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Zuiderweg A.,University Utrecht | Holzinger R.,University Utrecht | Martinerie P.,CNRS Laboratory for Glaciology and Environmental Geophysics | Schneider R.,University of Bern | And 7 more authors.
Atmospheric Chemistry and Physics | Year: 2013

A series of 12 high volume air samples collected from the S2 firn core during the North Greenland Eemian Ice Drilling (NEEM) 2009 campaign have been measured for mixing ratio and stable carbon isotope composition of the chlorofluorocarbon CFC-12 (CCl2F2). While the mixing ratio measurements compare favorably to other firn air studies, the isotope results show extreme 13C depletion at the deepest measurable depth (65 m), to values lower than δ13C Combining double low line-80‰ vs. VPDB (the international stable carbon isotope scale), compared to present day surface tropospheric measurements near-40‰. Firn air modeling was used to interpret these measurements. Reconstructed atmospheric time series indicate even larger depletions (to-120‰) near 1950 AD, with subsequent rapid enrichment of the atmospheric reservoir of the compound to the present day value. Mass-balance calculations show that this change is likely to have been caused by a large change in the isotopic composition of anthropogenic CFC-12 emissions, probably due to technological advances in the CFC production process over the last 80 yr, though direct evidence is lacking. © 2013 Author(s).

Crippa M.,Paul Scherrer Institute | Decarlo P.F.,Paul Scherrer Institute | Decarlo P.F.,Drexel University | Slowik J.G.,Paul Scherrer Institute | And 27 more authors.
Atmospheric Chemistry and Physics | Year: 2013

The effect of a post-industrial megacity on local and regional air quality was assessed via a month-long field measurement campaign in the Paris metropolitan area during winter 2010. Here we present source apportionment results from three aerosol mass spectrometers and two aethalometers deployed at three measurement stations within the Paris region. Submicron aerosol composition is dominated by the organic fraction (30-36%) and nitrate (28-29%), with lower contributions from sulfate (14-16%), ammonium (12-14%) and black carbon (7-13%). Organic source apportionment was performed using positive matrix factorization, resulting in a set of organic factors corresponding both to primary emission sources and secondary production. The dominant primary sources are traffic (11-15% of organic mass), biomass burning (13-15%) and cooking (up to 35% during meal hours). Secondary organic aerosol contributes more than 50% to the total organic mass and includes a highly oxidized factor from indeterminate and/or diverse sources and a less oxidized factor related to wood burning emissions. Black carbon was apportioned to traffic and wood burning sources using a model based on wavelength-dependent light absorption of these two combustion sources. The time series of organic and black carbon factors from related sources were strongly correlated. The similarities in aerosol composition, total mass and temporal variation between the three sites suggest that particulate pollution in Paris is dominated by regional factors, and that the emissions from Paris itself have a relatively low impact on its surroundings. © 2013 Author(s).

Petrenko V.V.,University of Colorado at Boulder | Petrenko V.V.,University of Rochester | Martinerie P.,UJF Andndash | Novelli P.,National Oceanic and Atmospheric Administration | And 22 more authors.
Atmospheric Chemistry and Physics | Year: 2013

We present the first reconstruction of the Northern Hemisphere (NH) high latitude atmospheric carbon monoxide (CO) mole fraction from Greenland firn air. Firn air samples were collected at three deep ice core sites in Greenland (NGRIP in 2001, Summit in 2006 and NEEM in 2008). CO records from the three sites agree well with each other as well as with recent atmospheric measurements, indicating that CO is well preserved in the firn at these sites. CO atmospheric history was reconstructed back to the year 1950 from the measurements using a combination of two forward models of gas transport in firn and an inverse model. The reconstructed history suggests that Arctic CO in 1950 was 140-150 nmol mol-1, which is higher than today's values. CO mole fractions rose by 10-15 nmol mol-1 from 1950 to the 1970s and peaked in the 1970s or early 1980s, followed by a ≈ 30 nmol mol-1 decline to today's levels. We compare the CO history with the atmospheric histories of methane, light hydrocarbons, molecular hydrogen, CO stable isotopes and hydroxyl radicals (OH), as well as with published CO emission inventories and results of a historical run from a chemistry-transport model. We find that the reconstructed Greenland CO history cannot be reconciled with available emission inventories unless unrealistically large changes in OH are assumed. We argue that the available CO emission inventories strongly underestimate historical NH emissions, and fail to capture the emission decline starting in the late 1970s, which was most likely due to reduced emissions from road transportation in North America and Europe. © Author(s) 2013.

Bonan B.,French Institute for Research in Computer Science and Automation | Nodet M.,French Institute for Research in Computer Science and Automation | Nodet M.,Joseph Fourier University | Ritz C.,UJF Andndash | Peyaud V.,UJF Andndash
Nonlinear Processes in Geophysics | Year: 2014

Estimating the contribution of Antarctica and Greenland to sea-level rise is a hot topic in glaciology. Good estimates rely on our ability to run a precisely calibrated ice sheet evolution model starting from a reliable initial state. Data assimilation aims to provide an answer to this problem by combining the model equations with observations. In this paper we aim to study a state-of-the-art ensemble Kalman filter (ETKF) to address this problem. This method is implemented and validated in the twin experiments framework for a shallow ice flowline model of ice dynamics. The results are very encouraging, as they show a good convergence of the ETKF (with localisation and inflation), even for small-sized ensembles. © Author(s) 2014. CC Attribution 3.0 License.

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