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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), Institute of Meteorology and Climate Research (IMK) and Consejo Superior de Investigaciones Científicas (CSIC), Instituto de Astrofísica de Andalucía (IAA). These profiles have been compared to measurements taken by the balloon-borne cryosampler, Mark IV (MkIV) and MIPAS-Balloon (MIPAS-B), the airborne MIPAS-STRatospheric aircraft (MIPAS-STR), the satellite-borne Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) and the High Resolution Dynamic Limb Sounder (HIRDLS), as well as the ground-based Halocarbon and other Atmospheric Trace Species (HATS) network for the reduced spectral resolution period (RR: January 2005–April 2012) of MIPAS. ACE-FTS, MkIV and HATS also provide measurements during the high spectral resolution period (full resolution, FR: July 2002–March 2004) and were used to validate MIPAS CFC-11 and CFC-12 products during that time, as well as profiles from the Improved Limb Atmospheric Spectrometer, ILAS-II. In general, we find that MIPAS shows slightly higher values for CFC-11 at the lower end of the profiles (below ∼ 15 km) and in a comparison of HATS ground-based data and MIPAS measurements at 3 km below the tropopause. Differences range from approximately 10 to 50 pptv ( ∼ 5–20 %) during the RR period. In general, differences are slightly smaller for the FR period. An indication of a slight high bias at the lower end of the profile exists for CFC-12 as well, but this bias is far less pronounced than for CFC-11 and is not as obvious in the relative differences between MIPAS and any of the comparison instruments. Differences at the lower end of the profile (below ∼ 15 km) and in the comparison of HATS and MIPAS measurements taken at 3 km below the tropopause mainly stay within 10–50 pptv (corresponding to ∼ 2–10 % for CFC-12) for the RR and the FR period. Between ∼ 15 and 30 km, most comparisons agree within 10–20 pptv (10–20 %), apart from ILAS-II, which shows large differences above ∼ 17 km. Overall, relative differences are usually smaller for CFC-12 than for CFC-11. For both species – CFC-11 and CFC-12 – we find that differences at the lower end of the profile tend to be larger at higher latitudes than in tropical and subtropical regions. In addition, MIPAS profiles have a maximum in their mixing ratio around the tropopause, which is most obvious in tropical mean profiles. Comparisons of the standard deviation in a quiescent atmosphere (polar summer) show that only the CFC-12 FR error budget can fully explain the observed variability, while for the other products (CFC-11 FR and RR and CFC-12 RR) only two-thirds to three-quarters can be explained. Investigations regarding the temporal stability show very small negative drifts in MIPAS CFC-11 measurements. These instrument drifts vary between ∼ 1 and 3 % decade−1. For CFC-12, the drifts are also negative and close to zero up to ∼ 30 km. Above that altitude, larger drifts of up to ∼ 50 % decade−1 appear which are negative up to ∼ 35 km and positive, but of a similar magnitude, above.
The organic rich Livello Bonarelli formed as a result of oxygen deficiency and carbonate dissolution in the oceans during the Cenomanian/Turonian (C/T) transition. During this Ocean Anoxic Event 2 (OAE2), a combination of factors caused increased productivity, incomplete decomposition of organic matter and widespread deposition of black shales. Although these sediments are extensively studied, the exact extent, cause, timing and duration of oceanic anoxia are debated (Sinton and Duncan, 1997; Mitchell et al., 2008). Contrasting causal mechanisms have been suggested, including stratification of the water column (Lanci et al., 2010) versus intensification of the hydrological cycle driving a dynamic ocean circulation (Trabucho-Alexandre et al., 2010). Studies on trace-elemental and (radiogenic) isotope compositions of Cenomanian marine successions have suggested a volcanic origin of OAE2, by delivering nutrients to the semi-enclosed proto-North Atlantic (Zheng et al., 2013, and references therein; Du Vivier et al., 2014). Deciphering the importance of volcanic and oceanographic processes requires tight constraints on their relative timing. Regularly occurring black cherts and shales below the Livello Bonarelli demonstrate that oceanic conditions in the Umbria-Marche Basin were punctuated by episodes of regional anoxia from the mid-Cenomanian onwards. Their hierarchical stacking pattern suggests an orbital control on the deposition of organic rich horizons (Mitchell et al., 2008; Lanci et al., 2010). Stable carbon isotope data reveal that long-term 15 variations in eccentricity paced the carbon cycle (Sprovieri et al., 2013) and sea level changes (Voigt et al., 2006) of the Late Cretaceous. Here we investigate the role of orbital forcing on climate and the carbon cycle, and, specifically, on organic-rich sedimentation prior, during, and after OAE2.
We also explore the potential for establishing an anchored astrochronology for the C/T interval in Europe. Recent improvements in the astronomical solution (La2011; Laskar et al., 2011b) and in the intercalibration of radiometric and astronomical dating techniques (Kuiper et al., 2008; Renne et al., 2013) allow the extension of the astronomical time scale into the Cretaceous. The C/T boundary in the Western Interior (USA) has been dated at 93.90 ± 0.15 Ma by intercalibration of radio-isotopic and astrochronologic time scales (Meyers et al., 2012b). Also, reinterpretation of proxy records spanning the C/T interval seems to resolve discrepancies in reported durations of the OAE2 (Sageman et al., 2006; Meyers et al., 2012a). The well-documented Italian rhythmic successions, reference sections for climatic processes in the Tethyan realm, need to be tied in with the absolute time scale. Biostratigraphic correlation to radioisotopically-dated ash beds in the Western Interior is complicated by the provinciality of faunas and floras. However, δ13C stratigraphy provides a reliable correlation tool (Gale et al., 2005) and we present a new 40Ar/39Ar age for the Thatcher bentonite from the Western Interior occurring within the mid-Cenomanian δ13C event (MCE). This study integrates the well-developed cyclostratigraphy from the Umbria-Marche Basin with radioisotopic ages from the Western Interior and derives a numerical timescale for this critical interval in Earth’s history.
The oceans at the time of the Cenomanian–Turonian transition were abruptly perturbed by a period of bottom-water anoxia. This led to the brief but widespread deposition of black organic-rich shales, such as the Livello Bonarelli in the Umbria–Marche Basin (Italy). Despite intensive studies, the origin and exact timing of this event are still debated. In this study, we assess leading hypotheses about the inception of oceanic anoxia in the Late Cretaceous greenhouse world by providing a 6 Myr long astronomically tuned timescale across the Cenomanian–Turonian boundary. We procure insights into the relationship between orbital forcing and the Late Cretaceous carbon cycle by deciphering the imprint of astronomical cycles on lithologic, physical properties, and stable isotope records, obtained from the Bottaccione, Contessa and Furlo sections in the Umbria–Marche Basin. The deposition of black shales and cherts, as well as the onset of oceanic anoxia, is related to maxima in the 405 kyr cycle of eccentricity-modulated precession. Correlation to radioisotopic ages from the Western Interior (USA) provides unprecedented age control for the studied Italian successions. The most likely tuned age for the base of the Livello Bonarelli is 94.17 ± 0.15 Ma (tuning 1); however, a 405 kyr older age cannot be excluded (tuning 2) due to uncertainties in stratigraphic correlation, radioisotopic dating, and orbital configuration. Our cyclostratigraphic framework suggests that the exact timing of major carbon cycle perturbations during the Cretaceous may be linked to increased variability in seasonality (i.e. a 405 kyr eccentricity maximum) after the prolonged avoidance of seasonal extremes (i.e. a 2.4 Myr eccentricity minimum). Volcanism is probably the ultimate driver of oceanic anoxia, but orbital periodicities determine the exact timing of carbon cycle perturbations in the Late Cretaceous. This unites two leading hypotheses about the inception of oceanic anoxia in the Late Cretaceous greenhouse world.
We present the first 3-D model of seismic P and S velocities in the crust and uppermost mantle beneath the Gulf of Aqaba and surrounding areas based on the results of passive travel time tomography. The tomographic inversion was performed based on travel time data from ∼ 9000 regional earthquakes provided by the Egyptian National Seismological Network (ENSN), and this was complemented with data from the International Seismological Centre (ISC). The resulting P and S velocity patterns were generally consistent with each other at all depths. Beneath the northern part of the Red Sea, we observed a strong high-velocity anomaly with abrupt limits that coincide with the coastal lines. This finding may indicate the oceanic nature of the crust in the Red Sea, and it does not support the concept of gradual stretching of the continental crust. According to our results, in the middle and lower crust, the seismic anomalies beneath the Gulf of Aqaba seem to delineate a sinistral shift (∼ 100 km) in the opposite flanks of the fault zone, which is consistent with other estimates of the left-lateral displacement in the southern part of the Dead Sea Transform fault. However, no displacement structures were visible in the uppermost lithospheric mantle.
Biomass burning impacts vegetation dynamics, biogeochemical cycling, atmospheric chemistry, and climate, with sometimes deleterious socio-economic impacts. Under future climate projections it is often expected that the risk of wildfires will increase. Our ability to predict the magnitude and geographic pattern of future fire impacts rests on our ability to model fire regimes, using either well-founded empirical relationships or process-based models with good predictive skill. While a large variety of models exist today, it is still unclear which type of model or degree of complexity is required to model fire adequately at regional to global scales. This is the central question underpinning the creation of the Fire Model Intercomparison Project (FireMIP), an international initiative to compare and evaluate existing global fire models against benchmark data sets for present-day and historical conditions. In this paper we review how fires have been represented in fire-enabled dynamic global vegetation models (DGVMs) and give an overview of the current state of the art in fire-regime modelling. We indicate which challenges still remain in global fire modelling and stress the need for a comprehensive model evaluation and outline what lessons may be learned from FireMIP.
Reconstructions of biomass burning from sediment-charcoal records to improve data–model comparisons
(2016)
The location, timing, spatial extent, and frequency of wildfires are changing rapidly in many parts of the world, producing substantial impacts on ecosystems, people, and potentially climate. Paleofire records based on charcoal accumulation in sediments enable modern changes in biomass burning to be considered in their long-term context. Paleofire records also provide insights into the causes and impacts of past wildfires and emissions when analyzed in conjunction with other paleoenvironmental data and with fire models. Here we present new 1000-year and 22 000-year trends and gridded biomass burning reconstructions based on the Global Charcoal Database version 3 (GCDv3), which includes 736 charcoal records (57 more than in version 2). The new gridded reconstructions reveal the spatial patterns underlying the temporal trends in the data, allowing insights into likely controls on biomass burning at regional to global scales. In the most recent few decades, biomass burning has sharply increased in both hemispheres but especially in the north, where charcoal fluxes are now higher than at any other time during the past 22 000 years. We also discuss methodological issues relevant to data–model comparisons and identify areas for future research. Spatially gridded versions of the global data set from GCDv3 are provided to facilitate comparison with and validation of global fire simulations.
MIPAS-Envisat is a satellite-borne sensor which measured vertical profiles of a wide range of trace gases from 2002 to 2012 using IR emission spectroscopy. We present geophysical validation of the MIPAS-Envisat operational retrieval (version 6.0) of N2O, CH4, CFC-12, and CFC-11 by the European Space Agency (ESA). The geophysical validation data are derived from measurements of samples collected by a cryogenic whole air sampler flown to altitudes of up to 34 km by means of large scientific balloons. In order to increase the number of coincidences between the satellite and the balloon observations, we applied a trajectory matching technique. The results are presented for different time periods due to a change in the spectroscopic resolution of MIPAS in early 2005. Retrieval results for N2O, CH4, and CFC-12 show partly good agreement for some altitude regions, which differs for the periods with different spectroscopic resolution. The more recent low spectroscopic resolution data above 20 km altitude show agreement with the combined uncertainties, while there is a tendency of the earlier high spectral resolution data set to underestimate these species above 25 km. The earlier high spectral resolution data show a significant overestimation of the mixing ratios for N2O, CH4, and CFC-12 below 20 km. These differences need to be considered when using these data. The CFC-11 results from the operation retrieval version 6.0 cannot be recommended for scientific studies due to a systematic overestimation of the CFC-11 mixing ratios at all altitudes.
Influence of sea surface roughness length parameterization on Mistral and Tramontane simulations
(2016)
The Mistral and Tramontane are mesoscale winds in southern France and above the Western Mediterranean Sea. They are phenomena well suited for studying channeling effects as well as atmosphere–land/ocean processes. This sensitivity study deals with the influence of the sea surface roughness length parameterizations on simulated Mistral and Tramontane wind speed and wind direction. Several simulations with the regional climate model COSMO-CLM were performed for the year 2005 with varying values for the Charnock parameter α. Above the western Mediterranean area, the simulated wind speed and wind direction pattern on Mistral days changes depending on the parameterization used. Higher values of α lead to lower simulated wind speeds. In areas, where the simulated wind speed does not change much, a counterclockwise rotation of the simulated wind direction is observed.
We present the characterization and application of a new gas chromatography time-of-flight mass spectrometry instrument (GC-TOFMS) for the quantitative analysis of halocarbons in air samples. The setup comprises three fundamental enhancements compared to our earlier work (Hoker et al., 2015): (1) full automation, (2) a mass resolving power R = m/Δm of the TOFMS (Tofwerk AG, Switzerland) increased up to 4000 and (3) a fully accessible data format of the mass spectrometric data. Automation in combination with the accessible data allowed an in-depth characterization of the instrument. Mass accuracy was found to be approximately 5 ppm in mean after automatic recalibration of the mass axis in each measurement. A TOFMS configuration giving R = 3500 was chosen to provide an R-to-sensitivity ratio suitable for our purpose. Calculated detection limits are as low as a few femtograms by means of the accurate mass information. The precision for substance quantification was 0.15 % at the best for an individual measurement and in general mainly determined by the signal-to-noise ratio of the chromatographic peak. Detector non-linearity was found to be insignificant up to a mixing ratio of roughly 150 ppt at 0.5 L sampled volume. At higher concentrations, non-linearities of a few percent were observed (precision level: 0.2 %) but could be attributed to a potential source within the detection system. A straightforward correction for those non-linearities was applied in data processing, again by exploiting the accurate mass information. Based on the overall characterization results, the GC-TOFMS instrument was found to be very well suited for the task of quantitative halocarbon trace gas observation and a big step forward compared to scanning, quadrupole MS with low mass resolving power and a TOFMS technique reported to be non-linear and restricted by a small dynamical range.
Amines are potentially important for atmospheric new particle formation, but their concentrations are usually low with typical mixing ratios in the pptv range or even smaller. Therefore, the demand for highly sensitive gas-phase amine measurements has emerged in the last several years. Nitrate chemical ionization mass spectrometry (CIMS) is routinely used for the measurement of gasphase sulfuric acid in the sub-pptv range. Furthermore, extremely low volatile organic compounds (ELVOCs) can be detected with a nitrate CIMS. In this study we demonstrate that a nitrate CIMS can also be used for the sensitive measurement of dimethylamine (DMA, (CH3/2NH) using the NO3−•(HNO3)1 − 2• (DMA) cluster ion signal. Calibration measurements were made at the CLOUD chamber during two different measurement campaigns. Good linearity between 0 and ~120 pptv of DMA as well as a sub-pptv detection limit of 0.7 pptv for a 10 min integration time are demonstrated at 278K and 38% RH.