New insights in the global cycle of acetonitrile: release from the ocean and acetonitrile: release from the ocean and Venezuela

International audienceCUsing the proton transfer reaction mass spectrometry (PTR-MS) technique, acetonitrile was measured during the wet season in a Venezuelan woodland savanna. The site was located downwind of the Caribbean Sea and no biomass burning events were observed in the region. High boundary layer concentrations of 211 ±36 pmol/mol (median, ± standard deviation) were observed during daytime in the well mixed boundary layer, which is about 60 pmol/mol above background concentrations recently measured over the Mediterranean Sea and the Pacific Ocean. Most likely acetonitrile is released from the warm waters of the Caribbean Sea thereby enhancing mixing ratios over Venezuela. Acetonitrile concentrations will probably still be much higher in biomass burning plumes, however, the general suitability of acetonitrile as a biomass burning marker should be treated with care. During nights, acetonitrile dropped to levels typically around 120 pmol/mol, which is consistent with a dry deposition velocity of ~0.14 cm/s when a nocturnal boundary layer height of 100 m is assumed

Stratospheric dryness: model simulations and satellite observations

The mechanisms responsible for the extreme dryness of the stratosphere have been debated for decades. A key difficulty has been the lack of comprehensive models which are able to reproduce the observations. Here we examine results from the coupled lower-middle atmosphere chemistry general circulation model ECHAM5/MESSy1 together with satellite observations. Our model results match observed temperatures in the tropical lower stratosphere and realistically represent the seasonal and inter-annual variability of water vapor. The model reproduces the very low water vapor mixing ratios (below 2 ppmv) periodically observed at the tropical tropopause near 100 hPa, as well as the characteristic tape recorder signal up to about 10 hPa, providing evidence that the dehydration mechanism is well-captured. Our results confirm that the entry of tropospheric air into the tropical stratosphere is forced by large-scale wave dynamics, whereas radiative cooling regionally decelerates upwelling and can even cause downwelling. Thin cirrus forms in the cold air above cumulonimbus clouds, and the associated sedimentation of ice particles between 100 and 200 hPa reduces water mass fluxes by nearly two orders of magnitude compared to air mass fluxes. Transport into the stratosphere is supported by regional net radiative heating, to a large extent in the outer tropics. During summer very deep monsoon convection over Southeast Asia, centered over Tibet, moistens the stratosphere

Temperature dependence of UV absorption cross sections and atmospheric implications of several alkyl iodides

The ultraviolet absorption spectra of a number of alkyl iodides which have been found in the troposphere, CH_3I, C_2H_5I, CH_3CH_2CH_2I, CH_3CHICH_3, CH_2I_2, and CH2_ClI, have been measured over the wavelength range 200–380 nm and at temperatures between 298 and 210 K. The absorption spectra of the monoiodides C_H3I, C_2H_5I, CH_3CH_2CH_2I, and CH_3CHICH_3 are nearly identical in shape and magnitude and consist of single broad bands centered near 260 nm. The addition of a chlorine atom in CH_2ClI shifts its spectrum to longer wavelengths (σ_(max) at 270 nm). The spectrum of CH_2I_2 is further red‐shifted, reaching a maximum of 3.85×10^(−18) cm^2 molecule^(−1) at 288 nm and exhibiting strong absorption in the solar actinic region, λ>290 nm. Atmospheric photolysis rate constants, J values, have been calculated assuming quantum efficiencies of unity for different solar zenith angles as a function of altitude using the newly measured cross sections. Surface photolysis rate constants, calculated from the absorption cross sections measured at 298 K, range from 3×10^(−6) s^(−1) for CH)3I to 5×10^(−3) s^(−1) for CH)2I)2 at a solar zenith angle of 40°

Comprehensive Laboratory Measurements of Biomass-Burning Emissions: 1. Emissions from Indonesian, African, and Other Fuels

[1] Trace gas and particle emissions were measured from 47 laboratory fires burning 16 regionally to globally significant fuel types. Instrumentation included the following: open-path Fourier transform infrared spectroscopy; proton transfer reaction mass spectrometry; filter sampling with subsequent analysis of particles with diameter \u3c2.5 μm for organic and elemental carbon and other elements; and canister sampling with subsequent analysis by gas chromatography (GC)/flame ionization detector, GC/electron capture detector, and GC/mass spectrometry. The emissions of 26 compounds are reported by fuel type. The results include the first detailed measurements of the emissions from Indonesian fuels. Carbon dioxide, CO, CH4, NH3, HCN, methanol, and acetic acid were the seven most abundant emissions (in order) from burning Indonesian peat. Acetol (hydroxyacetone) was a major, previously unobserved emission from burning rice straw (21–34 g/kg). The emission factors for our simulated African fires are consistent with field data for African fires for compounds measured in both the laboratory and the field. However, the higher concentrations and more extensive instrumentation in this work allowed quantification of at least 10 species not previously quantified for African field fires (in order of abundance): acetaldehyde, phenol, acetol, glycolaldehyde, methylvinylether, furan, acetone, acetonitrile, propenenitrile, and propanenitrile. Most of these new compounds are oxygenated organic compounds, which further reinforces the importance of these reactive compounds as initial emissions from global biomass burning. A few high-combustion-efficiency fires emitted very high levels of elemental (black) carbon, suggesting that biomass burning may produce more elemental carbon than previously estimated

Modeling atmospheric effects of the September 1859 Solar Flare

We have modeled atmospheric effects, especially ozone depletion, due to a solar proton event which probably accompanied the extreme magnetic storm of 1-2 September 1859. We use an inferred proton fluence for this event as estimated from nitrate levels in Greenland ice cores. We present results showing production of odd nitrogen compounds and their impact on ozone. We also compute rainout of nitrate in our model and compare to values from ice core data.Comment: Revised version including improved figures; Accepted for publication in Geophys. Res. Lett, chosen to be highlighted by AG

Biomass burning emission inventory with daily resolution: Application to aircraft observations of Asian outflow

Asian outflo

Stratospheric dryness

International audienceThe mechanisms responsible for the extreme dryness of the stratosphere have been debated for decades. A key difficulty has been the lack of models which are able to reproduce the observations. Here we examine results from a new atmospheric chemistry general circulation model (ECHAM5/MESSy1) together with satellite observations. Our model results match observed temperatures in the tropical lower stratosphere and realistically represent recurrent features such as the semi-annual oscillation (SAO) and the quasi-biennual oscillation (QBO), indicating that dynamical and radiation processes are simulated accurately. The model reproduces the very low water vapor mixing ratios (1?2 ppmv) periodically observed at the tropical tropopause near 100 hPa, as well as the characteristic tape recorder signal up to about 10 hPa, providing evidence that the dehydration mechanism is well-captured, albeit that the model underestimates convective overshooting and consequent moistening events. Our results show that the entry of tropospheric air into the stratosphere at low latitudes is forced by large-scale wave dynamics; however, radiative cooling can regionally limit the upwelling or even cause downwelling. In the cold air above cumulonimbus anvils thin cirrus desiccates the air through the sedimentation of ice particles, similar to polar stratospheric clouds. Transport deeper into the stratosphere occurs in regions where radiative heating becomes dominant, to a large extent in the subtropics. During summer the stratosphere is moistened by the monsoon, most strongly over Southeast Asia