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Introduction
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Publications
Publications (116)
UCATS (the UAS Chromatograph for Atmospheric Trace Species) was designed and built for observations of important atmospheric trace gases from unmanned aircraft systems (UAS) in the upper troposphere and lower stratosphere (UT/LS). Initially it measured major chlorofluorocarbons (CFCs) and the stratospheric transport tracers nitrous oxide (N2O) and...
The recovery of the stratospheric ozone layer relies on the continued decline in the atmospheric concentrations of ozone-depleting gases such as chlorofluorocarbons¹. The atmospheric concentration of trichlorofluoromethane (CFC-11), the second-most abundant chlorofluorocarbon, has declined substantially since the mid-1990s². A recently reported slo...
The Montreal Protocol was designed to protect the stratospheric ozone layer by enabling reductions in the abundance of ozone-depleting substances such as chlorofluorocarbons (CFCs) in the atmosphere. The reduction in the atmospheric concentration of trichlorofluoromethane (CFC-11) has made the second-largest contribution to the decline in the total...
We present top-down constraints on global monthly N2O emissions for 2011 from a multi-inversion approach and an ensemble of surface observations. The inversions employ the GEOS-Chem adjoint and an array of aggregation strategies to test how well current observations can constrain the spatial distribution of global N2O emissions. The strategies incl...
We present top-down constraints on global, monthly N2O emissions for 2011 from a multi-inversion approach and an ensemble of surface observations. The inversions employ the GEOS-Chem adjoint and an array of aggregation strategies to test how well current observations can constrain the spatial distribution of global N2O emissions. The strategies inc...
Ch 7. Regional Climates: f. Europe and the Middle East
Profiles of CFC-11 (CCl3F) and CFC-12 (CCl2F2) of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) aboard the European satellite Envisat have been retrieved from versions MIPAS/4.61 to MIPAS/4.62 and MIPAS/5.02 to MIPAS/5.06 level-1b data using the scientific level-2 processor run by Karlsruhe Institute of Technology (KIT), Ins...
We report ground-based atmospheric measurements and emission estimates for the halons H-1211 (CBrClF2), H-1301 (CBrF3), and H-2402 (CBrF2CBrF2) from the AGAGE (Advanced Global Atmospheric Gases Experiment) and the NOAA (National Oceanic and Atmospheric Administration) global networks. We also include results from archived air samples in canisters a...
Significance
Global-scale observations suggest large unexplained emissions of the ozone-depleting chemical carbon tetrachloride (CCl 4 ) despite stringent limits on its production for dispersive uses for many years. Identifying the sources of continued CCl 4 emission is necessary before steps can be taken to accelerate the emission decline and limi...
Profiles of CFC-11 (CCl3F) and CFC-12 (CCl2F2) of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) abord the European satellite Envisat have been retrieved from versions MIPAS/4.61–MIPAS/4.62 and MIPAS/5.02–MIPAS/5.06 level-1b data using the scientific level-2 processor run by Karlsruhe Institute of Technology (KIT), Institute...
We describe a new 4D-Var inversion framework for nitrous oxide (N2O) based on the GEOS-Chem chemical transport model and its adjoint, and apply it in a series of observing system simulation experiments to assess how well N2O sources and sinks can be constrained by the current global observing network. The employed measurement ensemble includes appr...
Ambient levels and variability of major atmospheric halocarbons, i.e. CFC-12, CFC-11, CFC-113, CCl4, CH3CCl3, C2HCl3, and C2Cl4 in a major metropolis (Taipei, Taiwan) were re-investigated after fourteen years by flask sampling in 2012. Our data indicates that the variability expressed as standard deviations (SD) of CFC-113 and CCl4 remained small (...
Chlorofluorocarbons (CFCs) play a key role in stratospheric ozone loss and are strong infrared absorbers that contribute to global warming. The stratospheric lifetimes of CFCs are a measure of their stratospheric loss rates that are needed to determine global warming and ozone depletion potentials. We applied the tracer–tracer correlation approach...
Chlorofluorocarbons (CFCs) play a key role in stratospheric ozone
loss and are strong infrared absorbers that contribute to global
warming. The stratospheric lifetimes of CFCs are a measure of their
stratospheric loss rates that are needed to determine global warming
and ozone depletion potentials. We applied the tracer–tracer
correlation approach...
Carbon tetrachloride (CCl4) is a major anthropogenic ozone-depleting substance and greenhouse gas and has been regulated under the Montreal Protocol. However, the near-zero 2007-2012 emissions estimate based on the UNEP reported production and feedstock usage cannot be reconciled with the observed slow decline of atmospheric concentrations and the...
We present a comprehensive estimate of nitrous oxide (N[subscript 2]O) emissions using observations and models from 1995 to 2008. High-frequency records of tropospheric N[subscript 2]O are available from measurements at Cape Grim, Tasmania; Cape Matatula, American Samoa; Ragged Point, Barbados; Mace Head, Ireland; and at Trinidad Head, California u...
We present a comprehensive estimate of nitrous oxide (N2O) emissions using observations and models from 1995 to 2008. High-frequency records of tropospheric N2O are available from measurements at Cape Grim, Tasmania; Cape Matatula, American Samoa; Ragged Point, Barbados; Mace Head, Ireland; and at Trinidad Head, California using the Advanced Global...
N2O surface fluxes were estimated for 1999 to 2009 using a
time-dependent Bayesian inversion technique. Observations were drawn from 5
different networks, incorporating 59 surface sites and a number of ship-based
measurement series. To avoid biases in the inverted fluxes, the data were
adjusted to a common scale and scale offsets were included in t...
The tropospheric seasonal cycles of N2O, CFC-11 (CCl3F), and CFC-12 (CCl2F2) are
influenced by atmospheric dynamics. The interannually varying summertime minima in mole
fractions of these trace gases have been attributed to interannual variations in mixing of
stratospheric air (depleted in CFCs and N2O) with tropospheric air with a few months lag....
Observations of SF6 are used to quantify the mean time since air was in (“mean age” from) the Northern Hemisphere (NH) midlatitude surface layer. The mean age is a fundamental property of tropospheric transport that can be used in theoretical studies and used to evaluate transport in comprehensive models. Comparisons of simulated SF6 and an idealiz...
of tropospheric N2O mixing ratio show significant variability
on interannual timescales (0.2 ppb, 1 standard deviation). We found that
interannual variability in N2O is weakly correlated with that
in CFC-12 and SF6 for the northern extratropics and more
strongly correlated for the southern extratropics, suggesting that
interannual variability in al...
Since the Montreal Protocol on Substances that Deplete the Ozone Layer and its amendments came into effect, growth rates of the major ozone depleting substances (ODS), particularly CFC-11, -12 and -113 and CH[subscript 3]CCl[subscript 3], have declined markedly, paving the way for global stratospheric ozone recovery. Emissions have now fallen to re...
For the first time in serveral years, the El Nino-Southern Oscillation did not dominate regional climate conditions around the globe. A weak La Ni a dissipated to ENSOneutral conditions by spring, and while El Nino appeared to be emerging during summer, this phase never fully developed as sea surface temperatures in the eastern conditions. Neverthe...
N2O surface fluxes were estimated for 1999 to 2009 using a
time-dependent Bayesian inversion technique. Observations were drawn
from 5 different networks, incorporating 59 surface sites and a number
of ship-based measurement series. To avoid biases in the inverted
fluxes, the data were adjusted to a common scale and scale offsets were
included in t...
Since the Montreal Protocol on substances that deplete the ozone layer
and its amendments came into effect, growth rates of the major ozone
depleting substances (ODS), particularly CFC-11, -12 and -113 and
CH3CCl3, have declined markedly, paving the way
for global stratospheric ozone recovery. Emissions have now fallen to
relatively low levels, the...
Vertical profiles of CFC-11 (CCl3F) and CFC-12
(CCl2F2) have been measured with the Michelson
Interferometer for Passive Atmospheric Sounding (MIPAS) with global
coverage under daytime and nighttime conditions. The profile retrieval
is based on constrained nonlinear least squares fitting of measured limb
spectral radiance to modeled spectra. CFC-11...
Since the Montreal Protocol on substances that deplete the ozone layer and its amendments came into effect, growth rates of the major ozone depleting substances (ODS), particularly CFC-11, -12 and -113 and CH3CCl3, have declined markedly, paving the way for global stratospheric ozone recovery. Emissions have now fallen to relatively low levels, the...
Vertical profiles of CFC-11 (CFCl3) and CFC-12
(CF2Cl2) have been measured with the Michelson
Interferometer for Passive Atmospheric Sounding (MIPAS) with global
coverage under daytime and nighttime conditions. The profile retrieval
is based on constrained nonlinear least squares fitting of measured limb
spectral radiance to modeled spectra. CFC-11...
Elevated mixing ratios of chlorofluorocarbons (CFC-11 and CFC-12), and sulfur hexafluoride (SF6) have been observed at Lamont-Doherty Earth Observatory (LDEO), located approximately 25 km north of New York City (NYC). Emissions and transport of these gases are of interest because of their global warming potential, the role of CFCs in depletion of s...
One of the important potential uses of the NASA Global Hawk Unmanned
Aircraft System (UAS) in scientific research is to study stratospheric
ozone (O3) depletion in polar regions. Manned flights involve
remote and hazardous duty, which pose great risks to pilots, crew, and
scientists. Arctic ozone depletion observed in the spring of 2010 by
satellit...
Nitrous oxide (N2O) emissions weighted by ozone depletion potential
currently dominate emissions of ozone depleting substances, and N2O is
now the third most significant long-lived anthropogenic greenhouse gas
after CO2 and CH4. Despite its impact on stratospheric ozone
destruction, it is not regulated under the Montreal Protocol, and global
observ...
The Arctic tundra plays an active role in the biogeochemical cycling of
ozone-depleting halocarbons. One of these compounds, chloroform
(CHCl3), is emitted at high rates from the tundra but only
during the thaw season. Thus atmospheric CHCl3 measurements
can be used as an indicator of seasonal transitions on the tundra. We
tested this idea through...
Sulfur hexafluoride (SF6) is a potent greenhouse gas and useful atmospheric tracer. Measurements of SF6 on global and regional scales are necessary to estimate emissions and to verify or examine the performance of atmospheric transport models. Typical precision for common gas chromatographic methods with electron capture detection (GC-ECD) is 1-2 %...
Seasonal cycles in the mixing ratios of tropospheric nitrous oxide (N2O) are derived by detrending long-term measurements made at sites across four global surface monitoring networks. The detrended monthly data display large interannual variability, which at some sites challenges the concept of a "mean" seasonal cycle. In the Northern Hemisphere, c...
We present atmospheric sulfur hexafluoride (SF6)[SF subscript 6] mole fractions and emissions estimates from the 1970s to 2008. Measurements were made of archived air samples starting from 1973 in the Northern Hemisphere and from 1978 in the Southern Hemisphere, using the Advanced Global Atmospheric Gases Experiment (AGAGE) gas chromatographic-mass...
Several large-scale climate patterns influenced climate conditions and weather patterns across the globe during 2010. The transition from a warm El Niño phase at the beginning of the year to a cool La Niña phase by July contributed to many notable events, ranging from record wetness across much of Australia to historically low Eastern Pacific basin...
Several large-scale climate patterns influenced climate conditions and weather patterns across the globe during 2010. The transition from a warm El Nino phase at the beginning of the year to a cool La Nina phase by July contributed to many notable events, ranging from record wetness across much of Australia to historically low Eastern Pacific basin...
Several large-scale climate patterns influenced climate conditions and weather patterns across the globe during 2010. The transition from a warm El Nino phase at the beginning of the year to a cool La Nina phase by July contributed to many notable events, ranging from record wetness across much of Australia to historically low Eastern Pacific basin...
In the mid-1970s, the National Oceanic and Atmospheric Administration's (NOAA) Geophysical Monitoring for Climate Change (GMCC) program made a commitment to measure and monitor trace gases including carbon dioxide, methane, nitrous oxide (N2O) and chlorofluorocarbons (CFCs). Over the next three decades GMCC grew into a division of NOAA/ESRL, and ma...
The global burden of sulfur hexafluoride (SF6), a very long-lived greenhouse gas, has been increasing steadily over the last few decades. Current atmospheric measurements of SF6 are sufficient to infer global-scale emissions, and recent studies (Levin, et al., 2010; Rigby et al., 2010) have shown that global inventories agree well with top-down emi...
Global Hawk Pacific (GloPac) 2010 was the first scientific mission of the Global Hawk unmanned aerial system (UAS), and included a payload designed for in situ measurement of trace gases and aerosols, remote sensing of gases and particles, and measurement of various meteorological parameters. The Global Hawk is capable of long-duration flight (rang...
We present atmospheric sulfur hexafluoride (SF<sub>6</sub>) mole fractions and emissions estimates from the 1970s to 2008. Measurements were made of archived air samples starting from 1973 in the Northern Hemisphere and from 1978 in the Southern Hemisphere, using the Advanced Global Atmospheric Gases Experiment (AGAGE) gas chromatographic–mass spec...
Seasonal cycles in the mixing ratios of tropospheric nitrous oxide (N2O) are derived by detrending long-term measurements made at sites across four global surface monitoring networks. These cycles are examined for physical and biogeochemical signals. The detrended monthly data display large interannual variability, which at some sites challenges th...
Methyl chloride (CH3Cl) is a chlorine-containing trace gas in the atmosphere contributing significantly to stratospheric ozone depletion. Large uncertainties in estimates of its source and sink magnitudes and temporal and spatial variations currently exist. GEIA inventories and other bottom-up emission estimates are used to construct a priori maps...
Carbon tetrachloride (CCl4) has substantial stratospheric ozone depletion potential and its consumption is controlled under the Montreal Protocol and its amendments. We implement a Kalman filter using atmospheric CC14 measurements and a 3-dimensional chemical transport model to estimate the interannual regional industrial emissions and seasonal glo...
Carbon tetrachloride (CCl<sub>4</sub>) has substantial stratospheric ozone depletion potential and its consumption is controlled under the Montreal Protocol and its amendments. We implement a Kalman filter using atmospheric CC1<sub>4</sub> measurements and a 3-dimensional chemical transport model to estimate the interannual regional industrial emis...
We present atmospheric sulfur hexafluoride (SF6) mole fractions and emissions estimates from the 1970s to 2008. Measurements were made of archived air samples starting from 1973 in the Northern Hemisphere and from 1978 in the Southern Hemisphere, using the Advanced Global Atmospheric Gases Experiment (AGAGE) gas chromatographic–mass spectrometric (...
The UTLS is a complex mixture of air transported from a variety of
different regions and over a wide range of time scales. This can make
the interpretation of tracer distributions in the UTLS quite difficult.
We present a method to use measurements of molecules with photolytic
processing in the stratosphere to quantitatively estimate the
stratosphe...
Methyl chloride (CH3Cl) is a chlorine-containing trace gas in the atmosphere contributing significantly to stratospheric ozone depletion. Large uncertainties in estimates of its source and sink magnitudes and temporal and spatial variations currently exist. GEIA inventories and other bottom-up emission estimates are used to construct a priori maps...
Previous airborne studies have proven the scientific value of chemical tracers in examining transport of the Upper Troposphere and Lower Stratosphere (UT/LS). ESRL scientists operated two airborne gas chromatographs on the NCAR G-V during the NSF sponsored Stratosphere-Troposphere Analyses of Regional Transport START-08 campaign over the midlatitud...
Nitrous oxide (N2O) is an important atmospheric trace gas that is responsible for climate forcing as the third strongest greenhouse gas and depletion of stratospheric ozone. A recent study (Ravishankara et al., 2009, Science, 10.1126/science.1176985) has calculated the Ozone Depletion Potential (ODP) for N2O as 0.017. Using the new ODP coupled with...
We use an atmospheric general circulation model (AGCM) driven chemistry-transport model (ACTM) to simulate the evolution of sulfur hexafluoride (SF<sub>6</sub>) in the troposphere. The model results are compared with continuous measurements at 6 sites over 71° N–90° S. These comparisons demonstrate that the ACTM simulations lie within the measureme...
We use an atmospheric general circulation model (AGCM) driven chemistry-transport model (ACTM) to simulate the evolution of sulfur hexafluoride (SF6) in the troposphere. The model results are compared with continuous measurements at 6 sites over 71° N-90° S. These comparisons demonstrate that the ACTM simulations lie within the measurement uncertai...
The chemical composition of the stratosphere is changing as a result of international limits on the industrial use of ozone-depleting substances (ODSs). Natural processes also influence the abundance of halogen- and sulfur-containing gases and affect stratospheric composition through changes in emissions or loss rates. Through a global network of f...
The Arctic Region is most sensitive to future climate change. Quantifying emissions and sinks of many important biogenic trace gases there may become important indicators of potential climate feedback. Once snowmelt at Pt. Barrow, Alaska (77o N) occurs, ground cover is exposed by sunlight and higher temperatures, then photosynthesis starts up. Peak...