Kimberly Strong

Atmospheric Chemistry Experiment (ACE): Mission overview

SCISAT-1, also known as the Atmospheric Chemistry Experiment (ACE), is a Canadian satellite mission for remote sensing of the Earths atmosphere. It was launched into low Earth circular orbit (altitude 650 km, inclination 74°) on 12 Aug. 2003. The primary ACE instrument is a high spectral resolution (0.02 cm-1) Fourier Transform Spectrometer (FTS) operating from 2.2 to 13.3 μm (750-4400 cm-1). The satellite also features a dual spectrophotometer known as MAESTRO with wavelength coverage of 285-1030 nm and spectral resolution of 1-2 nm. A pair of filtered CMOS detector arrays records images of the Sun at 0.525 and 1.02 μm. Working primarily in solar occultation, the satellite provides altitude profile information (typically 10-100 km) for temperature, pressure, and the volume mixing ratios for several dozen molecules of atmospheric interest, as well as atmospheric extinction profiles over the latitudes 85°N to 85°S. This paper presents a mission overview and some of the first scientific results. Copyright 2005 by the American Geophysical Union.

Process-evaluation of tropospheric humidity simulated by general circulation models using water vapor isotopologues: 1. Comparison between models and observations

The goal of this study is to determine how H2O and HDO measurements in water vapor can be used to detect and diagnose biases in the representation of processes controlling tropospheric humidity in atmospheric general circulation models (GCMs). We analyze a large number of isotopic data sets (four satellite, sixteen ground-based remote-sensing, five surface in situ and three aircraft data sets) that are sensitive to different altitudes throughout the free troposphere. Despite significant differences between data sets, we identify some observed HDO/H2O characteristics that are robust across data sets and that can be used to evaluate models. We evaluate the isotopic GCM LMDZ, accounting for the effects of spatiotemporal sampling and instrument sensitivity. We find that LMDZ reproduces the spatial patterns in the lower and mid troposphere remarkably well. However, it underestimates the amplitude of seasonal variations in isotopic composition at all levels in the subtropics and in midlatitudes, and this bias is consistent across all data sets. LMDZ also underestimates the observed meridional isotopic gradient and the contrast between dry and convective tropical regions compared to satellite data sets. Comparison with six other isotope-enabled GCMs from the SWING2 project shows that biases exhibited by LMDZ are common to all models. The SWING2 GCMs show a very large spread in isotopic behavior that is not obviously related to that of humidity, suggesting water vapor isotopic measurements could be used to expose model shortcomings. In a companion paper, the isotopic differences between models are interpreted in terms of biases in the representation of processes controlling humidity. Copyright

Spectral parameters of self- and hydrogen-broadened methane from 2000 to 9500 cm-1 for remote sounding of the atmosphere of Jupiter

Abstract Long-pathlength self- and H 2 -broadened absorption spectra of CH 4 have been recorded from 2000 to 9500 cm -1 at a resolution of 0.25 cm -1 . Thesespectra were obtained for a wide range of conditions relevant to the atmosphere of Jupiter, including nominal temperatures of 190, 240, and 296 K, pathlenghts from 64 to 512 m, and pressures from 0.2 to 700 torr, giving CH 4 column abundances from 0.016 to 530 m-amagat. A series of molecular band models were fitted to these spectra at 10 cm -1 resolution, showingthat the Goody and Malkmus random band models with the Voigt lineshape provided the best fits to the data. The Goody-Voigt model was subsequently used to calculate the level in the Jovian atmosphere that will be sounded by observations of CH 4 absorption, and estimates were made of the accuracy to be expected if this model were used to retrieve atmospheric parameters.

Polar vortex evolution during the 2002 Antarctic major warming as observed by the Odin satellite

In September 2002 the Antarctic polar vortex split in two under the influence of a sudden warming. During this event, the Odin satellite was able to measure both ozone (O3) and chlorine monoxide (ClO), a key constituent responsible for the so-called “ozone hole”, together with nitrous oxide (N2O), a dynamical tracer, and nitric acid (HNO3) and nitrogen dioxide (NO2), tracers of denitrification. The submillimeter radiometer (SMR) microwave instrument and the Optical Spectrograph and Infrared Imager System (OSIRIS) UV-visible light spectrometer (VIS) and IR instrument on board Odin have sounded the polar vortex during three different periods: before (19–20 September), during (24–25 September), and after (1–2 and 4–5 October) the vortex split. Odin observations coupled with the Reactive Processes Ruling the Ozone Budget in the Stratosphere (REPROBUS) chemical transport model at and above 500 K isentropic surfaces (heights above 18 km) reveal that on 19–20 September the Antarctic vortex was dynamically stable and chemically nominal: denitrified, with a nearly complete chlorine activation, and a 70% O3 loss at 500 K. On 25–26 September the unusual morphology of the vortex is monitored by the N2O observations. The measured ClO decay is consistent with other observations performed in 2002 and in the past. The vortex split episode is followed by a nearly complete deactivation of the ClO radicals on 1–2 October, leading to the end of the chemical O3 loss, while HNO3 and NO2 fields start increasing. This acceleration of the chlorine deactivation results from the warming of the Antarctic vortex in 2002, putting an early end to the polar stratospheric cloud season. The model simulation suggests that the vortex elongation toward regions of strong solar irradiance also favored the rapid reformation of ClONO2. The observed dynamical and chemical evolution of the 2002 polar vortex is qualitatively well reproduced by REPROBUS. Quantitative differences are mainly attributable to the too weak amounts of HNO3 in the model, which do not produce enough NO2 in presence of sunlight to deactivate chlorine as fast as observed by Odin.

Global CO2 fluxes inferred from surface air-sample measurements and from TCCON retrievals of the CO2 total column

We present the first estimate of the global distribution of CO_2 surface fluxes from 14 stations of the Total Carbon Column Observing Network (TCCON). The evaluation of this inversion is based on 1) comparison with the fluxes from a classical inversion of surface air-sample-measurements, and 2) comparison of CO_2 mixing ratios calculated from the inverted fluxes with independent aircraft measurements made during the two years analyzed here, 2009 and 2010. The former test shows similar seasonal cycles in the northern hemisphere and consistent regional carbon budgets between inversions from the two datasets, even though the TCCON inversion appears to be less precise than the classical inversion. The latter test confirms that the TCCON inversion has improved the quality (i.e., reduced the uncertainty) of the surface fluxes compared to the assumed or prior fluxes. The consistency between the surface-air-sample-based and the TCCON-based inversions despite remaining flaws in transport models opens the possibility of increased accuracy and robustness of flux inversions based on the combination of both data sources and confirms the usefulness of space-borne monitoring of the CO_2 column.

Stratospheric profiles of nitrogen dioxide observed by Optical Spectrograph and Infrared Imager System on the Odin satellite

[1] Vertical profiles of nitrogen dioxide in the 19–40 km altitude range are successfully retrieved over the globe from Optical Spectrograph and Infrared Imager System (OSIRIS) limb scatter observations in late 2001 and early 2002. The inclusion of multiple scattering in the radiative transfer model used in the inversion algorithm allows for the retrieval of NO2 down to 19 km. The slant column densities, which represent the observations in the inversion, are obtained by fitting the fine structure in normalized radiance spectra over the 435–449 nm range, where NO2 electronic absorption is readily observable because of long light paths through stratospheric layers rich in this constituent. Details of the spectral fitting and inversion algorithm are discussed, including the discovery of a pseudo-absorber associated with pixelated detectors and a new method to verify altitude registration. Comparisons are made with spatially and temporally coincident profile measurements of this photochemically active trace gas. Better than 20% agreement is obtained with all correlative measurements over the common retrieval altitude range, confirming the validity of OSIRIS NO2 profiles. Systematic biases in the number densities are not observed at any altitude. A ‘‘snapshot’’ meridional cross section between 40� N and 70� S is shown from observations during a fraction of an orbit. INDEX TERMS: 0340 Atmospheric Composition and Structure: Middle atmosphere—composition and chemistry; 0360 Atmospheric Composition and Structure: Transmission and scattering of radiation; 0394 Atmospheric Composition and Structure: Instruments and techniques; 3334 Meteorology and Atmospheric Dynamics: Middle atmosphere dynamics (0341, 0342); KEYWORDS: optical, Sun-synchronous, polar-orbiting, Fraunhofer, Ring effect, iterative onion peel

Detection of stratospheric ozone intrusions by windprofiler radars

Stratospheric ozone attenuates harmful ultraviolet radiation and protects the Earth’s biosphere. Ozone is also of fundamental importance for the chemistry of the lowermost part of the atmosphere, the troposphere. At ground level, ozone is an important by-product of anthropogenic pollution, damaging forests and crops, and negatively affecting human health. Ozone is critical to the chemical and thermal balance of the troposphere because, via the formation of hydroxyl radicals, it controls the capacity of tropospheric air to oxidize and remove other pollutants. Moreover, ozone is an important greenhouse gas, particularly in the upper troposphere. Although photochemistry in the lower troposphere is the major source of tropospheric ozone, the stratosphere–troposphere transport of ozone is important to the overall climatology, budget and long-term trends of tropospheric ozone. Stratospheric intrusion events, however, are still poorly understood. Here we introduce the use of modern windprofiler radars to assist in such transport investigations. By hourly monitoring the radar-derived tropopause height in combination with a series of frequent ozonesonde balloon launches, we find numerous intrusions of ozone from the stratosphere into the troposphere in southeastern Canada. On some occasions, ozone is dispersed at altitudes of two to four kilometres, but on other occasions it reaches the ground, where it can dominate the ozone density variability. We observe rapid changes in radar tropopause height immediately preceding these intrusion events. Such changes therefore serve as a valuable diagnostic for the occurrence of ozone intrusion events. Our studies emphasize the impact that stratospheric ozone can have on tropospheric ozone, and show that windprofiler data can be used to infer the possibility of ozone intrusions, as well as better represent tropopause motions in association with stratosphere–troposphere transport.

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...

Evaluating ethane and methane emissions associated with the development of oil and natural gas extraction in North America

Sharp rises in the atmospheric abundance of ethane (C2H6)have been detected from2009 onwards in theNorthernHemisphere as a result of the unprecedented growth in the exploitation of shale gas and tight oil reservoirs inNorthAmerica. Using time series of C2H6 total columns derived from groundbased Fourier transform infrared (FTIR) observationsmade atfive selectedNetwork for theDetection of Atmospheric CompositionChange sites, we characterize the recent C2H6 evolution and determine growth rates of∼5% yr atmid-latitudes and of∼3% yr at remote sites. Results fromCAM-chem simulations with theHemispheric Transport of Air Pollutants, Phase II bottom-up inventory for anthropogenic emissions are found to greatly underestimate the current C2H6 abundances. Doubling global emissions is required to reconcile the simulations and the observations prior to 2009.We further estimate thatNorthAmerican anthropogenic C2H6 emissions have increased from1.6 Tg yr −1 in 2008 to 2.8 Tg yr in 2014, i.e. by 75%over these six years.We also completed a second simulation with new top-down emissions of C2H6 fromNorthAmerican oil and gas activities, biofuel consumption and biomass burning, inferred from space-borne observations ofmethane (CH4) from GreenhouseGasesObserving SATellite. In this simulation, GEOS-Chem is able to reproduce FTIR measurements at themid-latitudinal sites, underscoring the impact of theNorthAmerican oil and gas development on the current C2H6 abundance. Finally we estimate that theNorthAmerican oil and gas emissions of CH4, amajor greenhouse gas, grew from20 to 35 Tg yr −1 over the period 2008–2014, in associationwith the recent C2H6 rise.

Ground-Based Solar Absorption FTIR Spectroscopy: Characterization of Retrievals and First Results from a Novel Optical Design Instrument at a New NDACC Complementary Station

Abstract The authors describe the optical design of a high-resolution Fourier Transform Spectrometer (FTS), which serves as the primary instrument at the University of Toronto Atmospheric Observatory (TAO). The FTS is dedicated to ground-based infrared solar absorption atmospheric measurements from Toronto, Ontario, Canada. Instrument performance is discussed in terms of instrumental line shape (ILS) and phase error and modulation efficiency as a function of optical path difference. Typical measurement parameters are presented together with retrieval parameters used to derive total and partial column concentrations of ozone. Retrievals at TAO employ the optimal estimation method (OEM), and some impacts of the necessary a priori constraints are examined. In March 2004, after participating in a retrieval algorithm user intercomparison exercise, the TAO FTS was granted the status of a Complementary Observation Station within the international community of high-resolution FTS users in the Network for the Dete...