13 km range. The standard error of these biases in this vertical range is 0.4 ppm. The multi-year ACE-FTS dataset is valuable in determining the seasonal variation of the latitudinal gradient which arises from the strong seasonal cycle in the Northern Hemisphere troposphere. The annual growth of CO2 in this time frame is determined to be 2.5 ± 0.7 ppm yr-1, in agreement with the currently accepted global growth rate based on ground-based measurements.
    01/2014; 7(2).
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    ABSTRACT: The long-term evolution of the vertical column abundance of carbon tetrafluoride (CF4) above the high altitude Jungfraujoch station (Swiss Alps, 46.5 °N, 8.0 °E, 3580 m a.s.l.) has been derived from the spectrometric analysis of Fourier transform infrared solar spectra recorded at that site between 1989 and 2012. The investigation is based on a multi-microwindow approach, two encompassing pairs of absorption lines belonging to the strong ν3 band of CF4 centered at 1283 cm-1, and two additional ones to optimally account for weak but overlapping HNO3 interferences. The analysis reveals a steady accumulation of the very long-lived CF4 above the Jungfraujoch at mean rates of (1.38 ± 0.11) × 1013 molec cm-2 yr-1 from 1989 to 1997, and (0.97 ± 0.02) × 1013 molec cm-2 yr-1 from 1998 to 2012, which correspond to linear growth rates of 1.71 ± 0.14 and 1.04 ± 0.02% yr-1, respectively referenced to 1989 and 1998. Related global CF4 emissions required to sustain these mean increases correspond to 15.8 ± 1.3 and 11.1 ± 0.2 Gg yr-1 over the above specified time intervals. Findings reported here are compared and discussed with respect to relevant results obtained remotely from space and balloons as well as in situ on the ground, including new gas chromatography mass spectrometry measurements performed at the Jungfraujoch since 2010.
    Atmos. Meas. Tech. 01/2014; 7(1):333-344.
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    ABSTRACT: Nitric acid trihydrate (NAT) particles in the polar stratosphere have been shown to be responsible for vertical redistribution of reactive nitrogen (NOy). Recent observations by Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) aboard the CALIPSO satellite have been explained in terms of heterogeneous nucleation of NAT on foreign nuclei, revealing this to be an important formation pathway for the NAT particles. In state of the art global- or regional-scale models, heterogeneous NAT nucleation is currently simulated in a very coarse manner using a constant, saturation-independent nucleation rate. Here we present first simulations for the Arctic winter 2009/2010 applying a new saturation-dependent parametrisation of heterogeneous NAT nucleation rates within the Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulation shows good agreement of chemical trace species with in situ and remote sensing observations. The simulated polar stratospheric cloud (PSC) optical properties agree much better with CALIOP observations than those simulated with a constant nucleation rate model. A comparison of the simulated particle size distributions with observations made using the Forward Scattering Spectrometer Probe (FSSP) aboard the high altitude research aircraft Geophysica, shows that the model reproduces the observed size distribution, except for the very largest particles above 15 μm diameter. The vertical NOy redistribution caused by the sedimentation of the NAT particles, in particular the denitrification and nitrification signals observed by the ACE-FTS satellite instrument and the in situ SIOUX instrument aboard the Geophysica, are reproduced by the improved model, and a small improvement with respect to the constant nucleation rate model is found.
    12/2013; 14(2).
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    ABSTRACT: We present vertical profiles of hydrogen chloride (HCl) and chlorine monoxide (ClO) as observed by the Su-perconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) on the International Space Station (ISS) inside the Antarctic vortex on 19–24 November 2009. The SMILES HCl value reveals 2.8–3.1 ppbv between 450 K and 500 K levels in potential temperature (PT). The high value of HCl is highlighted since it is suggested that HCl is a main com-ponent of the total inorganic chlorine (Cl y), defined as Cl y HCl + ClO + chlorine nitrate (ClONO 2), inside the Antarc-tic vortex in spring, owing to low ozone values. To con-firm the quality of two SMILES level 2 (L2) data prod-ucts provided by the Japan Aerospace Exploration Agency (JAXA) and Japan's National Institute of Information and Communications Technology (NICT), vis-à-vis the partition-ing of Cl y , comparisons are made using other satellite data from the Aura Microwave Limb Sounder (MLS) and At-mospheric Chemistry Experiment Fourier Transform Spec-trometer (ACE-FTS). HCl values from the SMILES NICT L2 product agree to within 10 % (0.3 ppbv) with the MLS HCl data between 450 and 575 K levels in PT and with the ACE-FTS HCl data between 425 and 575 K. The SMILES JAXA L2 product is 10 to 20 % (0.2–0.5 ppbv) lower than that from MLS between 400 and 700 K and from ACE-FTS between 500 and 700 K. For ClO in daytime, the difference between SMILES (JAXA and NICT) and MLS is less than ±0.05 ppbv (100 %) between 500 K and 650 K with the ClO values less than 0.2 ppbv. ClONO 2 values as measured by ACE-FTS also reveal 0.2 ppbv at 475–500 K level, resulting in the HCl / Cl y ratios of 0.91–0.95. The HCl / Cl y ratios de-rived from each retrieval agree to within −5 to 8 % with re-gard to their averages. The high HCl values and HCl / Cl y ratios observed by the three instruments in the lower strato-spheric Antarctic vortex are consistent with previous obser-vations in late Austral spring.
    Atmospheric Measurement Techniques 11/2013; 6:3099-3113. · 3.21 Impact Factor
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    ABSTRACT: [1] Monthly zonal mean climatologies of atmospheric measurements from satellite instruments can have biases due to the nonuniform sampling of the atmosphere by the instruments. We characterize potential sampling biases in stratospheric trace gas climatologies of the Stratospheric Processes and Their Role in Climate (SPARC) Data Initiative using chemical fields from a chemistry climate model simulation and sampling patterns from 16 satellite-borne instruments. The exercise is performed for the long-lived stratospheric trace gases O3 and H2O. Monthly sampling biases for O3 exceed 10% for many instruments in the high-latitude stratosphere and in the upper troposphere/lower stratosphere, while annual mean sampling biases reach values of up to 20% in the same regions for some instruments. Sampling biases for H2O are generally smaller than for O3, although still notable in the upper troposphere/lower stratosphere and Southern Hemisphere high latitudes. The most important mechanism leading to monthly sampling bias is nonuniform temporal sampling, i.e., the fact that for many instruments, monthly means are produced from measurements which span less than the full month in question. Similarly, annual mean sampling biases are well explained by nonuniformity in the month-to-month sampling by different instruments. Nonuniform sampling in latitude and longitude are shown to also lead to nonnegligible sampling biases, which are most relevant for climatologies which are otherwise free of biases due to nonuniform temporal sampling.
    Journal of Geophysical Research: Atmospheres. 10/2013; 118(20).
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    ABSTRACT: We present the results of total column measurements of CO, C2 H6 and fine-mode aerosol optical depth (AOD) during the “Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites” (BORTAS-B) campaign over eastern Canada. Ground-based observations, using Fourier transform spectrometers (FTSs) and sun photometers, were carried out in July and August 2011. These measurements were taken in Halifax, Nova Scotia, which is an ideal location to monitor the outflow of boreal fires from North America, and also in Toronto, Ontario. Measurements of fine-mode AOD enhancements were highly correlated with enhancements in coincident trace gas (CO and C2H6) observations between 19 and 21 July 2011, which is typical for a smoke plume event. In this paper, we focus on the identification of the origin and the transport of this smoke plume. We use back trajectories calculated by the Canadian Meteorological Centre as well as FLEXPART forward trajectories to demonstrate that the enhanced CO, C2H6 and fine-mode AOD seen near Halifax and Toronto originated from forest fires in northwestern Ontario that occurred between 17 and 19 July 2011. In addition, total column measurements of CO from the satellite-borne Infrared Atmospheric Sounding Interferometer (IASI) have been used to trace the smoke plume and to confirm the origin of the CO enhancement. Furthermore, the enhancement ratio – that is, in this case equivalent to the emission ratio (ERC2 H6 /CO) – was estimated from these ground- based observations. These C2 H6 emission results from boreal fires in northwestern Ontario agree well with C2H6 emission measurements from other boreal regions, and are relatively high compared to fires from other geographical regions. The ground-based CO and C2H6 observations were compared with outputs from the 3-D global chemical trans- port model GEOS-Chem, using the Fire Locating And Modeling of Burning Emissions (FLAMBE) inventory. Agreement within the stated measurement uncertainty (∼ 3 % for CO and ∼ 8 % for C2H6) was found for the magnitude of the enhancement of the CO and C2H6 total columns between the measured and modelled results. However, there is a small shift in time (of approximately 6 h) of arrival of the plume over Halifax between the results.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 10/2013; 13:10227-10241. · 5.51 Impact Factor
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    ABSTRACT: The international research project RECONCILE has addressed central questions regarding polar ozone depletion, with the objective to quantify some of the most relevant yet still uncertain physical and chemical processes and thereby improve prognostic modelling capabilities to realistically predict the response of the ozone layer to climate change. This overview paper outlines the scope and the general approach of RECONCILE, and it provides a summary of observations and modelling in 2010 and 2011 that have generated an in many respects unprecedented dataset to study processes in the Arctic winter stratosphere. Principally, it summarises important outcomes of RECONCILE including (i) better constraints and enhanced consistency on the set of parameters governing catalytic ozone destruction cycles, (ii) a better understanding of the role of cold binary aerosols in heterogeneous chlorine activation, (iii) an improved scheme of polar stratospheric cloud (PSC) processes that includes heterogeneous nucleation of nitric acid trihydrate (NAT) and ice on non-volatile background aerosol leading to better model parameterisations with respect to denitrification, and (iv) long transient simulations with a chemistry-climate model (CCM) updated based on the results of RECONCILE that better reproduce past ozone trends in Antarctica and are deemed to produce more reliable predictions of future ozone trends. The process studies and the global simulations conducted in RECONCILE show that in the Arctic, ozone depletion uncertainties in the chemical and microphysical processes are now clearly smaller than the sensitivity to dynamic variability.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 09/2013; · 5.51 Impact Factor
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    ABSTRACT: The diurnal variation of HOCl and the related species ClO, HO 2 and HCl measured by satellites has been compared with the results of a one-dimensional photochem-ical model. The study compares the data from various limb-viewing instruments with model simulations from the middle stratosphere to the lower mesosphere. Data from three sub-millimetre instruments and two infrared spectrometers are used, namely from the Sub-Millimetre Radiometer (SMR) on board Odin, the Microwave Limb Sounder (MLS) on board Aura, the Superconducting Submillimeter-wave Limb-Emission Sounder (SMILES) on the International Space Sta-tion, the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on board ENVISAT, and the Atmo-spheric Chemistry Experiment Fourier Transform Spectrom-eter (ACE-FTS) on board SCISAT. Inter-comparison of the measurements from instruments on sun-synchronous satel-lites (SMR, MLS, MIPAS) and measurements from solar occultation instruments (ACE-FTS) is challenging since the measurements correspond to different solar zenith angles (or local times). However, using a model which covers all solar zenith angles and data from the SMILES instrument which measured at all local times over a period of several months provides the possibility to verify the model and to indirectly compare the diurnally variable species. The satellite data were averaged for latitudes of 20 • S to 20 • N for the SMILES observation period from November 2009 to April 2010 and were compared at three altitudes: 35, 45 and 55 km. Besides presenting the SMILES data, the study also shows a first comparison of the latest MLS data (version 3.3) of HOCl, ClO, and HO 2 with other satellite observations, as well as a first evaluation of HO 2 observations made by Odin/SMR. The MISU-1D model has been carefully initialised and run for conditions and locations of the observations. The diurnal cycle features for the species investigated here are generally well reproduced by the model. The satellite observations and the model agree well in terms of absolute mixing ratios. The differences between the day and night values of the model are in good agreement with the observations although the ampli-tude of the HO 2 diurnal variation is 10–20 % lower in the model than in the observations. In particular, the data offered the opportunity to study the reaction ClO+HO 2 → HOCl+O 2 in the lower mesosphere at 55 km. At this altitude the HOCl Published by Copernicus Publications on behalf of the European Geosciences Union. 7588 M. Khosravi et al.: HOCl, ClO and HO 2 diurnal variation in the tropics night-time variation depends only on this reaction. The result of this analysis points towards a value of the rate constant within the range of the JPL 2006 recommendation and the upper uncertainty limit of the JPL 2011 recommendation at 55 km.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 08/2013; 13:7587-7606. · 5.51 Impact Factor
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    ABSTRACT: [1] Satellite observations from three instruments (Microwave Limb Sounder, Optical Spectrograph and Infrared Imaging System, and Atmospheric Chemistry Experiment Fourier Transform Spectrometer) reveal coherent patterns of low ozone events (
    Geophysical Research Letters. 07/2013; 40(14).
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    ABSTRACT: We describe the design and execution of the BORTAS (Quantifying the impact of BOReal forest fires on Tropospheric oxidants using Aircraft and Satellites) experiment, which has the overarching objective of understanding the chemical aging of airmasses that contain the emission products from seasonal boreal wildfires and how these airmasses subsequently impact downwind atmospheric composition. The central focus of the experiment was a two-week deployment of the UK BAe-146-301 Atmospheric Research Aircraft (ARA) over eastern Canada. The planned July 2010 deployment of the ARA was postponed by 12 months because of activities related to the dispersal of material emitted by the Eyjafjallajo¨kull volcano. However, most other planned model and measurement activities, including ground-based measurements at the Dalhousie University Ground Station (DGS), enhanced ozonesonde launches, and measurements at the Pico Atmospheric Observatory in the Azores, went ahead and constituted phase A of the experiment. Phase B of BORTAS in July 2011 included the same measurements, but included the ARA, special satellite observations and a more comprehensive measurement suite at the DGS. The high-frequency aircraft data provided a comprehensive snapshot of the pyrogenic plumes from wildfires. The coordinated ground-based and sonde data provided detailed but spatially-limited information that put the aircraft data into context of the longer burning season. We coordinated aircraft vertical profiles and overpasses of the NASA Tropospheric Emission Spectrometer and the Canadian Atmospheric Chemistry Experiment. These space-borne data, while less precise than other data, helped to relate the two-week measurement campaign to larger geographical and longer temporal scales. We interpret these data using a range of chemistry models: from a near-explicit gas-phase chemical mechanism, which tests out under standing of the underlying chemical mechanism, to regional and global 3-D models of atmospheric transport and lumped chemistry, which helps to assess the performance of the simplified chemical mechanism and effectively act as intermediaries between different measurement types. We also present an overview of some of the new science that has originated from this project from the mission planning and execution to the analysis of the ground-based, aircraft, and space-borne data.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 07/2013; 13:6239-6261. · 5.51 Impact Factor
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    ABSTRACT: This paper will discuss progress on development of the CSA-led Chemical and Aerosol Sounding Satellite (CASS) with specific focus on the Fourier Transform Spectrometer (CASS-FTS) that will perform solar occultation observations of Earth& rsquo;s atmosphere.
    Fourier Transform Spectroscopy; 06/2013
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    ABSTRACT: This presentation will describe the use of ground-based FTIR spectroscopy to measure atmospheric composition. It will focus on measurements made at the UofT Atmospheric Observatory and the high-Arctic PEARL facility, and introduce a new Canadian FTIR network.
    Fourier Transform Spectroscopy; 06/2013
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    ABSTRACT: [1] Ozone profiles in the upper mesosphere (70–100 km) retrieved from nine instruments are compared. Ozone from the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) instrument is used as the basis of comparison. Other measurements are from the Halogen Occultation Experiment, the High Resolution Doppler Imager, the Michelson Interferometer for Passive Atmospheric Sounding, the Global Ozone Monitoring by Occultation of Stars, the Atmospheric Chemistry Experiment—Fourier Transform Spectrometer, the Solar Occultation For Ice Experiment, the Optical Spectrograph and InfraRed Imaging System, and the Superconducting Submillimeter-Wave Limb-Emission Sounder. Comparisons of each data set with SABER using coincident profiles indicate agreement in the basic vertical profile of ozone but also some systematic differences in daytime ozone. Ozone from the SABER 9.6 μm channel is higher than the other measurements over the altitude range 60–80 km by 20–50%. Nighttime comparisons indicate better relative agreement (<10% difference). Taking all the data, not limited to coincidences, shows the global and seasonal distributions of ozone in the upper mesosphere from each instrument. The average maximum in ozone mixing ratio is around 90–92 km during daytime and 95 km at night. There is a maximum in ozone density at night (∼90 km) and during some hours of the day. The latitude structure of ozone has appreciable variations with season, particularly in the tropical upper mesosphere. The basic latitude-altitude structure of ozone depends on local time, even when the analysis is restricted to day-only observations.
    Journal of Geophysical Research 05/2013; · 3.17 Impact Factor

Publication Stats

2k Citations
549.07 Total Impact Points

Institutions

  • 2007–2014
    • University of Toronto
      • Department of Physics
      Toronto, Ontario, Canada
  • 1991–2013
    • University of Waterloo
      • Department of Chemistry
      Waterloo, Ontario, Canada
  • 2008
    • Belgian Institute for Space Aeronomy
      Bruxelles, Brussels Capital Region, Belgium