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Boone, Chris D.

Publications and source records attributed to Boone, Chris D..

Model Sensitivity Studies of the Decrease in Atmospheric Carbon Tetrachloride

Carbon tetrachloride (CCl4) is an ozone-depleting substance, which is controlled by the Montreal Protocol and for which the atmospheric abundance is decreasing. However, the current observed rate of this decrease is known to be slower than expected based on reported CCl4 emissions and its estimated overall atmospheric lifetime. Here we use a three-dimensional (3-D) chemical transport model to investigate the impact on its predicted decay of uncertainties in the rates at which CCl4 is removed from the atmosphere by photolysis, by ocean uptake and by degradation in soils. The largest sink is atmospheric photolysis (74% of total), but a reported 10% uncertainty in its combined photolysis cross section and quantum yield has only a modest impact on the modelled rate of CCl4 decay. This is partly due to the limiting effect of the rate of transport of CCl4 from the main tropospheric reservoir to the stratosphere, where photolytic loss occurs. The model suggests large interannual variability in the magnitude of this stratospheric photolysis sink caused by variations in transport. The impact of uncertainty in the minor soil sink (9%of total) is also relatively small. In contrast, the model shows that uncertainty in ocean loss (17%of total) has the largest impact on modelled CCl4 decay due to its sizeable contribution to CCl4 loss and large lifetime uncertainty range (147 to 241 years). With an assumed CCl4 emission rate of 39 Gg year(exp -1), the reference simulation with the best estimate of loss processes still underestimates the observed CCl4 (overestimates the decay) over the past 2 decades but to a smaller extent than previous studies. Changes to the rate of CCl4 loss processes, in line with known uncertainties, could bring the model into agreement with in situ surface and remote-sensing measurements, as could an increase in emissions to around 47 Gg year(exp -1). Further progress in constraining the CCl4 budget is partly limited by systematic biases between observational datasets. For example, surface observations from the National Oceanic and Atmospheric Administration (NOAA) network are larger than from the Advanced Global Atmospheric Gases Experiment (AGAGE) network but have shown a steeper decreasing trend over the past 2 decades. These differences imply a difference in emissions which is significant relative to uncertainties in the magnitudes of the CCl4 sinks.

Carbon Trechloride

First Global Observations of Atmospheric COCIF from the Atmospheric Chemistry Experiment Mission

Carbonyl chlorofluoride (COCIF) is an important reservoir of chlorine and fluorine in the Earth's atmosphere. Satellite-based remote sensing measurements of COCIF, obtained by the Atmospheric Chemistry Experiment (ACE) for a time period spanning February 2004 through April 2007, have been used in a global distribution study. There is a strong source region for COCIF in the tropical stratosphere near 27 km. A layer of enhanced COCIF spans the low- to mid-stratosphere over all latitudes, with volume mixing ratios of 40-100 parts per trillion by volume, largest in the tropics and decreasing toward the poles. The COCIF volume mixing ratio profiles are nearly zonally symmetric, but they exhibit a small hemispheric asymmetry that likely arises from a hemispheric asymmetry in the parent molecule CCl3 F. Comparisons are made with a set of in situ stratospheric measurements from the mid-1980s and with predictions from a 2-D model.

Fu, Dejian

First Global Observations of Atmospheric COClF from the Atmospheric Chemistry Experiment Mission

Carbonyl chlorofluoride (COClF) is an important reservoir of chlorine and fluorine in the Earth's atmosphere. Satellite-based remote sensing measurements of COClF, obtained by the Atmospheric Chemistry Experiment (ACE) for a time period spanning February 2004 through April 2007, have been used in a global distribution study. There is a strong source region for COClF in the tropical stratosphere near 27 km. A layer of enhanced COClF spans the low- to mid-stratosphere over all latitudes, with volume mixing ratios of 40-100 parts per trillion by volume, largest in the tropics and decreasing toward the poles. The COClF volume mixing ratio profiles are nearly zonally symmetric, but they exhibit a small hemispheric asymmetry that likely arises from a hemispheric asymmetry in the parent molecule CCl3F. Comparisons are made with a set of in situ stratospheric measurements from the mid-1980s and with predictions from a 2-D model.

Fu, Dejian

Appendix C: First Global Observations of Atmospheric COClF from the Atmospheric Chemistry Experiment Mission

Carbonyl chlorofluoride (COCIF) is an important reservoir of chlorine and Fluorine in the Earth's atmosphere. Satellite-based remote sensing measurements of COCIF, obtained by Received in revised form the Atmospheric Chemistry Experiment (ACE) for a time period spanning February 2004 through April 2007, have been used in a global distribution study. There is a strong Accepted 18 February 2009 source region for COCIF in the tropical stratosphere near 27 km. A layer of enhanced COCIF spans the low- to mid-stratosphere over all latitudes, with volume mixing ratios of 40-100 parts Per trillion by volume, largest in the tropics and decreasing toward the poles. The COCIF volume mixing ratio profiles are nearly zonally symmetric, but they exhibit a small hemispheric asymmetry that likely arises from a hemispheric asymmetry in the parent molecule CCl3F. Comparisons are made with a set of in situ stratospheric measurements from the mid-1980s and with predictions from a 2-D model.

Fu, Djian

Satellite Boreal Measurements over Alaska and Canada During June-July 2004: Simultaneous Measurements of Upper Tropospheric CO, C2H6, HCN, CH3Cl, CH4, C2H2, CH2OH, HCOOH, OCS, and SF6 Mixing Ratios

Simultaneous ACE (Atmospheric Chemistry Experiment) upper tropospheric CO, C2H6, HCN, CH3Cl, CH4 , C2H2 , CH30H, HCOOH, and OCS measurements show plumes up to 185 ppbv (10 (exp -9) per unit volume) for CO, 1.36 ppbv for C2H6, 755 pptv (10(exp -12) per unit volume) for HCN, 1.12 ppbv for CH3C1, 1.82 ppmv, (10(exp -6) per unit volume) for CH4, 0.178 ppbv for C2H2, 3.89 ppbv for CH30H, 0.843 ppbv for HCOOH, and 0.48 ppbv for OCS in western Canada and Alaska at 50 deg N-68 deg N latitude between 29 June and 23 July 2004. Enhancement ratios and emission factors for HCOOH, CH30H, HCN, C2H6, and OCS relative to CO at 250-350 hPa are inferred from measurements of young plumes compared with lower mixing ratios assumed to represent background conditions based on a CO emission factor derived from boreal measurements. Results are generally consistent with the limited data reported for various vegetative types and emission phases measured in extratropical forests including boreal forests. The low correlation between fire product emission mixing ratios and the S176 mixing ratio is consistent with no significant SF6 emissions from the biomass fires.

Rinsland, Curtis P.

Spectroscopic Detection of COClF in the Tropical and Mid-Latitude Lower Stratosphere

We report retrievals of COClF (carbonyl chlorofluoride) based on atmospheric chemistry experiment (ACE) solar occultation spectra recorded at tropical and mid-latitudes during 2004-2005. The COClF molecule is a temporary reservoir of both chlorine and fluorine and has not been measured previously by remote sensing. A maximum COClF mixing ratio of 99.7+/-48.0 pptv (10(exp -12) per unit volume, 1 sigma) is measured at 28km for tropical and subtropical occultations (latitudes below 20deg in both hemispheres) with lower mixing ratios at both higher and lower altitudes. Northern hemisphere mid-latitude mixing ratios (30-50degN) resulted in an average profile with a peak mixing ratio of 51.7+/-32.1 pptv, 1 sigma, at 27 km, also decreasing above and below that altitude. We compare the measured average profiles with the one reported set of in situ lower stratospheric mid-latitude measurements from 1986 and 1987, a previous two-dimensional (2-D) model calculation for 1987 and 1993, and a 2-D-model prediction for 2004. The measured average tropical profile is in close agreement with the model prediction; the northern mid-latitude profile is also consistent, although the peak in the measured profile occurs at a higher altitude (2.5-4.5km offset) than in the model prediction. Seasonal average 2-D-model predictions of the COClF stratospheric distribution for 2004 are also reported.

Rinsland, Curtis P.

ACE-FTS Observation of a Young Biomass Burning Plume: First Reported Measurements of C2H4, C3H6O, H2CO and PAN by Infrared Occultation from Space

In the course of our study of the upper tropospheric composition with the infrared 35 Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE FTS), we 36 found an occultation sequence that on 8 October 2005, sampled a remarkable plume near the 37 east coast of Tanzania. Model simulations of the CO distribution in the Southern hemisphere 38 are performed for this period and they demonstrate that the emissions for this event originated 39 from a nearby forest fire, after which the plume was transported from the source region to the 40 upper troposphere. Taking advantage of the very high signal-to-noise ratio of the ACE FTS 41 spectra over a wide wavenumber range (750-4400 cm(exp -1), we present in-depth analyses of the 42 chemical composition of this plume in the middle and upper troposphere, focusing on the 43 measurements of weakly absorbing pollutants. For this specific biomass burning event, we 44 report simultaneous observations of an unprecedented number of organic species. 45 Measurements of C2H4 (ethene), C3H4 (propyne), H2CO (formaldehyde), C3H6O (acetone) 46 and CH3COO2NO2 (perxoxyacetylnitrate, abbreviated as PAN) are the first reported 47 detections using infrared occultation spectroscopy from satellites. Based on the lifetime of the 48 emitted species, we discuss the photochemical age of the plume and also report, whenever 49 possible, the enhancement ratios relative to CO.

Coheur, Pierre-Francois

Early Validation Analyses of Atmospheric Profiles from EOS MLS on the Aura Satellite

We present results of early validation studies using retrieved atmospheric profiles from the Earth Observing System Microwave Limb Sounder (MLS) instrument on the Aura satellite. 'Global' results are presented for MLS measurements of atmospheric temperature, ozone, water vapor, hydrogen chloride, nitrous oxide, nitric acid, and carbon monoxide, with a focus on the January-March 2005 time period. These global comparisons are made using long-standing global satellites and meteorological datasets, as well as some measurements from more recently launched satellites. Comparisons of MLS data with measurements from the Ft. Sumner, NM, September 2004 balloon flights are also presented. Overall, good agreeement is obtained, often within 5% to 10%, but we point out certain issues to resolve and some larger systematic differences; some artifacts in the first publicly released MLS (version 1.5) dataset are noted.We comment briefly on future plans for validation and software improvements.

Atmospheric retrievals