Decrease of carbon tetrachloride (CCl4) over 2004-2013 as inferred from global occultation measurements with ACE-FTS

In this contribution, we use infrared solar occultation measurements performed by the ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) instrument onboard the SCISAT-1 Canadian satellite (Bernath et al., 2005). Since its launch in August 2003, this spectrometer has been in continuous operation with no significant degradation of its performance, and global measurements are available from late February 2004 onwards, spanning now more than a decade

Revisiting global fossil fuel and biofuel emissions of ethane

Recent measurements over the Northern Hemisphere indicate that the long-term decline in the atmospheric burden of ethane (C2H6) has ended and the abundance increased dramatically between 2010 and 2014. The rise in C2H6 atmospheric abundances has been attributed to oil and natural gas extraction in North America. Existing global C2H6 emission inventories are based on outdated activity maps that do not account for current oil and natural gas exploitation regions. We present an updated global C2H6 emission inventory based on 2010 satellite-derived CH4 fluxes with adjusted C2H6 emissions over the U.S. from the National Emission Inventory (NEI 2011). We contrast our global 2010 C2H6 emission inventory with one developed for 2001. The C2H6 difference between global anthropogenic emissions is subtle (7.9 versus 7.2 Tg yr−1), but the spatial distribution of the emissions is distinct. In the 2010 C2H6 inventory, fossil fuel sources in the Northern Hemisphere represent half of global C2H6 emissions and 95% of global fossil fuel emissions. Over the U.S., unadjusted NEI 2011 C2H6 emissions produce mixing ratios that are 14–50% of those observed by aircraft observations (2008–2014). When the NEI 2011 C2H6 emission totals are scaled by a factor of 1.4, the Goddard Earth Observing System Chem model largely reproduces a regional suite of observations, with the exception of the central U.S., where it continues to underpredict observed mixing ratios in the lower troposphere. We estimate monthly mean contributions of fossil fuel C2H6 emissions to ozone and peroxyacetyl nitrate surface mixing ratios over North America of ~1% and ~8%, respectively

VUV and X-ray coherent light with tunable polarization from single-pass free-electron lasers

Tunable polarization over a wide spectral range is a required feature of light sources employed to investigate the properties of local symmetry in both condensed and low-density matter. Among new-generation sources, free-electron lasers possess a unique combination of very attractive features, as they allow to generate powerful and coherent ultra-short optical pulses in the VUV and X-ray spectral range. However, the question remains open about the possibility to freely vary the light polarization of a free-electron laser, when the latter is operated in the so-called nonlinear harmonic-generation regime. In such configuration, one collects the harmonics of the free-electron laser fundamental emission, gaining access to the shortest possible wavelengths the device can generate. In this letter we provide the first experimental characterization of the polarization of the harmonic light produced by a free-electron laser and we demonstrate a method to obtain tunable polarization in the VUV and X-ray spectral range. Experimental results are successfully compared to those obtained using a theoretical model based on the paraxial solution of Maxwell's equations. Our findings can be expected to have a deep impact on the design and realization of experiments requiring full control of light polarization to explore the symmetry properties of matter samples

Measurements of hydrogen cyanide (HCN) and acetylene (C2H2) from the Infrared Atmospheric Sounding Interferometer (IASI)

Hydrogen cyanide (HCN) and acetylene (C2H2) are ubiquitous atmospheric trace gases with medium lifetime, which are frequently used as indicators of combustion sources and as tracers for atmospheric transport and chemistry. Because of their weak infrared absorption, overlapped by the CO2 Q branch near 720 cm−1, nadir sounders have up to now failed to measure these gases routinely. Taking into account CO2 line mixing, we provide for the first time extensive measurements of HCN and C2H2 total columns at Reunion Island (21° S, 55° E) and Jungfraujoch (46° N, 8° E) in 2009–2010 using observations from the Infrared Atmospheric Sounding Interferometer (IASI). A first order comparison with local ground-based Fourier transform InfraRed (FTIR) measurements has been carried out allowing tests of seasonal consistency which is reasonably captured, except for HCN at Jungfraujoch. The IASI data shows a greater tendency to high C2H2 values. We also examine a nonspecific biomass burning plume over austral Africa and show that the emission ratios with respect to CO agree with previously reported values

Two-colour generation in a chirped seeded Free-Electron Laser

We present the experimental demonstration of a method for generating two spectrally and temporally separated pulses by an externally seeded, single-pass free-electron laser operating in the extreme-ultraviolet spectral range. Our results, collected on the FERMI@Elettra facility and confirmed by numerical simulations, demonstrate the possibility of controlling both the spectral and temporal features of the generated pulses. A free-electron laser operated in this mode becomes a suitable light source for jitter-free, two-colour pump-probe experiments

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