[1] Large disagreements between measured and simulated NO 2 have been observed several times in the Arctic polar vortex. Here we report on the comparison of two sets of nighttime balloonborne measurements of the couple (OClO, NO 2 ) with Lagrangian model outputs in order to study the interactions between halogen and nitrogen species. Those measurements were characterized by the simultaneous presence of significant amounts of both species. Large disagreements are observed between modeled and measured NO 2 . Very surprisingly, good agreement can be achieved for OClO in spite of the supposed strong coupling between these two species. The only simultaneous agreement between model and measurements for both species occurs in the case of denoxified conditions, i.e., when there is no interaction between halogen and nitrogen compounds. Furthermore, agreement for OClO cannot be obtained if a source for NO 2 is assumed to fit the measurements of this specie. This result shows that some uncertainties still exist in the interaction between nitrogen and halogen species.
Recent theories of solid polar stratospheric clouds (PSCs) formation have shown that particles could remain liquid down to 3 K or 4 K below the ice frost point. Such temperatures are rarely reached in the Arctic stratosphere at synoptic scale, but nevertheless, solid PSCs are frequently observed. Mesoscale processes such as mountain‐induced gravity waves could be responsible for their formation. In this paper, a microphysical‐chemical Lagrangian model (MiPLaSMO) and a mountain wave model (NRL/MWFM) are used to interpret balloon‐borne measurements made by an optical particle counter (OPC) and by the Absorption par Minoritaires Ozone et NOx (AMON) instrument above Kiruna on February 25 and 26, 1997, respectively. The model results show good agreement with the particle size distributions obtained by the OPC in a layer of large particles, and allow us to interpret this layer as an evaporating mesoscale type Ia PSC (nitric acid trihydrate) mixed with liquid particles. The detection of a layer of solid particles by AMON is also qualitatively reproduced by the model and is interpreted to be frozen sulfate acid aerosols (SAT). In this situation, the impact of mountain waves on chlorine activation is studied. It appears that mesoscale perturbations amplify significantly the amount of computed ClO, as compared to synoptic runs. Moreover, MiPLaSMO chemical results concerning HNO3 and HCl agree with measurements made by the Limb Profile Monitor of the Atmosphere (LPMA) instrument on February 26 at a very close location to AMON, and explain part of the differences between LPMA measurement and Reactive Processes Ruling the Ozone Budget in the Stratosphere (REPROBUS) model outputs.
Abstract. We describe the diurnal cycle of ozone in the marine boundary layer measured at Reunion Island (21øS, 55øE) in the western part of the Indian Ocean in August-September 1995. Results from a box chemistry model are compared with ozone measurements at Reunion Island. We focus on the peak-to-peak amplitude of ozone concentration, since our measurements show a variation of about 4 parts per billion by volume, which is close to the value obtained by Johnson et al. [1990] during the SovietAmerican Gases and Aerosols (SAGA) 1987 Indian Ocean cruise. Different dynamical mechanisms are examined in order to reproduce such a variation. We conclude that the most important one is the exchange between the ozone-rich free troposphere and the ozone-poor boundary layer. This exchange is supposed to be more important during the night than during the day, allowing ozone nighttime recovery. This is the key point of the observed diurnal cycle, since daytime ozone photochemistry is well described by the model. Then we assume an entrainment velocity equal to 1 mm s -• during the day and 14 mm s -• during the night to closely match our measurements. Topography influences, together with clouds, are presumed to be responsible for this difference between nighttime and daytime entrainment velocities of free tropospheric air into the boundary layer at Reunion Island. Over the open ocean the difference of the turbulent flux of sensible heat between the day and the night explains the strong ozone nighttime recovery observed by us and by Johnson et al. [1990].
Abstract. In this study, we present an estimation of photochemical ozone production during free tropospheric transport between the African biomass burning area and Reunion Island (Indian Ocean) by means of trajectory-chemistry model calculations. Indeed, enhanced ozone concentrations (80-100 ppbv) between 5 and 8 km height over Reunion Island are encountered during September-October when African biomass burning is active. The measurements performed during flight 10 of the TRACE-A campaign (October 6, 1992) have been used to initialise the lagrangian trajectory-chemistry model and several chemical forward trajectories, which reach the area of Reunion Island some days later, are calculated. We show that the ozone burden already present in the middle and upper troposphere over Southern Africa, formed from biomass burning emissions, is further enhanced by photochemical production over the Indian Ocean at the rate of 2.5-3 ppbv/day. The paper presents sensitivity studies of how these photochemical ozone production rates depend on initial conditions. The rates are also compared to those obtained by other studies over the Atlantic Ocean. The importance of our results for the regional ozone budget over the Indian Ocean is briefly discussed.
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