Trace gas exchange at the air/water interface: Measurements of mass accommodation coefficients

A liquid jet of 90 m diameter and variable length has been utilized to determine absorption rates and, hence, mass accommodation coefficients , of atmospheric trace gases. The compounds investigated are HCl (0.01), HNO₃ (0.01), N₂O₅ (0.005), peroxyacetyl nitrate (>0.001), and HONO (0.005). It is concluded that the absorption of these trace gases by liquid atmospheric water is not significantly retarded by interfacial mass transport. The strengths and limitations of the liquid jet technique for measuring mass accommodation coefficients are explored.     

On the similarity in atmospheric fluctuations of carbon dioxide,water vapor and temperature over vegetated fields

This paper describes the similarity between atmospheric fluctuations of carbon dioxide, water vapor and temperature using data which cover a wide range of instability (0.02 < < 10). The is the Monin-Obukhov stability parameter including the humidity effect.The spectral analysis shows that the coherency between fluctuations of carbon dioxide and water vapor or temperature is very close to unity, and the phase difference is basically out of phase for whole frequency ranges analyzed. The stability dependence of the normalized standard deviation of carbon dioxide is very similar to those of water vapor and temperature. The normalized standard deviation is about 2.5 under near neutral conditions, and it decreases with increasing instability following the -1/3; power law as (-)^-1/3. The skewness factors of carbon dioxide, water vapor and temperature show a systematic departure with increasing instabilities for 0.02 < s- < 1, and level off at high instabilities for 1 < -\s < 10. The stability dependence of the flatness factors is not so clear as that noted in the standrard deviation and skewness factors. Dissipation rates of carbon dioxide, water vapor and temperature variance are well related to the spectral peak wavelength. This seems to be real since the local production and local dissipation rates are the main terms, almost balancing one another in the variance budget equations for scalar entities.     

Turbulence Reynolds number and the turbulent kinetic energy balance in the atmospheric surface layer

The relation between the turbulence Reynolds numberR and a Reynolds numberz* based on the friction velocity and height from the ground is established using direct measurements of the r.m.s. longitudinal velocity and turbulent energy dissipation in the atmospheric surface layer. Measurements of the relative magnitude of components of the turbulent kinetic energy budget in the stability range 0 >z/L 0.4 indicate that local balance between production and dissipation is maintained. Approximate expressions, in terms of readily measured micrometeorological quantities, are proposed for the Taylor microscale and the Kolmogorov length scale .     

Stable Isotope Ratios: Hurricane Olivia

The oxygen and hydrogen isotopic compositions of rains from HurricaneOlivia (1994) in the eastern Pacific were measured. The rains werecollected on 24 and 25 September during airplane flights conducted at anelevation of 3 km. Hurricane Olivia peaked in intensity to a category-4storm between the two dates. Isotope ratios of rains from HurricaneOlivia were markedly lower ( ¹⁸O = –13.9to –28.8) than that of rain collected from a thunderstormat an elevation of 2.3 km outside the influence of Olivia (¹⁸O = –3.8). A distinct decrease in isotoperatios from the first day to the next ( ¹⁸O =–18.4 to –21.9) in Hurricane Olivia wasattributed to decreased updraft velocities and outflow aloft. Thisshifted the isotopic water mass balance so that fewer hydrometeors werelifted and more ice descended to flight level. A decrease in the averagedeuterium excess from the first day to the next (d = 15.5 to 7.1)was attributed to an increase in the relative humidity of the watervapor `source' area. We hypothesize that the `source' region for therain was in the boundary layer near the storm center and that becausethe hurricane was at peak intensity prior to the second day the relative humidity was higher.     

ALPEX-Simulation

Summary In a project ALPEX-Simulation, sponsored by the Österreichischer Fond zur Förderung der wissenschaftlichen Forschung (FWF), all eight cases of ALPEX-SOP cyclones were numerically simulated with a fine mesh isentropic model of the atmosphere. These numerical simulations in six-hourly intervals allow a deeper insight into the synoptics and dynamics of the cyclogeneses in the Western Mediterranean, especially into the genesis of the two basic types of cyclones: the so-called Überströmungs-type and Vorderseiten-type. In the first phase of cyclogenesis of the Überströmungs-type, the blocking and flow splitting of the cold air due to the Alps and the canalization between the Alps and the Massif Central are important. Cold air flows cyclonically around the western part of the Alps, creating a vorticity maximum at the south western edge of the Alpine, bow and leads also to an enhanced PV. In connection with warm air in the Mediterranean, a strong baroclinic zone is generated. The interaction between the arriving PV maximum in the upper troposphere and the enhanced PV at the bottom leads to cyclogenesis in the Western Mediterranean. In the case of the Vorderseiten-type warm air advection dominates with the exception of a shallow layer of cold air in the inner Po-Valley, which is shielded by the Alpine ridge. A well-pronounced PV maximum builds up and couples with the PV maximum arriving at upper levels, even before the cold air, coming from the north-west, has surrounded the Alps. The cold air only intensifies the development by raising the baroclinity. Therefore, the Vorderseiten-cyclogenesis is an orographically modified cyclogenesis, in the course of which the cyclonic development is triggered by the Alps, whereas the Überströmungs-cyclogenesis is an orographically induced cyclogenesis i.e. a true lee cyclogenesis.With 14 FiguresDied in a tragic traffic accident on June 6, 1993.     

The behaviour of aerosol optical depth during clear summer days in Athens,Greece

Summary The integral aerosol optical depths (k ) at the hour of 08:20 Local Standard Time (LST), are compared with those calculated previously at 11:20 and 14:20 LST, for clear days during summer in Athens over the period 1962–1988. The mean values at 08:20 LST were consistently lower than the values at 11:20 and 14:20 LST. The influence of the vertical wind profile on the values ofk was also investigated. A comparison was made of the wind profiles at 02:00 and 14:00 LST, for days in which the 11:20 and 14:20 LST values ofk were 0.200 andk 0.350, respectively. The corresponding bulk wind shear s was also found for the period 1980–1988. The most significant results occurred with the first category of days. The resultant wind velocities from the surface to the 900 hPa level, in each hour were higher by 2–4 m·s^–1 with respect to the corresponding values for the second category. At 02:00 LST the bulk wind shear showed a considerable difference (1.8) between the two categories of days in the surface to 700 hPa layer at 02:00 LST. Finally, the associated weather conditions that appear to initiate a period of low values ofk (k 0.200) at 11:20 and 14:20 LST were examined for the period 1980–1988. Fifteen such cases were identified and it was found that they all occurred after the passage of weak cold fronts.With 6 Figures     

On the log-linear wind profile and the relationship between shear stress and stability characteristics over the sea

Wind and stability characteristics in the atmospheric surface boundary layer at a height,Z, less than 20 m above the sea were examined in nine oceanic investigations. The analysis lends further support to the utility of the log-linear wind-profile law in the stability region of –0.4Z/L0.9, whereL is the Monin-Obukhov length. However, it is also shown that, inasmuch as better than 90% of the measurements fall within the range of ¦Z/L¦ 0.25, and inasmuch as this correction to the drag coefficient under neutral conditions amounts to less than 10%, the familiar logarithmic wind law may be used rather than the log-linear form. A wind-stress drag coefficient,C _d (=1.2×10^–3 between 1.0 m Z 18.3 m), is thus recommended for general deepwater oceanic applications. The situation over shallow water, which is different, is discussed briefly.     

Nitrate in the atmospheric boundary layer of the tropical South Pacific: Implications regarding sources and transport

Weekly bulk aerosol samples collected at Funafuti, Tuvalu (8°30S, 179°12E), American Samoa (14°15S, 170°35W), and Rarotonga (21°15S, 159°45W), from 1983 through most of 1987 have been analyzed for nitrate and other constituents. The mean nitrate concentration is about 0.11 g m^–3 at each of these stations: 0.107±0.011 g m^–3 at Funafuti; 0.116±0.008 at American Samoa; and 0.117±0.010 at Rarotonga. Previous measurements of mineral aerosol and trace metal concentrations at American Samoa are among the lowest ever recorded for the near-surface troposphere and indicate that this region is minimally affected by transport of soil material and pollutants from the continents. Consequently, the nitrate concentration of 0.11 g m^–3 can be regarded as the natural level for the remote marine boundary layer of the tropical South Pacific Ocean. In contrast, over the tropical North Pacific which is significantly impacted by the transport of material from Asia and North America, the mean nitrate concentrations are about three times higher, 0.29 and 0.36 g m^–3 at Midway and Oahu, respectively. The major sources of the nitrate over the tropical South Pacific are still very uncertain. A very significant correlation between the nitrate concentrations at American Samoa and the concentrations of ²¹⁰Pb suggests that transport from continental sources might be important. This continental source could be lightning, which occurs most frequently over the tropical continents. A near-zero correlation with ⁷Be indicates that the stratosphere and upper troposphere are probably not the major sources. A significant biogenic source would be consistent with the higher mean nitrate concentrations, 0.16 to 0.17 g m^–3, found over the equatorial Pacific at Fanning Island (3°55N, 159°20W) and Nauru (0°32S, 166°57E). The lack of correlation between nitrate and nss sulfate at American Samoa does not necessarily preclude an important role for marine biogenic sources.     

The validation of various schemes for parameterizing evaporation from bare soil for use in meteorological models: A numerical study using in situ data

Parameterization of evaporation from a non-plant-covered surface is very important in the hierarchy strategy of modelling land surface processes. One of the representations frequently used in its computation is the resistance formulation. The performance of the evaporation schemes using the , , and their combination resistance approaches to parameterize evaporation from bare soil surfaces is discussed. For that purpose, the nine schemes, based on a different dependence of and on volumetric soil moisture content and its saturated value, are used.The tests of performances of the considered schemes are based on time integrations by the land surface module (BARESOIL) using observed data. The 23 data sets at a bare surface experimental site in Rimski anevi, Yugoslavia on chernozem soil, were used for the resistance algorithm evaluation. The quality of the schemes was compared with the observed values of the latent heat flux using several statistical parameters.     

Modification Of The Standard ∈-Equation For The Stable Abl Through Enforced Consistency With Monin–Obukhov Similarity Theory

A condition is derived for consistency of the standard-equation with Monin–Obukhov (MO) similarity theory of thestably-stratified surface layer. The condition is derivedby extending the procedure used to derive the analogous condition forneutral theory to stable stratification. It is shown that consistencywith MO theory requires a function of flux Richardson number, Ri_f, to be absorbed into either of two closure parameters, c ₁ or c ₂.Inconsistency, on the other hand, results if constant values of these are maintained for all Ri_f, as is done in standardapplication of the equation, and the large overpredictions ofturbulence found in such application to the one-dimensionalstable atmospheric boundary layer (1D-SBL) are traced to thisinconsistency. Guided by this, we formulate a MO-consistent-equation by absorbing the aforementioned function intoc ₁, and combine this with a Level-2.5 second-orderclosure model for vertical eddy viscosity and diffusivities.Numerical predictions of the 1D-SBL by the modified model converge to a quasi-steady state, rectifying the predictive failure of the standard -equation for the case.Quasi-steady predictions of non-dimensional variables agree stronglywith Nieuwstadt's theory. Qualitative accuracy of predictionsis inferred from comparisons to field data, large-eddy simulationresults and Rossby-number similarity relationships.     

Numerical modelling of the turbulent flow developing within and over a 3-d building array,part iii: a istributed drag force approach,its implementation and application

A modified k- model is used for the simulation of the mean wind speed and turbulence for a neutrally-stratified flow through and over a building array, where the array is treated as a porous medium with the drag on the unresolved buildings in the array represented by a distributed momentum sink. More specifically, this model is based on time averaging the spatially averaged Navier–Stokes equation, in which the effects of the obstacle-atmosphere interaction are included through the introduction of a distributed mean-momentum sink (representing drag on the unresolved buildings in the array). In addition, closure of the time-averaged, spatially averaged Navier–Stokes equation requires two additional prognostic equations, namely one for the time-averaged resolved-scale kinetic energy of turbulence,, and another for its dissipation rate, . The performance of the proposed model and some simplified versions derived from it is compared with the spatially averaged, time-mean velocity and various spatially averaged Reynolds stresses diagnosed from a high-resolution computational fluid dynamics (CFD) simulation of the flow within and over an aligned array of sharp-edged cubes with a plan area density of 0.25. Four different methods for diagnosis of the drag coefficient C_Dfor the aligned cube array, required for the volumetric drag force representation of the cubes, are investigated here. We found that the model predictions for mean wind speed and turbulence in the building array were not sensitive to the differing treatments of the source and sink terms in the and equations (e.g., inclusion of only the `zeroth-order' approximation for the source/sink terms compared with inclusion of a higher-order approximation for the source/sink terms in the and equations), implying that the higher-order approximations of these source/sink terms did not offer any predictive advantage. A possible explanation for this is the utilization of the Boussinesq linear stress–strain constitutive relation within the k– modelling framework, whose implicit omission of any anisotropic eddy-viscosity effects renders it incapable of predicting any strong anisotropy of the turbulence field that might exist in the building array.     

Re-analysis of the nuclear winter phenomenon

Summary An analysis of the report of the (U.S.) National Academy of Sciences (NAS) on atmospheric effects of a nuclear exchange leads to conclusions that differ from those of the NAS and of the earlier TTAPS and AMBIO studies. Any cooling of the earth's surface is likely to beshort-lived because of rapid removal of the smoke clouds originating from nuclear burst-initiated fires, andminor because of appreciable green-house effects due to several distinct physical causes. (One of these, neglected in prior analyses, is the infrared absorption from cirrus clouds produced directly by the nuclear bursts.) Taken together, these effects may even induce slight surface warming (nuclear summer) instead of cooling (nuclear winter). The consequences to atmospheric ozone are similarly ambiguous; depending on the detailed nuclear scenario, the net ozone content may increase-rather than decrease as argued by TTAPS. Experiments could settle some uncertainties.With 2 Figures     

Transport-Dissipation Analytical Solutions to the E-∈Turbulence Model and their Role in Predictions of the Neutral ABL

E- turbulence model predictions of the neutralatmospheric boundary layer (NABL) are reinvestigated to determine thecause for turbulence overpredictions found in previous applications. Analytical solutions to the coupled E and equations for the case of steady balance between transport and dissipation terms, the dominant balance just below the NABL top, are derived. It is found that analytical turbulence profiles laminarizeat a finite height only for values of closure parameter ratio c ₂ /_e equal toor slightly greater than one, with laminarization as z for greater . The point = 2 is additionally foundthat where analytical turbulent length scale (l) profilesmade a transition from ones ofdecreasing ( < 2) to increasing ( > 2)values with height. Numerically predicted profiles near the NABL topare consistent with analytical findings. The height-increasingvalues of l predicted throughout the NABL with standard values ofclosure parameters thus appear a consequence of 2.5(> 2), implied by these values (c ₂ = 1.92, _{= 1.3}, _{e = 1}). Comparison of numericalpredictions with DNS data shows that turbulence overpredictions obtained with standard-valued parameters are rectifiedby resetting and _e to 1.1 and 1.6, respectively, giving, with c ₂ = 1.92, 1.3, and laminarization of the NABL's cappingtransport-dissipation region at a finite height.     

Numerical modelling of the turbulent flow developing within and over a 3-d building array,part ii: a mathematical foundation for a distributed drag force approach

In this paper, we lay the foundations of a systematic mathematical formulation for the governing equations for flow through an urban canopy (e.g., coarse-scaled building array) where the effects of the unresolved obstacles on the flow are represented through a distributed mean-momentum sink. This, in turn, implies additional corresponding terms in the transport equations for the turbulence quantities. More specifically, a modified k-- model is derived for the simulation of the mean wind speed and turbulence for a neutrally stratified flow through and over a building array, where groups of buildings in the array are aggregated and treated as a porous medium. This model is based on time averaging the spatially averaged Navier--Stokes equations, in which the effects of the obstacle--atmosphere interaction are included through the introduction of a volumetric momentum sink (representing drag on the unresolved buildings in the array).The k-- turbulence closure model requires two additional prognostic equations, namely one for the time-averaged resolved-scale kinetic energy of turbulence,, and another for the dissipation rate, , of . The transport equation for is derived directly from the transport equation for the spatially averaged velocity, and explicitly includes additional sources and sinks that arise from time averaging the product of the spatially averaged velocity fluctuations and the distributed drag force fluctuations. We show how these additional source/sink terms in the transport equation for can be obtained in a self-consistent manner from a parameterization of the sink term in the spatially averaged momentum equation. Towards this objective, the time-averaged product of the spatially averaged velocity fluctuations and the distributed drag force fluctuations can be approximated systematically using a Taylor series expansion. A high-order approximation is derived to represent this source/sink term in the transport equation for . The dissipation rate () equation is simply obtained as a dimensionally consistent analogue of the equation. The relationship between the proposed mathematical formulation of the equations for turbulent flow within an urban canopy (where the latter is treated as a porous medium) and an earlier heuristic two-band spectral decomposition for parameterizing turbulence in a plant canopy is explored in detail.     

Airflow above changes in surface heat flux,temperature and roughness; an extension to include the stable case

A numerical model of airflow above changes in surface roughness and thermal conditions is extended to include cases with stable thermal stratification within the internal boundary-layer. The model uses a mixing-length approach with empirical forms for M and H.Results are presented for some basic cases and an attempt is then made to compare results given by the model with the experimental results of Rider, Philip and Bradley. Tolerable agreement is achieved. The importance of roughness change and thermal stability effects in the diffusion of heat and moisture near a leading edge is emphasised.Notation A Refers to Taylor (1970) - B Businger-Dyer constant (= 16.0) in forms for _M and _H - C Constant in form for in stable case - c _p Specific heat at constant pressure - E Scaled absolute humidity - g Acceleration due to gravity - H Upward vertical heat flux - H ₀, H ₁ Surface heat fluxes for x <0, x0 - H _E Upward latent heat flux - k Von Kármán's constant (= 0.4) - K _H K _W Eddy transfer coefficients for heat and water vapour - L Monin-Obukhov length - L _H Latent heat of evaporation for water - m Ratio of roughness lengths ( = z ₁/z ₀) - RPB Refers to Rider et al. (1964) - RL* Non-dimensional parameter (see Equations (9), (20a), (22a), (24a)) - R* Net radiation less ground heat flux (see Equations (15), (16)) - T Scaled temperature - T ₁ Downstream scaled surface temperature - u ₀ u ₁(x) Surface friction velocities for x <0, x0 - U, W Horizontal and vertical mean velocities - x, z Horizontal and vertical co-ordinates - Z _i Local roughness length - z ₀, z _i Roughness lengths for x < 0, x 0 - Temperature - ₀, ₁ Surface temperatures for x<0, x0 - _E Non-dimensional absolute humidity gradient - _H Non-dimensional temperature gradient of heat flux - _M Non-dimensional wind shear - = _M = _H = _E an assumption used in stable conditions - Air density - Absolute humidity - _w Density of water - Kinematic shear stress - Logarithmic height scale (= ln(z+z ₁)/z ₁)     

Nine fallacies of natural disaster: The case of the Sahel

This article presents nine statements which are generally accepted as true. However, when they are applied to a particular situation, in this case the recent prolonged drought in the Sahelian zone in West Africa, they are as often untrue as they are true. For example, such generalizations as people learn from their mistakes or when the rains come, everything will return to normal or technology is the answer, when applied uncritically to a specific situation often prove to become part of the problem as well as a hindrance to the attainment of a solution to that problem.It is strongly suggested that these nine generalizations, here called fallacies, be carefully assessed when applied, thereby removing one more obstacle in dealing with environmental problems in general and natural hazards in particular.Published in Michael H. Glantz (ed.), The Politics of Natural Disasters: The Case of the Sahel Drought (NY: Praeger Publ., 1976) reprinted by permission.Michael H. Glantz is a scientist in the Advanced Study Program at the National Center for Atmospheric Research which is sponsored by the National Science Foundation.     

Analysis of Astex-Stratocumulus Observational Data Using a Mass-Flux Approach

A mass-flux approach is applied to observational data obtained in a convective boundary layer topped with stratocumulus clouds. The observational data were obtained from aircraft measurements during the Atlantic Stratocumulus Transition Experiment (ASTEX). A conditional sampling method is used to calculate average updraft and downdraft values. The vertical fluxes calculated with the mass-flux approach are found to be proportional to the real (measured) fluxes, with a proportionality factor being about 0.6. This value is predicted by theory for two variables having a joint Gaussian distribution function; proportionality factor = 2^-1 0.637. The horizontal fractional entrainment and detrainment rates calculated from the data ( 1–2 × 10^-2 m^-1) are an order of magnitude higher than the rates obtained by large eddy simulations for cumulus convection ( 2–3 × 10^-3 m^-1) and two orders of magnitude higher than those used in modelling cumulus convection with a mass-flux scheme in an operational weather forecast model ( 3 × 10^-4 m^-1). A numerical mass-flux model for the thermodynamics was developed and showed that results are in good agreement when compared with measured profiles of the liquid water content.     

On Trajectory Curvature as a Selection Criterion for Valid Lagrangian Stochastic Dispersion Models

Recently Wilson and Flesch (Boundary-Layer Meteorology, 84, 411-426, 1997) suggested that the average increment d z to the orientation = arctan(w/u) of the Lagrangian velocity-fluctuation vector can be used to distinguish the better Lagrangian stochastic models within the well-mixed class. Here it is demonstrated that the specification of d z constitutes neither a sufficient or universally applicable criterion to distinguish the better Lagrangian stochastic models within the well-mixed class. The hypothesis made by Wilson and Flesch that Lagrangian stochastic models with /P_E irrotational are zero-spin models, having d z=0, is proven     

Gas-Phase Ozone Oxidation of Monoterpenes: Gaseous and Particulate Products

Atmospheric oxidation of monoterpenes contributes to formation of tropospheric ozone and secondary organic aerosol, but their products are poorly characterized. In this work, we report a series of outdoor smog chamber experiments to investigate both gaseous and particulate products in the ozone oxidation of four monoterpenes: -pinene, -pinene, ³-carene, and sabinene. More than ten oxygenated products are detected and identified in each monoterpene/O₃ reaction by coupling derivatization techniques and GC/MS detection. A denuder/filter pack sampling system is used to separate and simultaneously collect gas and aerosol samples. The identified products, consisting of compounds containing carbonyl, hydroxyl, and carboxyl functional groups, are estimated to account for about 34–50%, 57%, 29–67%, and 24% of the reacted carbon mass for -pinene, sabinene, -pinene, and ³-carene, respectively. The identified individual products account for >83%, 100%, >90%, and 61% of the aerosol mass produced in the ozone reaction of -pinene, sabinene, -pinene, and ³-carene. The uncertainty in the yield data is estimated to be ±50%. Many of the products partition between gas and aerosol phases, and their gas-aerosol partitioning coefficients are determined and reported here. Reaction schemes are suggested to account for the products observed.     

The Value Of The β Coefficient In The Relaxed Eddy Accumulation Method In Terms Of Fourth-Order Moments

The commonly measured value of in the relaxed eddy accumulationmethod of about 0.56is shown to arise from the non-Gaussiannature of turbulence. Fourth-orderGram–Charlier functions forthe two-dimensional probability distributionsof variation in the horizontal component of wind velocityand concentrations of water vapour, carbondioxide and methane with respect to thevertical component of wind velocity are used to examinethe value of .An analytical solution for ispresented in terms of fourth-order moments.Under mean conditions, this solution givesa value for of0.557. Variation of is shown to be controlledprimarily by the ratio of the mean ofc'w3 (where c'is relevant to the entity of interest andw' is vertical component of windvelocity) to the correlationcoefficient between the entity concentrationand vertical component of wind velocity.