High Rayleigh number convection with double diffusive fingers

An electrodeposition cell is used to sustain a destabilizing concentration difference of copper ions in aqueous solution between the top and bottom boundaries of the cell. The resulting convecting motion is analogous to Rayleigh-B\'enard convection at high Prandtl numbers. In addition, a stabilizing temperature gradient is imposed across the cell. Even for thermal buoyancy two orders of magnitude smaller than chemical buoyancy, the presence of the weak stabilizing gradient has a profound effect on the convection pattern. Double diffusive fingers appear in all cases. The size of these fingers and the flow velocities are independent of the height of the cell, but they depend on the ion concentration difference between top and bottom boundaries as well as on the imposed temperature gradient. The scaling of the mass transport is compatible with previous results on double diffusive convection

Modelling multiphase chemistry in deliquescent aerosols and clouds using CAPRAM3.0i

Modelling studies were performed with the multiphase mechanism RACM- MIM2ext/CAPRAM 3.0i to investigate the tropospheric multiphase chemistry in deli- quesced particles and non-precipitating clouds using the SPACCIM model framework. Simulations using a non-permanent cloud scenario were carried out for two different environmental conditions focusing on the multiphase chemistry of oxidants and other linked chemical subsystems. Model results were analysed by time-resolved reaction flux analyses allowing advanced interpretations. The model shows significant effects of multiphase chemical interactions on the tropospheric budget of gas-phase oxidants and organic com- pounds. In-cloud gas-phase OH radical concentration reductions of about 90 % and 75 % were modelled for urban and remote conditions, respectively. The reduced in-cloud gas- phase oxidation budget increases the tropospheric residence time of organic trace gases by up to about 30 %. Aqueous-phase oxidations of methylglyoxal and 1,4-butenedial were identified as important OH radical sinks under polluted conditions. The model revealed that the organic C3 and C4 chemistry contributes with about 38 %/48 % and 8 %/9 % consid- erably to the urban and remote cloud / aqueous particle OH sinks. Furthermore, the simulations clearly implicate the potential role of deliquescent particles to operate as a reactive chemical medium due to an efficient TMI/HOx,y chemical processing including e.g. an effective in-situ formation of OH radicals. Considerable chemical differences be- tween deliquescent particles and cloud droplets, e.g. a circa 2 times more efficient daytime iron processing in the urban deliquescent particles, were identified. The in-cloud oxidation of methylglyoxal and its oxidation products is identified as efficient sink for NO3 radicals in the aqueous phase

Treatment of non-ideality in the SPACCIM multiphase model – Part 1: Model development

Ambient tropospheric deliquesced particles generally comprise a complex mixture of electrolytes, organic compounds, and water. Dynamic modeling of physical and chemical processes in this complex matrix is challenging. Thus, up-to-date multiphase chemistry models generally do not consider non-ideal solution effects. Therefore, the present study was aimed at presenting further development of the SPACCIM (Spectral Aerosol Cloud Chemistry Interaction Model) through treatment of solution non-ideality, which has not been considered before. The present paper firstly describes the model developments including (i) the implementation of solution non-ideality in aqueous-phase reaction kinetics in the SPACCIM framework, (ii) the advancements in the coupling scheme of microphysics and multiphase chemistry and (iii) the required adjustments of the numerical schemes, especially in the sparse linear solver and the calculation of the Jacobian. Secondly, results of sensitivity investigations are outlined, aiming at the evaluation of different activity coefficient modules and the examination of the contributions of different intermolecular forces to the overall activity coefficients. Finally, first results obtained with the new model framework are presented. The SPACCIM parcel model was developed and, so far, applied for the description of aerosol–cloud interactions. To advance SPACCIM also for modeling physical and chemical processes in deliquesced particles, the solution non-ideality has to be taken into account by utilizing activities in reaction terms instead of aqueous concentrations. The main goal of the extended approach was to provide appropriate activity coefficients for solved species. Therefore, an activity coefficient module was incorporated into the kinetic model framework of SPACCIM. Based on an intercomparison of different activity coefficient models and the comparison with experimental data, the AIOMFAC approach was implemented and extended by additional interaction parameters from the literature for mixed organic–inorganic systems. Moreover, the performance and the capability of the applied activity coefficient module were evaluated by means of water activity measurements, literature data and results of other activity coefficient models. Comprehensive comparison studies showed that the SpactMod (SPACCIM activity coefficient module) is valuable for predicting the thermodynamic behavior of complex mixtures of multicomponent atmospheric aerosol particles. First simulations with a detailed chemical mechanism have demonstrated the applicability of SPACCIM-SpactMod. The simulations indicate that the treatment of solution non-ideality might be needed for modeling multiphase chemistry processes in deliquesced particles. The modeled activity coefficients imply that chemical reaction fluxes of chemical processes in deliquesced particles can be both decreased and increased depending on the particular species involved in the reactions. For key ions, activity coefficients on the order of 0.1–0.8 and a strong dependency on the charge state as well as the RH conditions are modeled, implying a lowered chemical processing of ions in concentrated solutions. In contrast, modeled activity coefficients of organic compounds are in some cases larger than 1 under deliquesced particle conditions and suggest the possibility of an increased chemical processing of organic compounds. Moreover, the model runs have shown noticeable differences in the pH values calculated with and without consideration of solution non-ideality. On average, the predicted pH values of the simulations considering solution non-ideality are -0.27 and -0.44 pH units lower under 90 and 70%RH con- ditions, respectively. More comprehensive results of detailed SPACCIM-SpactMod studies on the multiphase processing in organic–inorganic mixtures of deliquesced particles are described in a companion paper

Global fluctuations in magnetohydrodynamic dynamos

The spectrum of temporal fluctuations of total magnetic energy for several dynamo models is different from white noise at frequencies smaller than the inverse of the turnover time of the underlying turbulent velocity field. Examples for this phenomenon are known from previous work and we add in this paper simulations of the G.O. Roberts dynamo and of convectively driven dynamos in rotating spherical shells. The appearance of colored noise in the magnetic energy is explained by simple phenomenological models. The Kolmogorov theory of turbulence is used to predict the spectrum of kinetic and magnetic energy fluctuations in the inertial range

Tilt-over mode in a precessing triaxial ellipsoid

The tilt-over mode in a precessing triaxial ellipsoid is studied theoretically and numerically. Inviscid and viscous analytical models previously developed for the spheroidal geometry by Poincar\'e [Bull. Astr. 27, 321 (1910)] and Busse [J. Fluid Mech., 33, 739 (1968)] are extended to this more complex geometry, which corresponds to a tidally deformed spinning astrophysical body. As confirmed by three-dimensional numerical simulations, the proposed analytical model provides an accurate description of the stationary flow in an arbitrary triaxial ellipsoid, until the appearance at more vigorous forcing of time dependent flows driven by tidal and/or precessional instabilities.Comment: http://link.aip.org/link/doi/10.1063/1.350435

CAPRAM reduction towards an operational multiphase halogen and dimethyl sulfide chemistry treatment in the chemistry transport model COSMO-Muscat(5.04e)

A condensed multiphase halogen and dimethyl sulfide (DMS) chemistry mechanism for application in chemistry transport models is developed by reducing the CAPRAM DMS module 1.0 (CAPRAM-DM1.0) and the CAPRAM halogen module 3.0 (CAPRAM-HM3.0). The reduction is achieved by determining the main oxidation pathways from analysing the mass fluxes of complex multiphase chemistry simulations with the air parcel model SPACCIM (SPectral Aerosol Cloud Chemistry Interaction Model). These simulations are designed to cover both pristine and polluted marine boundary layer conditions. Overall, the reduced CAPRAM-DM1.0 contains 32 gas-phase reactions, 5 phase transfers, and 12 aqueous-phase reactions, of which two processes are described as equilibrium reactions. The reduced CAPRAM-HM3.0 contains 199 gas-phase reactions, 23 phase transfers, and 87 aqueous-phase reactions. For the aqueous-phase chemistry, 39 processes are described as chemical equilibrium reactions. A comparison of simulations using the complete CAPRAM-DM1.0 and CAPRAM-HM3.0 mechanisms against the reduced ones indicates that the relative deviations are below 5 % for important inorganic and organic air pollutants and key reactive species under pristine ocean and polluted conditions. The reduced mechanism has been implemented into the chemical transport model COSMO-MUSCAT and tested by performing 2D simulations under prescribed meteorological conditions that investigate the effect of stable (stratiform cloud) and more unstable meteorological conditions (convective clouds) on marine multiphase chemistry. The simulated maximum concentration of HCl is of the order of 109 molecules cm−3 and that of BrO is around 1×107 molecules cm−3, reproducing the range of ambient measurements. Afterwards, the oxidation pathways of DMS in a cloudy marine atmosphere have been investigated in detail. The simulations demonstrate that clouds have both a direct and an indirect photochemical effect on the multiphase processing of DMS and its oxidation products. The direct photochemical effect is related to in-cloud chemistry that leads to high dimethyl sulfoxide (DMSO) oxidation rates and a subsequently enhanced formation of methane sulfonic acid compared to aerosol chemistry. The indirect photochemical effect is characterized by cloud shading, which occurs particularly in the case of stratiform clouds. The lower photolysis rate affects the activation of Br atoms and consequently lowers the formation of BrO radicals. The corresponding DMS oxidation flux is lowered by up to 30 % under thick optical clouds. Moreover, high updraught velocities lead to a strong vertical mixing of DMS into the free troposphere predominately under cloudy conditions. The photolysis of hypohalous acids (HOX, X = Cl, Br, or I) is reduced as well, resulting in higher HOX-driven sulfite-to-sulfate oxidation in aerosol particles below stratiform clouds. Altogether, the present model simulations have demonstrated the ability of the reduced mechanism to be applied in studying marine aerosol–cloud processing effects in regional models such as COSMO-MUSCAT. The reduced mechanism can be used also by other regional models for more adequate interpretations of complex marine field measurement data

Towards an experimental von Karman dynamo: numerical studies for an optimized design

Numerical studies of a kinematic dynamo based on von Karman type flows between two counterrotating disks in a finite cylinder are reported. The flow has been optimized using a water model experiment, varying the driving impellers configuration. A solution leading to dynamo action for the mean flow has been found. This solution may be achieved in VKS2, the new sodium experiment to be performed in Cadarache, France. The optimization process is described and discussed, then the effects of adding a stationary conducting layer around the flow on the threshold, on the shape of the neutral mode and on the magnetic energy balance are studied. Finally, the possible processes involved into kinematic dynamo action in a von Karman flow are reviewed and discussed. Among the possible processes we highlight the joint effect of the boundary-layer radial velocity shear and of the Ohmic dissipation localized at the flow/outer-shell boundary

Dynamo action at low magnetic Prandtl numbers: mean flow vs. fully turbulent motion

We compute numerically the threshold for dynamo action in Taylor-Green swirling flows. Kinematic calculations, for which the flow field is fixed to its time averaged profile, are compared to dynamical runs for which both the Navier-Stokes and the induction equations are jointly solved. The kinematic instability is found to have two branches, for all explored Reynolds numbers. The dynamical dynamo threshold follows these branches: at low Reynolds number it lies within the low branch while at high kinetic Reynolds number it is close to the high branch.Comment: 4 pages, 4 figure

The influence of clouds on radical concentrations: observations and modelling studies of HOx during the Hill Cap Cloud Thuringia (HCCT) campaign in 2010

The potential for chemistry occurring in cloud droplets to impact atmospheric composition has been known for some time. However, the lack of direct observations and uncertainty in the magnitude of these reactions led to this area being overlooked in most chemistry transport models. Here we present observations from Mt Schmücke, Germany, of the HO2 radical made alongside a suite of cloud measurements. HO2 concentrations were depleted in-cloud by up to 90% with the rate of heterogeneous loss of HO2 to clouds necessary to bring model and measurements into agreement, demonstrating a dependence on droplet surface area and pH. This provides the first observationally derived assessment for the uptake coefficient of HO2 to cloud droplets and was found to be in good agreement with theoretically derived parameterisations. Global model simulations, including this cloud uptake, showed impacts on the oxidising capacity of the troposphere that depended critically on whether the HO2 uptake leads to production of H2O2 or H2O