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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.
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.
In this meeting report, particularly addressing the topic of protection of the cardiovascular system from ischemia/reperfusion injury, highlights are presented that relate to conditioning strategies of the heart with respect to molecular mechanisms and outcome in patients’ cohorts, the influence of co-morbidities and medications, as well as the contribution of innate immune reactions in cardioprotection. Moreover, developmental or systems biology approaches bear great potential in systematically uncovering unexpected components involved in ischemia–reperfusion injury or heart regeneration. Based on the characterization of particular platelet integrins, mitochondrial redox-linked proteins, or lipid-diol compounds in cardiovascular diseases, their targeting by newly developed theranostics and technologies opens new avenues for diagnosis and therapy of myocardial infarction to improve the patients’ outcome.
In this study, we aim to reconstruct a relevant and new database of monthly zonal mean distribution of carbon dioxide (CO2) at global scale extending from the upper-troposphere (UT) to stratosphere (S). This product can be used for model and satellite validation in the UT/S, as a prior for inversion modelling and mainly to analyse a plausible feature of the stratospherictropospheric exchange as well as the stratospheric circulation and its variability. To do so, we investigate the ability of a Lagrangian trajectory model guided by ERA-Interim reanalysis to construct the CO2 abundance in the UT/S. From 10 year backward trajectories and tropospheric observations of CO2, we reconstruct upper-tropospheric and stratospheric CO2 over the period 2000–2010. The inter-comparisons of the reconstructed CO2 with mid-latitude vertical profiles measured by balloon samples as well as quasi-horizontal air samples from ER-2 aircraft during SOLVE and CONTRAIL campaigns exhibit a remarkable agreement. That demonstrates the potential of Lagrangian model to reconstruct CO2 in the UT/S. The zonal mean distribution exhibits relatively large CO2 in the tropical stratosphere due to the seasonal variation of the tropical upwelling of Brewer-Dobson circulation. During winter and spring, the tropical pipe is relatively isolated but is less confined during summer and autumn so that high CO2 values are more readily transported out of the tropics to the mid- and high latitude stratosphere. The shape of the vertical profiles suggests that relatively high CO2 above 20 km altitude mainly enter the stratosphere through tropical upwelling. CO2 mixing ratio is relatively low in the polar and tropical regions above 25 km. On average the CO2 mixing ratio decreases with altitude by 6-8 ppmv from the UT to stratosphere (e.g. up to 35 km) and is nearly constant with altitude.
AirCore-HR: a high resolution column sampling to enhance the vertical description of CH₄ and CO₂
(2016)
An original and innovative sampling system called AirCore was presented by NOAA in 2010 (Karion et al., 2010). It consists of a long (> 100 m) and narrow (< 1 cm) stainless steel tube that can retain a profile of atmospheric air. The captured air sample has then to be analyzed with a gas analyzer for trace mole fraction. In this study, we introduce a new AirCore aiming at improved resolution along the vertical with the objectives to: (i) better capture the vertical distribution of CO2 and CH4, (ii) provide a tool to compare AirCores and validate the estimated vertical resolution achieved by AirCores. This AirCore-HR (high resolution) consists of a 300 m tube, combining 200 m of 1/8 in. (3.175 mm) tube and a 100 m of 1/4 in. (6.35 mm) tube. This new configuration allows to achieve a vertical resolution of 300 m up to 15 km and better than 500 m up to 22 km (if analysis of the retained sample is performed within 3 hours). The AirCore-HR was flown for the first time during the annual StratoScience campaign from CNES in August 2014 from Timmins (Ontario, Canada). High-resolution vertical profiles of CO2 and CH4 up to 25 km were successfully retrieved. These profiles revealed well defined transport structures in the troposphere (also seen in CAMS-ECMWF high resolution forecasts of CO2 and CH4 profiles) and captured the decrease of CO2 and CH4 in the stratosphere. The multi-instruments gondola from the flight carried two other low-resolution AirCore-GUF that allowed to perform direct comparisons and study the underlying processing method used to convert the sample of air to greenhouse gases vertical profiles. In particular, degrading the AirCore-HR derived profiles to the low resolution of AirCore-GUF yields an excellent match between both sets of CH4 profiles, and shows a good consistency between vertical structures of CO2 and CH4. These results fully validate the theoretical vertical resolution achievable by AirCores. Finally, the uncertainties associated with the measurements are assessed, yielding an average uncertainty below 3 ppb for CH4 and 0.25 ppm for CO2 with the major source of uncertainty coming from the potential loss of air sample on the ground and the choice of the starting and ending point of the collected air sample inside the tube. In an ideal case where the sample would be fully retained, it would be possible to know precisely the pressure at which air was sampled last and thus to improve the overall uncertainty to about 0.1 ppm for CO2 and 2 ppb for CH4.