Towards an online-coupled chemistry-climate model: evaluation of trace gases and aerosols in COSMO-ART

Peer reviewe

Strong influence of lowermost stratospheric ozone on lower tropospheric background ozone changes over Europe

Using ozone measurements from two sounding sites and two high-altitude stations in Central Europe, we show evidence for a dominant influence of changes in lowermost stratospheric ozone on the variability and overall upward trend of background ozone in the lower troposphere (3000-3500 m asl) during the 1992-2004 period. Numerical simulations with a stratospheric chemistry transport model suggest that changes in lower stratospheric ozone were driven by dynamics rather than by changes in stratospheric chlorine loading. In addition, Lagrangian model simulations indicate that changes in downward transport of ozone from the stratosphere into the troposphere were dominated by changes in lowermost stratospheric ozone concentrations rather than by variations of cross-tropopause air mass transport. This suggests that the positive ozone trends and concentration anomalies in the lower free troposphere over Europe during the 1990s were likely to a large extent due to enhanced stratospheric ozone contributions, particularly in winter-spring. Copyright 2007 by the American Geophysical Union

Quantifying the ionic reaction channels in the Secondary Organic Aerosol formation from glyoxal

International @ AIR+AMX:BNO:SRS:CGOInternational audienceGlyoxal, a common organic gas in the atmosphere, has been identified in recent years as an important Secondary Organic Aerosol (SOA) precursor (Volkamer et al., 2007). But, unlike with other precursors, the SOA is largely produced by particle-phase reactions (Volkamer et al., 2009) and equilibria (Kampf et al. 2013) that are still not entirely characterized. Since 2009 series of smog chamber experiments have been performed within the Eurochamp program at the Paul Scherrer Institute, Switzerland, to investigate SOA formation from glyoxal. In these experiments, glyoxal was produced by the gas-phase oxidation of acetylene in the presence of seeds, the seed composition and other conditions being varied. The 2011 campaign resulted in the identification of salting processes controlling the glyoxal partitioning in the seeds (Kampf et al. 2013). This presentation will report results of the 2013 campaign focusing on the identification of the various reactions (ionic or photo-induced) contributing to the SOA mass. In particular, the contribution of the ionic reactions, i.e. mediated by NH4+, were investigated by quantifying the formation of imidazoles (imidazole, imidazole-2-carboxaldehyde, 2,2-biimidazole) from the small condensation channel of glyoxal with ammonia. For this, the SOA produced were collected on quartz filters and analyzed by Orbitrap LC/MS (Q-Exactive Thermo Fisher). The formation of other products such as organic acids was also investigated to determine potential competing reactions. Time-resolved MOUDI sampling coupled with nano-DESY/ESI-MS/MS analysis was also used to identify nitrogen- and sulphur-containing products from all the reactions. The results obtained for a range of conditions will be presented and compared with recent mechanistic information on the ionic reaction channels (Nozičre et al., in preparation, 2013). The implementation of all this new information into a glyoxal-SOA model will be discussed