Fluxes and (co-)variances of reacting scalars in the convective boundary layer

The effects of chemistry on the transport and the mixing of reacting scalars in the convective atmospheric boundary layer (CBL) are investigated. To do this, we use large-eddy simulation (LES) to calculate explicitly the different terms of the flux and (co)variance budget equations and to analyse in particular the role of the chemical term with respect to the thermodynamical terms. We examine a set of chemical cases that are representative of various turbulent reacting flows. The chemical scheme involves two reacting scalars undergoing a second-order reaction. In addition, we study a chemical cycle, based on a first- and a second-order reaction, to study the behaviour of chemical systems in equilibrium in turbulent flows. From the budget analysis, we found that the chemical terms become more relevant when the chemical timescale is similar to the turbulent timescale. In order to detemine the importance of the chemical terms, we compared these terms to the dynamical terms of the budget equations. For the flux of reactants, the chemical term becomes the dominant sink in the bulk of the CBL. As a result, flux profiles of reacting scalars have non-linear shapes. For the covariance, which accounts for the segregation of species in the CBL, the chemical term can act as a sink or source term. Consequently, reacting scalar covariance profiles deviate considerably from the inert scalar profile. When the chemistry is in equilibrium, the chemical term becomes negligible and therefore the flux and (co-)variance profiles are similar to those of inert scalrs. On the basis of the previous budget results, we develop a parameterisation that represents the segregation of reacting species in large-scale models under convective conditions. The parameterisation is applied to an atmospheric chemical mechanism that accounts for ozone formation and depletion in the CBL. We found a good agreement between the parameterisation and the LES results

Relative Humidity as an Indicator for Cloud Formation over Heterogeneous land surfaces

The influence of land surface heterogeneity on potential cloud formation is investigated using relative humidity as an indicator. This is done by performing numerical experiments using a large-eddy simulation model (LES). The land surface in the model was divided into two patches that had the same sum of latent and sensible heat flux but different Bowen ratios to simulate heterogeneous land surfaces. For heterogeneity in the meso-¿ scale (2¿20 km), sensitivity analyses were carried out on the heterogeneity amplitude (Bowen ratio difference between contrasting areas) and the inversion strength of potential temperature and specific humidity. The competition between absolute temperature decrease by ABL growth and dry air entrainment in heterogeneous conditions is analyzed using the LES results. First, it is shown that entrainment is located and enhanced over patches with higher Bowen ratios (warm patches) than their surroundings (cold patches). The heterogeneity-induced strong thermals can further penetrate the inversion at the ABL top, thereby reaching lower absolute temperatures than in homogeneous conditions. Second, because of the heterogeneity-induced circulations the moisture is located over the warm patch, and higher time-averaged RH values at the ABL top (RHzi) than over the cold patches are found here, even for dry atmospheres. These RHzi exceed values found over homogeneous land surfaces and are an indication that surface heterogeneity may facilitate cloud formation. In vertical profiles of RH, few differences are found between the homogeneous and heterogeneous cases, but the essential heterogeneity-induced modifications are within the domain variability

Zenith total delay study of a mesoscale convective system : GPS observations and fine-scale modelling

Zenith Total Delay (ZTD) observations and model calculations are used to analyze a mesoscale convective system which yielded a large amount of precipitation over a short period of time in the north-western Mediterranean. ZTD observations are derived from the GPS signal delay whereas the ZTD model results are calculated by means of the MM5 mesoscale model. Large values of the root-mean-square (rms) differences between the ZTD derived from the observations and the modeling are found for the maximum activity of the mesoscale convective system. It appears that the average bias between observations and modeling results is slightly affected (20%) by the passage of the storm system which is associated to the water vapor variability of the atmosphere. We have analyzed the ZTD differences in terms of the two components: the Zenith Hydrostatic Delay (ZHD) and the Zenith Wet Delay (ZWD). The hydrostatic error is mainly caused by the differences between the elevation of the GPS stations and the model topography and is reduced when using a more accurate topography data set. We propose a correction for this error assuming hydrostatic equilibrium. The remaining average ZTD difference is associated to the ZWD and is mainly generated by inaccuracies of the mesoscale model to predict the water vapor content during the rainfall event

Surface and boundary layer exchanges of volatile organic compounds, nitrogen oxides and ozone during the GABRIEL campaign

We present an evaluation of sources, sinks and turbulent transport of nitrogen oxides, ozone and volatile organic compounds (VOC) in the boundary layer over French Guyana and Suriname during the October 2005 GABRIEL campaign by simulating observations with a single-column chemistry and climate model (SCM) along a zonal transect. Simulated concentrations of O3 and NO as well as NO2 photolysis rates over the forest agree well with observations when a small soil-biogenic NO emission flux was applied. This suggests that the photochemical conditions observed during GABRIEL reflect a pristine tropical low-NOx regime. The SCM uses a compensation point approach to simulate nocturnal deposition and daytime emissions of acetone and methanol and produces daytime boundary layer mixing ratios in reasonable agreement with observations. The area average isoprene emission flux, inferred from the observed isoprene mixing ratios and boundary layer height, is about half the flux simulated with commonly applied emission algorithms. The SCM nevertheless simulates too high isoprene mixing ratios, whereas hydroxyl concentrations are strongly underestimated compared to observations, which can at least partly explain the discrepancy. Furthermore, the model substantially overestimates the isoprene oxidation products methlyl vinyl ketone (MVK) and methacrolein (MACR) partly due to a simulated nocturnal increase due to isoprene oxidation. This increase is most prominent in the residual layer whereas in the nocturnal inversion layer we simulate a decrease in MVK and MACR mixing ratios, assuming efficient removal of MVK and MACR. Entrainment of residual layer air masses, which are enhanced in MVK and MACR and other isoprene oxidation products, into the growing boundary layer poses an additional sink for OH which is thus not available for isoprene oxidation. Based on these findings, we suggest pursuing measurements of the tropical residual layer chemistry with a focus on the nocturnal depletion of isoprene and its oxidation products

Turbulent dispersion in cloud-topped boundary layers

Compared to dry boundary layers, dispersion in cloud-topped boundary layers has received less attention. In this LES based numerical study we investigate the dispersion of a passive tracer in the form of Lagrangian particles for four kinds of atmospheric boundary layers: 1) a dry convective boundary layer (for reference), 2) a "smoke" cloud boundary layer in which the turbulence is driven by radiative cooling, 3) a stratocumulus topped boundary layer and 4) a shallow cumulus topped boundary layer. We show that the dispersion characteristics of the smoke cloud boundary layer as well as the stratocumulus situation can be well understood by borrowing concepts from previous studies of dispersion in the dry convective boundary layer. A general result is that the presence of clouds enhances mixing and dispersion ¿ a notion that is not always reflected well in traditional parameterization models, in which clouds usually suppress dispersion by diminishing solar irradiance. The dispersion characteristics of a cumulus cloud layer turn out to be markedly different from the other three cases and the results can not be explained by only considering the well-known top-hat velocity distribution. To understand the surprising characteristics in the shallow cumulus layer, this case has been examined in more detail by 1) determining the velocity distribution conditioned on the distance to the nearest cloud and 2) accounting for the wavelike behaviour associated with the stratified dry environmen

On inferring isoprene emission surface flux from atmospheric boundary layer concentration measurements

We examine the dependence of the inferred isoprene surface emission flux from atmospheric concentration on the diurnal variability of the convective boundary layer (CBL). A series of systematic numerical experiments carried out using the mixed-layer technique enabled us to study the sensitivity of isoprene fluxes to the entrainment process, the partition of surface fluxes, the horizontal advection of warm/cold air masses and subsidence. Our findings demonstrate the key role played by the evolution of boundary layer height in modulating the retrieved isoprene flux. More specifically, inaccurate values of the potential temperature lapse rate lead to changes in the dilution capacity of the CBL and as a result the isoprene flux may be overestimated or underestimated by as much as 20%. The inferred emission flux estimated in the early morning hours is highly dependent on the accurate estimation of the discontinuity of the thermodynamic values between the residual layer and the rapidly forming CBL. Uncertainties associated with the partition of the sensible and latent heat flux also yield large deviations in the calculation of the isoprene surface flux. Similar results are obtained if we neglect the influence of warm or cold advection in the development of the CBL.We show that all the above-mentioned processes are non-linear, for which reason the dynamic and chemical evolutions of the CBL must be solved simultaneously. Based on the discussion of our results, we suggest the measurements needed to correctly apply the mixed-layer technique in order to minimize the uncertainties associated with the diurnal variability of the convective boundary layer

Mean and Flux Horizontal Variability of Virtual Potential Temperature, Moisture, and Carbon Dioxide: Aircraft Observations and LES Study

The effects of the horizontal variability of surface properties on the turbulent fluxes of virtual potential temperature, moisture, and carbon dioxide are investigated by combining aircraft observations with large-eddy simulations (LESs). Daytime fair-weather aircraft measurements from the 2002 International H2O Project¿s 45-km Eastern Track over mixed grassland and winter wheat in southeast Kansas reveal that the western part of the atmospheric boundary layer was warmer and drier than the eastern part, with higher values of carbon dioxide to the east. The temperature and specific humidity patterns are consistent with the pattern of surface fluxes produced by the High-Resolution Land Data Assimilation System. However, the observed turbulent fluxes of virtual potential temperature, moisture, and carbon dioxide, computed as a function of longitude along the flight track, do not show a clear east¿west trend. Rather, the fluxes at 70 m above ground level related better to the surface variability quantified in terms of the normalized differential vegetation index (NDVI), with strong correlation between carbon dioxide fluxes and NDVI

Interactions between dry-air entrainment, surface evaporation and convective boundary-layer development

The influence of dry-air entrainment on surface heat fluxes and the convective boundary-layer (CBL) properties is studied for vegetated land surfaces, using a mixed-layer CBL model coupled to the Penman¿Monteith equation under a wide range of conditions. In order to address the complex behaviour of the system, the feedback mechanisms involved were put into a mathematical framework. Simple expressions for the evaporative fraction and the Priestley¿Taylor parameter were derived, based on the concept of equilibrium evaporation. Dry-air entrainment enhances the surface evaporation under all conditions, but the sensitivity of the evaporation rate to the moisture content of the free troposphere falls as temperature rises. Due to the evaporation enhancement, shallower CBLs develop beneath dry atmospheres. In all cases, dry-air entrainment reduces the relative humidity at the land surface and at the top of the CBL. However, because of dry-air entrainment-induced land¿atmosphere feedback mechanisms, relative humidity at the top of the CBL responds nonlinearly to temperature rise; it decreases as temperature rises beneath a moist free troposphere, whereas it increases beneath a dry free troposphere. Finally, it was found that in certain conditions the evolution of the surface fluxes, relative humidity and CBL height can be as sensitive to the free tropospheric moisture conditions as to the land-surface properties. Therefore, studies of the land surface and of convective clouds have to take into account the influence of dry-air entrainment through land¿atmosphere feedback mechanism