Feature-based predictability of 500 hpa height in the Australia-New Zealand region

Summary Feature-based predictability stratifies forecast model errors on the basis of individual weather systems. We examine only one level and chose very simple categories: high, cut-off low, trough and block. European Centre for Medium-range Weather Forecasts data are used. We emphasize systems found near Australia and New Zealand during winter 1987. Calculations for the preceding summer and fall and for other midlatitude regions of the southern hemisphere yield similar results.The approach herein is fully automated and simple to implement. Features are identified in the verification field. Then an error calculation is made on moving grids that are each centered upon and contain one system.The total error is the root mean square difference (RMS) between forecast and verification. The structural error is the RMS difference when the forecast and verification small grids are independently centered upon the corresponding feature in each field. The difference between the structural and total errors, called the locational error, is typically a quarter of the total. Even when normalized by presistence, highs are forecast better than troughs; cut-off lows and troughs have similar errors. The distance between the forecast and observed positions is typically 3° longitude west and 0.5° latitude north of where features should be at 72 hours. The model has a systematic bias of too small amplitude of vorticity. No relation is found between skill and jet stream splitting.With 4 Figures     

Fog chemistry during EUMAC Joint Cases: Analysis of routine measurements in southern Germany and model calculations

Summary The role of fog events for acid production and moist deposition in southern Germany during three EUMAC Joint Cases has been investigated by analysis of routine measurements and simulations with a one-dimensional fog-chemistry model. To identify the chemical and meteorological conditions, routine measurements by different institutions have been interpreted. The periods under consideration include a smog episode with low photooxidant concentrations during the Winter Case in February 1982. The Wet Case in spring 1986 represents a period with higher photooxidant concentrations. Conditions which are mostly characterized by low SO₂ and oxidant concentrations and comparatively high pH-values in the fog are given during the SANA 1 case in autumn 1990. Fog mostly occurs as a subscale phenomenon, but sometimes it can also cover large areas and it can contribute significantly to moist deposition.The model results indicate that the liquid phase sulfate production in the fog layer may even exceed the gas phase production during 24 hours within a layer of the same height occasionally. On the other hand, during the SANA 1 case the sulfate production in the fog was extremely low at night due to lack of oxidants and SO₂. Depending on the dissipation time of the fog a remarkable effect on the photolysis rates is possible. Since a significant amount of particulate mass is lost by moist deposition during fog, it is evident that fog events can have a noticeable effect on some of the gas phase constituents which are easily soluble.With 17 Figures     

Gas and Particle Products Distribution from the Reaction of β-Caryophyllene with Ozone

Gas and particulate reaction products from the ozonolysis of -caryophyllene (I) in the presence of atmospheric air were investigated using a combination of gas chromatography-mass spectrometry (GC-MS) and high performance liquid chromatography (HPLC). A Scanning Mobility Particle Sizer system (3936, TSI) and a Condensation Particle Counter (3025A, TSI) were used to study secondary organic aerosol formation. The nighttime oxidation was carried out in a large outdoor smog chamber (190 m³). A wide range of ring retaining and ring opening products in the gas and particle phase are reported over the course of the reaction. On average, measured gas and particle phase products accounted for 64% of the reacted -caryophyllene (I) carbon. Measurements show that a number of reaction products with low vapor pressure (e.g., -caryophyllone aldehyde (IV), -norcaryophyllone aldehyde (V), -caryophyllonic acid (VIII), -14-hydroxycaryophyllonic acid (XIV)) were found in the sample taken during the first 20 min of the reaction and may play an important role in the early formation of secondary organic aerosol. A detailed mechanism is proposed to account for most products observed in this investigation.     

The carbon isotopic ratio of atmospheric carbon dioxide at Tsukuba,Japan

To find out the secular and seasonal trends of the ¹³C value and CO₂ concentration in the surface air and the determination of the ¹³C in the atmospheric CO₂ collected at Tsukuba Science City was carried out during the period from July 1981 to October 1983. The monthly average of the ¹³C value of CO₂ in the surface air collected at 1400 LMT ranged from -7.52 to \s-8.45 with an average of -7.96±0.25 and the CO₂ concentration in the air varied from 334.5 l 1^-1 to 359 l 1^-1 with an average of 347.2±6.3 l 1^-1. The ¹³C value is high in summer and low in winter and is negatively correlated with the CO₂ concentration. In general, the relationship between the ¹³C and the CO₂ concentration is explainable by a simple mixing model of two different constant carbon isotopic species but the relationship does not always follow the model. The correlation between the ¹³C value and the CO₂ concentration is low during the plant growth season and high at other times. The observed negative deviation of the ¹³C value from the simple mixing model in the plant growth season is partly due to the isotopic fractionation process which takes place in the land biota.     

The representation of foreseeable natural risks: A contribution to a new cartography of Avalanches

Summary Research carried out on a favourable site in the Pre-Alps of Savoy has allowed the development of risk cartography where avalanche phenomena are defined according to three criteria: maximum extension, type of avalanche, and frequency of avalanche. The maps, composed of simple symbols, allowing easy updating, could be a useful tool for mountain professionals.With 4 Figures     

Final results of the CONDORS convective diffusion experiment

TheConvectiveDiffusionObserved byRemoteSensors (CONDORS) field experiment conducted at the Boulder Atmospheric Observatory used innovative techniques to obtain three-dimensional mappings of plume concentration fields, /Q, of oil fog detected by lidar and chaff detected by Doppler radar. It included extensive meteorological measurements and, in 1983, tracer gases measured at a single sampling arc. Final results from ten hours of elevated and surface release data are summarized here. Many intercomparisons were made. Oil fog /Q measured 40m above the arc are mostly in good agreement withSF ₆ values, except in a few instances with large spacial inhomogeneities over short distances. After a correction scheme was applied to compensate for the effect of its settling speed, chaff dy/Q agreed well with those of oil except in two cases of oil fog hot spots. Mass or frequency distribution vs. azimuth or elevation angle comparisons were made for chaff, oil, and wind, with mostly good agreements. Spacial standard deviations, _y and _z, of chaff and oil agree overall and are consistent at short range with velocity standard deviations _vand _w 0.6w^* (the convective scale velocity), as measured atz>100m. Surface release _y is enhanced up to 60% at smallx, consistent with the Prairie Grass measurements and with larger _v and reduced wind speed measured near the surface. Decreased _y at small dimensionless average times is also noted. Finally, convectively scaled dy, C _y, were plotted versus dimensionlessx andz for oil, chaff, and corrected chaff for each 30–60 min period. Aggregated CONDORSC _y fields compare well with laboratory tank and LES numerical simulations; surface-released oil fog compares expecially well with the tank experiments. However, large deviations from the norm occurred in individual averaging periods; these deviations correlated strongly with anomalies in measured distributions.On assignment to the US Environmental Protection Agency, Atmospheric Research and Exposure Assessment Laboratory, RTP, NC.     

The Effect of Atmospheric Stability on the Surface-Layer Characteristics in a Low-Wind Area of Tropical West Africa

This study details the observed effects ofatmospheric stability on characteristics of thesurface layer in a low wind speed (U = 1.5 m s-1)regime of tropical West Africa. Theaerodynamic roughness length, z0, anddisplacement height, d, obtained from profilewind-speed data at our bush land site (height 2 m)have values of 0.24 ± 0.10 m and 1.54 ± 0.04 mrespectively. In the unstable range (-2.5 < Ri < -0.1; Riis gradient Richardson number), thestandard deviation in wind speed fluctuations, u, increased from 0.57 ± 0.19 m s-1 toa maximum of 0.7 ± 0.2 m s-1 in near-neutralconditions, and in the stable range, the parameterdecreased rapidly to 0.41 ± 0.15 m s-1 at Ri 0.2.In the same stability range, the horizontal winddispersion, , decreased withincreasing stability from 19 ± 8 deg. to 13 ± 5 deg.The surface-layer integral quantity, u/u*, when plottedas a function of stability, is in agreement with theempirical results. The ratio ofsensible heat flux (estimated) to the net radiationranged between 0.1 and 0.2 at nighttime,increasing to about 0.5 during the daytime, and showeda strong dependency on season.     

Evaporation from a blanket bog in a foggy coastal environment

Frequent fog severely restricts evaporation from blanket bogs in Newfoundland because it more than halves the radiant energy input, and it eliminates the vapor pressure deficit, resulting in evaporation at the equilibrium rate (average = 0.99 during fog). During these periods, there is no surface resistance to evaporation because the bog has been wetted by fog drip, and although the latent heat flux dominates over sensible heat (average = 0.8), both are small. In contrast, the surface dries during clear periods, increasing the surface resistance to evaporation so that sensible heat becomes more important ( = 1.05). When the mosses are dry, evaporation is below the equilibrium rate ( = 0.87), although the higher available energy ensures that actual evaporation is higher. During clear periods, daily evaporation averaged 2.5 mm, compared to 1.1 and 0.7 mm for fog and rain, respectively. The suppressed evaporation at this site is important in maintaining appropriate hydrological conditions for blanket bog development.     

Measurement of isoprene and its atmospheric oxidation products in a central Pennsylvania deciduous forest

Ambient concentrations of isoprene and several of its atmospheric oxidation productsmethacrolein, methylvinyl ketone, formaldehyde, formic acid, acetic acid, and pyruvic acid-were measured in a central Pennsylvania deciduous forest during the summer of 1988. Isoprene concentrations ranged from near zero at night to levels in excess of 30 ppbv during daylight hours. During fair weather periods, midday isoprene levels normally fell in the 5–10 ppbv range. Methacrolein and methylvinyl ketone levels ranged from less than 0.5 ppbv to greater than 3 ppbv with average midday concentrations in the 1 to 2 ppbv range. The diurnal behavior of formaldehyde paralleled that of isoprene with ambient concentrations lowest (1 ppbv) in the predawn hours and highest (>9.0 ppbv) during the afternoon. The organic acids peaked during the midday period with average ambient concentration of 2.5, 2.0, and 0.05 ppbv for formic, acetic, and pyruvic acid, respectively. These data indicate that oxygenated organics comprise a large fraction of the total volatile organic carbon containing species present in rural, forested regions of the eastern United States. Consequently, these compounds need to be included in photochemical models that attempt to simulate oxidant behavior and/or atmospheric acidity in these forested regions.     

The Askervein Hill Project: Mean wind variations at fixed heights above ground

This is one of a series of papers on the Askervein Hill Project. It presents results on the variations in mean wind speed at fixed heights (z) above the ground from linear arrays of anemometer posts and towers. Most of the data are for z = 10 m but some are for z = 3 m. Selected and directionally grouped data from the 55 Mean Flow runs are presented together with mean flow data from Askervein '83 Turbulence runs. Comparisons are made between the data and guideline estimates of fractional speed-up ratio at hilltop locations and between the data and MS3DJH/3 model predictions along the tower lines. There is good agreement in most cases.     

The Reaction of Unsaturated Aliphatic Oxygenates with Ozone

The reaction of ozone with unsaturated aliphatic oxygenates has been studied at ambient T (287–297 K) and p = 1 atm. of air (RH = 55 ± 10%) with sufficient cyclohexane added to scavenge the hydroxyl radical. Reaction rate constants, in units of 10-18 cm3 molecule-1 s-1, are 10.7 ± 1.4 for methyl trans-3-methoxy acrylate, 63.7 ± 9.9 for 4-hexen-3-one (predominantly the trans isomer), 125 ± 17 for trans-4-methoxy-3-buten-2-one, 148 ± 13 for cis-4-heptenal, 439 ± 37 for 3- methyl-2-buten-1-ol and 585 ± 132 for (cis + trans)-ethyl 1-propenyl ether. The influence of the oxygen-containing substituents on reactivity toward ozone is examined. Unsaturated ethers react with ozone faster than their alkene structural homologues; the reverse is observed for unsaturated esters and unsaturated carbonyls. Major reaction products have been identified by liquid chromatography with ultraviolet detection (LC-UV), particle beam-mass spectrometry (PB- MS) and gas chromatography-mass spectrometry (GC-MS) and are methyl formate and methyl glyoxylate from methyl trans-3-methoxy acrylate, acetaldehyde and 2-oxobutanal from 4-hexen-3-one, propanal and succinic dialdehyde from cis-4-heptenal, hydroxyacetaldehyde and acetone from 3-methyl-2-buten-1-ol, and ethyl formate and acetaldehyde from (cis + trans)-ethyl 1-propenyl ether. PB-MS and GC- MS were also employed to identify new reaction products and to confirm the structure of products tentatively identified in a previous study of the reaction of ozone with five unsaturated oxygenates (Grosjean and Grosjean, 1997a): formic acid and methyl glyoxylate from methyl acrylate, formic acid and formic acetic anhydride from vinyl acetate, 2-oxoethyl acetate and 3-oxopropyl acetate from cis-3-hexenyl acetate, ethyl formate and formic acid from ethyl vinyl ether, and methyl formate from trans-4-methoxy-3- buten-2-one. The nature and formation yields of the reaction products are consistent with (and supportive of) the reaction mechanism: O3 + R1R2C=CR3X (R1COR2 + R3C(X)OO) + (1 - )(R3COX + R1C(R2)OO), where R1, R2 and R3 = H or alkyl, X is the oxygen-containing substituent, R1COR2 and R3COX are the primary products and R1C(R2)OO and R3C(X)OO are the carbonyl oxide biradicals. The variations of the coefficient , which ranges from 0.25 to 0.61, are discussed in terms of the number and nature of alkyl and oxygen-containing substituents. Subsequent reactions of the alkyl-substituted biradicals R1C(R2)OO and of the biradicals R3C(X)OO that bear the oxygen-containing substituent are discussed. For the biradical CH3CHOO, the ratio ka/kb for the competing pathways of rearrangement to acetic acid (CH3CHOO CH3C(O)OH, reaction (a) and formation of an unsaturated hydroperoxide (CH3CHOO CH2=CH(OOH), reaction (b) is <0.25 for ethyl 1-propenyl ether and <0.27 for 4-hexen-3-one. Concentrations measured in co- located samples, one downstream of a water impinger and the other without water impinger, show the uptake in water impingers to be high (from 83.2 to >99.9%) and comparable to that for formaldehyde (98.4%) for formic acetic anhydride and for difunctional oxygenated compounds. Uptake in water impingers was lower (19–78%) for monofunctional aldehydes and ketones.     

Methodological Development of the Conditional Sampling Method. Part I: Sensitivity to Statistical and Technical Characteristics

The relaxed eddy accumulation (REA), method based on the conditional sampling concept, has received increasing attention over the past few years as it can be used to measure surface fluxes of a wide variety of trace gases for which fast response analysers are not available. In the REA method, a turbulent flux is simply expressed as the product of the standard deviation of vertical wind velocity, the difference between mean scalar concentration in the updrafts and downdrafts and an empirical coefficient, (about 0.63 as based on simulations with a Gaussian distribution, and 0.58 as derived from experimental data). A simulation technique is developed here to evaluate the performance of a ground-based REA system. This analysis uses generated series whose internal structure can be controlled to a large extent. They are stationary and their characteristics are similar to those of physical turbulence. In a first step the influence of some statistical characteristics of vertical velocity and scalar concentration series is investigated. The effect of the third- and fourth-order moments can explain to some degree the difference between calculated and measured values. The impact of a threshold on the vertical velocity is then considered, and its effect on is quantified. The influence of the time lag between and the effective scalar sampling, and the consequences of lowpass filtering of the signal are also investigated. The simulation technique presented in this study can be used to develop elaborate algorithms for near real-time conditional sampling, based on the statistical characteristics of the previous sample.     

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.     

Land use and local climate: A case study near Santa Cruz, Bolivia

Summary The Tierras Bajas regions of eastern Santa Cruz, Bolivia have undergone among the most rapid rates of concentrated deforestation during the 1980s and 1990s. We investigate the sensitivity of local climate to these land cover changes as observed from Landsat images acquired between 1975 and 1999. The Simple Biosphere model (SiB2) is used to assess the effects of both morphological and physiological changes in vegetation and the implications for fluxes of water, energy and carbon between the vegetation and the atmosphere during the rainy season.Conversion from tropical forest to cropland implicates morphological changes in vegetation as the primary drivers for a daily maximum warming of about 2°C and a slight nighttime cooling, suggesting that clearing of tropical forests for agricultural use may increase the diurnal temperature range, mainly by increasing the maximum temperature. On the other hand, the conversion of wooded grassland to cropland resulted in a similar daily warming and drying but exclusively due to vegetation physiological activity.The area-averaged monthly mean response for each conversion type resulted in a warming of about 0.6°C for the conversion of broadleaf evergreen and 1.2°C for conversion of wooded grassland. These temperature differences represent an augmentation in the local heat source associated with a reduction in evapotranspiration due to land cover conversion and do not reflect variations forced by changes in atmospheric circulation.When averaged over the entire domain, the effect of landscape conversion results in a reduction of the latent heat flux and an increase in sensible heat flux, producing a large-scale apparent heat source of 0.5°C during January. This warming is in line with an increasing trend observed in monthly mean temperature in Santa Cruz, Bolivia during the same period.     

Ab initio study on carbon Kinetic Isotope Effect (KIE) in the reaction of CH4+Cl•

Recent studies suggest that the destruction of methane by Cl in the marine boundary layer could be accounted for as another major sink besides the methane destruction by OH. High level ab initio molecular orbital calculations have been carried out to study the CH₄+Cl reaction, the carbon Kinetic Isotope Effect (KIE) is calculated using Conventional Transition-State Theory (CTST) plus Wigner and Eckart semiclassical tunneling corrections. The calculated KIE is around 1.026 at 300 K and has a small temperature variation. This is by far the largest KIE among different processes involving atmospheric methane destruction (e.g., OH, soil). A calculated mass balance of atmospheric methane including the KIE for the CH₄+Cl reaction is found to favor those methane budgets with enhanced biological methane sources, which have relatively lighter carbon isotope composition.     

Occurrence of roll circulations in a shallow boundary layer

Meteorological measurements taken at the Näsudden wind turbine site during slightly unstable conditions have been analyzed. The height of the convective boundary layer (CBL) was rather low, varying between 60 and 300 m. Turbulence statistics near the ground followed Monin-Obukhov similarity, whereas the remaining part of the boundary layer can be regarded as a near neutral upper layer. In 55% of the runs, horizontal roll vortices were found. Those were the most unstable runs, with -z _i/L > 5. Spectra and co-spectra are used to identify the structures. Three roll indicators were identified: (i) a low frequency peak in the spectrum of the lateral component at low level; (ii) a corresponding increase in the vertical component at mid-CBL; (iii) a positive covariance {ovvw} together with positive wind shear in the lateral direction (V/z) in the CBL. By applying these indicators, it is possible to show that horizontal roll circulations are likely to be a common phenomenon over the Baltic during late summer and early winter.     

Rainwater composition over a rural area with special emphasis on the size distribution of insoluble particulate matter

The rainwater composition in the vicinity of Mainz, FRG, has been investigated with special emphasis on insoluble constituents. The number size distribution was determined in the range from 0.1 m up to 100 m radius. For particles with r>0.5 m radius the shape of the size distribution of insoluble particles in rain follows the shape of the average urban and rural aerosol. In this particular size range no major size selective removal processes could be seen. For r<0.5 m the number size distribution tends to flatten compared to the average aerosol. This might be the indication of a size selective removal process (Greenfield Gap).     

Size-Resolved Characterisation of Soluble Ions in the Particles in the Tropospheric Plume of Masaya Volcano, Nicaragua: Origins and Plume Processing

We present the first application of a multi-stage impactor to study volcanic particle emissions to the troposphere from Masaya volcano, Nicaragua. Concentrations of soluble SO₄ ^2–,Cl^–, F^–, NO₃ ^–, K⁺, Na⁺,NH₄ ⁺, Ca²⁺ and Mg²⁺ were determined in 11 size bins from 0.07 m to >25.5 m. The near-source size distributions showed major modes at 0.5m (SO₄ ^2–, H⁺,NH₄ ⁺); 0.2 m and 5.0 m (Cl^–) and 2.0–5.0 m(F^–). K⁺ and Na⁺ mirrored the SO₄ ^2– size-resolvedconcentrations closely, suggesting that these were transported primarily asK₂SO₄ and Na₂SO₄ in acidic solution, while Mg²⁺ andCa²⁺ presented modes in both <1 m and >1 m particles. Changes in relative humidity were studied by comparing daytime (transparent plume) and night-time (condensed plume) results. Enhanced particle growth rates were observed in the night-time plume as well as preferential scavenging of soluble gases, such as HCl, by condensed water. Neutralisation of the acidic aerosol by background ammonia was observed at the crater rim and to a greater extent approximately 15 km downwind of the active crater. We report measurements of re-suspended near-source volcanic dust, which may form a component of the plume downwind. Elevated levels ofSO₄ ^2–, Cl^–, F^–,H⁺, Na⁺, K⁺ and Mg²⁺ were observed around the 10 m particle diameter in this dust. The volcanic SO₄ ^2– flux leaving the craterwas 0.07 kg s^–1.     

Winter storms in Switzerland North of the Alps 1864/1865–1993/1994

Summary In the framework of the Swiss National Research Program 31 Climate changes and natural disasters the question was brought up whether a global warming of the atmosphere would have an influence on the frequency and/or intensity of the extratropical storms of the Swiss winter season. In order to investigate a possible trend, time series of days with a minimum wind speed estimate or measurement equivalent to Beaufort 7, 8 and 9 were established. The longest being a record of the mesonet station Zürich from the period 1864 until 1993 (130 years). Slightly shorter time series for three additional stations in Northern Switzerland were compiled to control the behavior of the longest record and to verify the observed temporal trend. From the location of the four investigated wind records the observational domain was restricted to the part of Switzerland north of the Alps whereas for further meteorological considerations the whole North-Atlantic-European area was included.A negative regional trend in the number of storm days has been observed during the last century. In particular, the period before 1940 has to be interpreted as windier than the following decades. The duration of a storm event also decreased on average. In spite of an increase in cyclonic westwind situations since about 1960 over Europe, Switzerland was hit by fewer storms during the same period. One explanation could be that the whole westwind belt has moved slightly further north where a deepening of the cyclones was observed in recent times. Switzerland is usually situated at the southernmost edge of the particular storm fields and is therefore less influenced by strong gales. Rare exceptions are the cases when a secondary depression directly hits Central Europe, e.g. as happened in February 1990 (storm Vivian).With 11 Figures     

A Second-Order Closure for Neutrally Stratified Vegetative Canopy Flows

An existing second-order closure model is modified to include the effects on mean and turbulent motions of form and viscous drag in vegetative canopies. The additional physical mechanisms represented by the closure are viscous and pressure drag on canopy elements, their role in momentum absorption, in the creation of fine scale turbulent eddies and in enhancing the total viscous dissipation in the canopy airspace. Viscous dissipation is split into a standard 'isotropic contribution associated with the spectral eddy cascade and a foliage contribution associated with work against pressure and viscous drag on the foliage. Changes in the turbulent time scale that result from these mechanisms are included in the standard parameterisations of third moments and of the eddy cascade contribution to dissipation. The model is tested against a wind- tunnel 'wheat canopy, a corn canopy and a eucalypt canopy, a height range from 50 mm to 12.6 m. Model results show that the parameterisations of foliage interaction used in the closure are sufficiently robust to reproduce second-moment profiles within and above vegetative canopies to a high degree of accuracy without resorting to 'tuning of the model constants. The model also shows the natural emergence of two length scales, one associated with the familiar eddy cascade isotropic contribution to total dissipation and the other associated with the length scales of the canopy elements.