Showing papers by "Kaley A. Walker published in 2010"

Asian monsoon transport of pollution to the stratosphere.

Abstract: Transport of air from the troposphere to the stratosphere occurs primarily in the tropics, associated with the ascending branch of the Brewer-Dobson circulation. Here, we identify the transport of air masses from the surface, through the Asian monsoon, and deep into the stratosphere, using satellite observations of hydrogen cyanide (HCN), a tropospheric pollutant produced in biomass burning. A key factor in this identification is that HCN has a strong sink from contact with the ocean; much of the air in the tropical upper troposphere is relatively depleted in HCN, and hence, broad tropical upwelling cannot be the main source for the stratosphere. The monsoon circulation provides an effective pathway for pollution from Asia, India, and Indonesia to enter the global stratosphere.

Multimodel assessment of the upper troposphere and lower stratosphere: Extratropics

Abstract: A multimodel assessment of the performance of chemistry-climate models (CCMs) in the extratropical upper troposphere/lower stratosphere (UTLS) is conducted for the first time. Process-oriented diagnostics are used to validate dynamical and transport characteristics of 18 CCMs using meteorological analyses and aircraft and satellite observations. The main dynamical and chemical climatological characteristics of the extratropical UTLS are generally well represented by the models, despite the limited horizontal and vertical resolution. The seasonal cycle of lowermost stratospheric mass is realistic, however with a wide spread in its mean value. A tropopause inversion layer is present in most models, although the maximum in static stability is located too high above the tropopause and is somewhat too weak, as expected from limited model resolution. Similar comments apply to the extratropical tropopause transition layer. The seasonality in lower stratospheric chemical tracers is consistent with the seasonality in the Brewer-Dobson circulation. Both vertical and meridional tracer gradients are of similar strength to those found in observations. Models that perform less well tend to use a semi-Lagrangian transport scheme and/or have a very low resolution. Two models, and the multimodel mean, score consistently well on all diagnostics, while seven other models score well on all diagnostics except the seasonal cycle of water vapor. Only four of the models are consistently below average. The lack of tropospheric chemistry in most models limits their evaluation in the upper troposphere. Finally, the UTLS is relatively sparsely sampled by observations, limiting our ability to quantitatively evaluate many aspects of model performance.

Hydrogen fluoride total and partial column time series above the Jungfraujoch from long-term FTIR measurements: Impact of the line-shape model, characterization of the error budget and seasonal cycle, and comparison with satellite and model data

Abstract: [1] Time series of hydrogen fluoride (HF) total columns have been derived from ground-based Fourier transform infrared (FTIR) solar spectra recorded between March 1984 and December 2009 at the International Scientific Station of the Jungfraujoch (Swiss Alps, 46.5°N, 8.0°E, 3580 m asl) with two high-resolution spectrometers (one homemade and one Bruker 120-HR). Solar spectra have been inverted with the PROFFIT 9.5 algorithm, using the optimal estimation method. An intercomparison of HF total columns retrieved with PROFFIT and SFIT-2–the other reference algorithm in the FTIR community–is performed for the first time. The effect of a Galatry line shape model on HF retrieved total columns and vertical profiles, on the residuals of the fits and on the error budget is also quantified. Information content analysis indicates that in addition to HF total vertical abundance, three independent stratospheric HF partial columns can be derived from our Bruker spectra. A complete error budget has been established and indicates that the main source of systematic error is linked to HF spectroscopy and that the random error affecting our HF total columns does not exceed 2.5%. Ground-based middle and upper stratospheric HF amounts have been compared to satellite data collected by the HALOE or ACE-FTS instruments. Comparisons of our FTIR HF total and partial columns with runs performed by two three-dimensional numerical models (SLIMCAT and KASIMA) are also included. Finally, FTIR and model HF total and partial columns time series have been analyzed to derive the main characteristics of their seasonal cycles.

An evaluation of infrared microwindows for ozone retrievals using the Eureka Bruker 125HR Fourier transform spectrometer

Abstract: A Bruker 125HR Fourier transform spectrometer was installed at the Polar Environment Atmospheric Research Laboratory (PEARL) at Eureka, Nunavut, Canada in the summer of 2006 to study atmospheric composition. Using the optimal estimation method, typically over a limited spectral region called a microwindow, information about the vertical distribution of trace gas species that have absorption bands in the mid-infrared spectral range can be retrieved. Total and partial columns can also be determined to show the temporal evolution of the target gas. For ozone in particular, retrievals have been performed using several of its many mid-infrared absorption features, resulting in a lack of consistency in the literature in the microwindows chosen for retrievals. This work focuses on the optimization of the ozone retrieval, assessing a set of 22 microwindows between 780 and 3052 cm −1 to determine which is best suited to conditions at Eureka. The 1000–1004.5 cm −1 spectral interval is shown to be the most sensitive to both the stratosphere and troposphere. This microwindow gives the highest number of degrees of freedom for signal (∼7 for total column), and the smallest total error (4.3%) compared with 21 other spectral regions. Retrievals performed with this microwindow agree well with results obtained from other instruments on-site. Total column ozone measured by the Bruker 125HR in this microwindow agreed to 2% with two other Fourier transform spectrometers, to 0.7% with a Brewer spectrophotometer, to 8% with a SAOZ UV–VIS spectrometer, and to 7% with ozone sondes.

Validation of v1.022 mesospheric water vapor observed by the Solar Occultation for Ice Experiment instrument on the Aeronomy of Ice in the Mesosphere satellite

Abstract: [1] Water vapor measured by the Solar Occultation for Ice Experiment (SOFIE) instrument on the Aeronomy of Ice in the Mesosphere satellite has been validated in the vertical range 45–95 km. Precision estimates for SOFIE v1.022 H2O are ∼0.2%–2.5% up to 80 km and degrade to ∼20% at ∼90 km. The SOFIE total systematic error from the retrieval analysis remains at ∼3%–4% throughout the lower to middle mesosphere and increases from ∼9% at 85 km to ∼16% at 95 km. Comparisons with Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS) and Microwave Limb Sounder (MLS) H2O show excellent agreement (0%–2%) up to 80 km in the Northern Hemisphere with rare exceptions. Percentage differences above ∼85 km increase to ∼20% or worse due largely to the low H2O volume mixing ratios in the upper mesosphere. For the Southern Hemisphere SOFIE is consistently biased low by 10%–20% relative to both ACE-FTS and MLS H2O. Slopes of SOFIE daily mean H2O isopleths on an altitude versus time cross section are used as an indicator of upwelling air motion. In the lower to middle mesosphere, the slope is the largest from mid-May to mid-June (maximum of ∼1.5 cm/s), and then in July and August, it is reduced significantly. Both SOFIE and MLS daily mean H2O volume mixing ratios at the polar mesospheric cloud height increase rapidly from ∼2.0 to ∼5.0 ppmv prior to the solstice and then approach a near-constant but slightly increasing level (6.0–6.5 ppmv) throughout the season.

NO2 air afterglow and O and NO densities from Odin‐OSIRIS night and ACE‐FTS sunset observations in the Antarctic MLT region

Abstract: [1] The continuum spectrum produced by the NO + O(+M) → NO 2 (+M) + hv chemiluminescent reaction has been detected in the upper mesospheric dark polar regions by Optical Spectrograph and Infra-Red Imager System (OSIRIS) on the Odin spacecraft. For the sample period of 8-9 May 2005, Southern Hemisphere, limb radiance profiles of continuum spectra, resolved from OH airglow and auroral contamination, are inverted to obtain volume emission rate altitude profiles. The maximum observed differential brightness referred to zenith viewing is 1.2 × 10 7 photons cm -2 s -1 nm -1 at 580 nm with a measurement uncertainty 5 × 10 5 photons cm - s -1 nm -1 , for an analysis range 80-101 km. Atomic oxygen densities [O] required by the analysis to derive NO densities [NO] are determined from OSIRIS O 2 (b 1 Σ + g - X 3 Σ - g ) 0-0 band night airglow observations and from Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS) sunset ozone observations. The derived Southern Hemisphere [O] map that shows pronounced longitudinal variation, maximum of 7 × 10 11 cm -3 , considerably exceeding MSIS model values, and suggests significant dynamical influence. Combining the continuum observations and the derived [O], a hemispheric map of derived [NO] is assembled that also shows considerable spatial variation, maximum of 1.1 × 10 9 cm 3 measurement uncertainty of 3 × 10 7 cm -3 . Comparing the two maps, the geographical distribution of [NO] differs considerably from that of [O]. From a qualitative comparison, the distribution of derived [NO] is similar to that in coordinated GUVI LBH1 auroral precipitation images. The OSIRIS-derived [NO] agrees with the measured ACE-FTS [NO] to within 1 × 10 8 cm -3 . The estimated systematic uncertainty of the NO densities derived from OSIRIS observations is approximately 30%.

Four Fourier transform spectrometers and the Arctic polar vortex: instrument intercomparison and ACE-FTS validation at Eureka during the IPY springs of 2007 and 2008

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.

What causes the irregular cycle of the atmospheric tape recorder signal in HCN

Abstract: Received 27 May 2010; accepted 8 July 2010; published 20 August 2010. [1] Variations in the mixing ratio of long‐lived trace gases entering the stratosphere in the tropics are carried upward with the rising air with the signal being observable throughout the tropical lower stratosphere. This phenomenon, referred to as “atmospheric tape recorder” has previously been observed for water vapor, CO2 ,a nd CO which exhibit an annual cycle. Recently, based on Microwave Limb Sounder (MLS) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE‐ FTS) satellite measurements, the tape recorder signal has been observed for hydrogen cyanide (HCN) but with an approximately two‐year period. Here we report on a model simulation of the HCN tape recorder for the time period 2002–2008 using the Chemical Lagrangian Model of the Stratosphere (CLaMS). The model can reproduce the observed pattern of the HCN tape recorder signal if time‐resolved emissions from fires in Indonesia are used as lower boundary condition. This finding indicates that inter‐annual variations in biomass burning in Indonesia, which are strongly influenced by El Nino events, control the HCN tape recorder signal. A longer time series of tropical HCN data will probably exhibit an irregular cycle rather than a regular biannual cycle. Citation: Pommrich, R., R. Muller, J.-U. Groos, G. Gunther, P. Konopka, M. Riese, A. Heil, M. Schultz, H.-C. Pumphrey, and K. A. Walker (2010), What causes the irregular cycle of the atmospheric tape recorder signal in HCN?, Geophys. Res. Lett., 37, L16805, doi:10.1029/ 2010GL044056.

Validating the reported random errors of ACE‐FTS measurements

Abstract: In order to validate the reported precision of space-based atmospheric composition measurements, validation studies often focus on measurements in the tropical stratosphere, where natural variability is weak. The scatter in tropical measurements can then be used as an upper limit on single-profile measurement precision. Here we introduce a method of quantifying the scatter of tropical measurements which aims to minimize the effects of short-term atmospheric variability while maintaining large enough sample sizes that the results can be taken as representative of the full data set. We apply this technique to measurements of O(3), HNO(3), CO, H(2)O, NO, NO(2), N(2)O, CH(4), CCl(2)F(2), and CCl(3)F produced by the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS). Tropical scatter in the ACE-FTS retrievals is found to be consistent with the reported random errors (RREs) for H(2)O and CO at altitudes above 20 km, validating the RREs for these measurements. Tropical scatter in measurements of NO, NO(2), CCl(2)F(2), and CCl(3)F is roughly consistent with the RREs as long as the effect of outliers in the data set is reduced through the use of robust statistics. The scatter in measurements of O(3), HNO(3), CH(4), and N(2)O in the stratosphere, while larger than the RREs, is shown to be consistent with the variability simulated in the Canadian Middle Atmosphere Model. This result implies that, for these species, stratospheric measurement scatter is dominated by natural variability, not random error, which provides added confidence in the scientific value of single-profile measurements.

Updating hydrogen fluoride (HF) FTIR time series above Jungfraujoch: comparison of two retrieval algorithms and impact of line shape models

Abstract: (1) University of Liège, Institute of Astrophysics and Geophysics, Liège, Belgium (p.duchatelet@ulg.ac.be), (2) Karlsruhe Institute of Technology, Institute for Meteorology and Climate Research (IMK-ASF), Karlsruhe, Germany, (3) Department of Chemistry, University of York, Heslington, UK, (4) Department of Chemistry, University of Waterloo, Waterloo, Canada, (5) Department of Physics, University of Toronto, Toronto, Canada

A Climatological Data Set from the ACE-FTS instrument for the period of 2004-2009

Abstract: (1) University of Toronto, Physics, Toronto, Ontario, Canada (kwalker@atmosp.physics.utoronto.ca, 416 978 8905), (2) Department of Chemistry, University of Waterloo, Waterloo, Ontario, Canada, (3) Jet Propulsion Laboratory, California Institute of Technology, Pasadena, California, U.S.A., (4) National Center for Atmospheric Research, Boulder, Colorado, U.S.A., (5) Department of Chemistry, University of York, Heslington, York, United Kingdom, (6) Also at New Mexico Institute of Mining and Technology, Socorro, New Mexico, U.S.A.