Characteristics of the ozone decline in the northern polar and middle latitudes during the winter-spring

Summary The total ozone decline during the past twenty years, especially strong during the winter-spring season poleward from 50° N, is well established with known average trends of 5–7% per decade. This study presents a number of additional characteristics such as ozone-mass deficiency (O₃MD) from the pre- 1976 base average, and areal extent with negative deviations greater than2 and3. Gridded satellite data combined with ground-based total ozone maps, permit calculations of daily and regional ozone deficiencies from the anthropogenically undisturbed average ozone levels of the 1960s and early 1970s. Then the quantity of the O₃MD and the changes in surface area, with deficiencies larger than-10 and-15% are integrated for the 1 January to 15 April period for each of the last 20 years, and compared. In addition, the polar vortex extent during the last 10 years is determined using the PV at 475°K. The quantity of the O₃MD within the sunlit part of the vortex is shown to contribute from15 to 35% of the overall ozone deficiency within the-10% contours over the area 35–90°N. The ozone deficiency, integrated for the first 105 days of each year, has increased dramatically from 2,800Mt in the early 1980s to7,800Mt in the 1990s, exceeded 12,000Mt in the winter-springs of 1993 and 1995. The latter quantity is comparable with the average O₃MD over the same Southern latitudes in the last ten austral springs. During the 1990s over the 35–90° latitudes the average ozone deficiency in the Southern hemisphere belt is less than over the Northern hemisphere belt by40%. It is known that the main ozone decline is observed in the lower stratosphere and the ozone loss over the Arctic is very sensitive to decreasing stratospheric temperatures; negative 50hPa monthly anomalies greater than 4°C have occurred during 7 of the springs in the last decade, thus possibly facilitating doubling the area with negative ozone deviations greater than-10% in the 1990s to5,000.10⁶km² and nearly tripling the O₃MD as stated above. The changes in total eddy heat fluxes as a proxy indicator of the long wave perturbations are positively correlated with the ozone deficiency in the 45–75°N. The strong anticorrelation between the ozone deficiency in the region>55° N. versus the 35–50° N belt is discussed in relation to possible transport of air masses with low ozone from the sub-tropics, which in some years are the dominant reason for the observed ozone deficiency.With 11 Figures     

Simultaneous Measurements of Black Carbon, PM10, Ozone and NOx Variability at a Locally Polluted Island in the Southern Tropics

This paper shows a comparative study of particle and surface ozone concentration measurements undertaken simultaneously at two distinct semi-urban locations distant by 4 km at Saint-Denis, the main city of La Réunion island (21.5° S, 55.5° E) during austral autumn (May 2000). Black carbon (BC) particles measured at La Réunion University, the first site situated in the suburbs of Saint-Denis, show straight-forward anti-correlation with ozone, especially during pollution peaks ( 650 ng/m³ and 15 ppbv, for BC and ozone respectively) and at night-time (90 ng/m³ and 18.5 ppbv, for BC and ozone respectively). NO_x (NO and NO₂) and PM₁₀ particles were also measured in parallel with ozone at Lislet Geoffroy college, a second site situated closer to the city centre. NO_x and PM₁₀ particles are anti-correlated with ozone, with noticeable ozone destruction during peak hours (mean 6 and 9 ppbv at 7 a.m. and 8 p.m. respectively) when NO_x and PM₁₀ concentrations exhibit maximum values. We observe a net daytime ozone creation (19 ppbv, O₃ +4.5 ppbv), following both photochemical and dynamical processes. At night-time however, ozone recovers (mean 11 ppbv) when anthropogenic activities are lower ([BC] 100 ng/m³). BC and PM₁₀ concentration variation obtained during an experiment at the second site shows that the main origin of particles is anthropogenic emission (vehicles), which in turn influences directly ozone variability. Saint-Denis BC and ozone concentrations are also compared to measurements obtained during early autumn (March 2000) at Sainte-Rose (third site), a quite remote oceanic location. Contrarily to Saint-Denis observations, a net daytime ozone loss (14.5 ppbv at 4 p.m.) is noticed at Sainte-Rose while ozone recovers (17 ppbv) at night-time, with however a lower amplitude than at Saint-Denis. Preliminary results presented here are handful data sets for modelling and which may contribute to a better comprehension of ozone variability in relatively polluted areas.     

Photochemistry in the Arctic Free Troposphere: Ozone Budget and Its Dependence on Nitrogen Oxides and the Production Rate of Free Radicals

Local ozone production and loss rates for the arctic free troposphere (58–85° N, 1–6 km, February–May) during the TroposphericOzone Production about the Spring Equinox (TOPSE) campaign were calculated using a constrained photochemical box model. Estimates were made to assess the importance of local photochemical ozone production relative to transport in accounting for the springtime maximum in arctic free tropospheric ozone. Ozone production and loss rates from our diel steady-state box model constrained by median observations were first compared to two point box models, one run to instantaneous steady-state and the other run to diel steady-state. A consistent picture of local ozone photochemistry was derived by all three box models suggesting that differences between the approaches were not critical. Our model-derived ozone production rates increased by a factor of 28 in the 1–3 km layer and a factor of 7 in the 3–6 kmlayer between February and May. The arctic ozone budget required net import of ozone into the arctic free troposphere throughout the campaign; however, the transport term exceeded the photochemical production only in the lower free troposphere (1–3 km) between February and March. Gross ozone production rates were calculated to increase linearly with NO_x mixing ratiosup to 300 pptv in February and for NO_x mixing ratios up to 500 pptv in May. These NO_x limits are an order of magnitude higher thanmedian NO_x levels observed, illustrating the strong dependence ofgross ozone production rates on NO_x mixing ratios for the majority of theobservations. The threshold NO_x mixing ratio needed for netpositive ozone production was also calculated to increase from NO_x 10pptv in February to 25 pptv in May, suggesting that the NO_x levels needed to sustain net ozone production are lower in winter than spring. This lower NO_x threshold explains how wintertime photochemical ozone production can impact the build-up of ozone over winter and early spring. There is also an altitude dependence as the threshold NO_x neededto produce net ozone shifts to higher values at lower altitudes. This partly explains the calculation of net ozone destruction for the 1–3 km layerand net ozone production for the 3–6 km layer throughout the campaign.     

Formation of Organic Aerosols from the Oxidation of Biogenic Hydrocarbons

Measurements of aerosol formation during thephotooxidation of -pinene, -pinene,d-3-carene, d-limonene, ocimene, linalool, terpinene-4-ol, andtrans-caryophyllene were conducted in anoutdoor smog chamber. Daylight experiments in thepresence of and dark experiments withelevated ozone concentrations were performed. Theevolution of the aerosol was simulated by theapplication of a gas/particle absorption model inconnection with a chemical reaction mechanism. Thefractional aerosol yield is shown to be a function ofthe organic aerosol mass concentration andtemperature. Ozone and, for selected hydrocarbons, theNO₃ reaction of the compounds were found torepresent efficient routes to the formation ofcondensable products. For initial hydrocarbon mixingratios of about 100 ppb, the fractional aerosol yieldsfrom daylight runs have been estimated to be 5%for open-chain hydrocarbons, such as ocimene andlinalool, 5–25% for monounsaturated cyclicmonoterpenes, such as -pinene, d-3-carene, orterpinene-4-ol, and 40% for a cyclic monoterpenewith two double bonds like d-limonene. For the onlysesquiterpene investigated, trans-caryophyllene, afractional aerosol yield of close to 100% wasobserved. The majority of the compounds studied showedan even higher aerosol yield during dark experimentsin the presence of ozone.     

Arctic hazes in summer over Greenland and the North American Arctic. III: A contribution from the natural burning of carbonaceous materials and pyrites

Airborne measurements of the emissions from natural fires, fueled by pyrites and organic materials, at the Smoking Hills in the Northwest Territories, show that they are a regionally significant source of SO₂ (0.3 kg s^–1 or 10⁴ T yr^–1) and particles (0.3 kg s^–1). It appears likely that the Smoking Hills are a source for some of the dense, lower-level, haze layers that occur in the North American Arctic.     

Application of a “Big-Tree” model to regional climate modeling: a sensitivity study

Summary ¶In order to better understand land-atmosphere interactions and increase the predictability of climate models, it is important to investigate the role of forest representation in climate modeling. Corresponding to the big-leaf model commonly employed in land surface schemes to represent the effects of a forest, a so called big-tree model, which uses multi-layer vegetation to represent the vertical canopy heterogeneity, was introduced and incorporated into the National Center for Atmospheric Research (NCAR) regional climate model RegCM2, to make the vegetation model more physically based. Using this augmented RegCM2 and station data for China during 1991 Meiyu season, we performed 10 experiments to investigate the effects of the application of the big-tree model on the summer monsoon climate.With the big-tree model incorporated into the regional climate model, some climate characteristics, e.g. the 3-month-mean surface temperature, circulation, and precipitation, are significantly and systematically changed over the model domain, and the change of the characteristics differs depending on the area. Due to the better representation of the shading effect in the big-tree model, the temperature of the lower layer atmosphere above the plant canopy is increased, which further influences the 850hPa temperature. In addition, there are significant decreases in the mean latent heat fluxes (within 20–30W/m²) in the three areas of the model domain.The application of the big-tree model influences not only the simulated climate of the forested area, but also that of the whole model domain, and its impact is greater on the lower atmosphere than on the upper atmosphere. The simulated rainfall and surface temperature deviate from the originally simulated result and are (or seem to be) closer to the observations, which implies that an appropriate representation of the big-tree model may improve the simulation of the summer monsoon climate.We also find that the simulated climate is sensitive to some big-tree parameter values and schemes, such as the shape, height, zero-plane displacement height and mixing-length scheme. The simulated local/grid differences may be very large although the simulated areal-average differences may be much lower. The area-average differences in the monthly-mean surface temperature and heat fluxes can amount to 0.5°C and 4W/m², respectively, which correspond to maximum local/grid differences of 3.0°C and 40W/m² respectively. It seems that the simulated climate is most sensitive to the parameter of the zero-plane displacement among the parameters studied.     

Three million years of monsoon variability over the northern Sahara

We present a 3 million year record of aeolian dust supply into the eastern Mediterranean Sea, based on hematite contents derived from magnetic properties of sediments from Ocean Drilling Program Site 967. Our record has an average temporal resolution of 400 years. Geochemical data validate this record of hematite content as a proxy for the supply of aeolian dust from the Sahara. We deduce that the aeolian hematite in eastern Mediterranean sediments derives from the eastern Algerian, Libyan, and western Egyptian lowlands located north of the central Saharan watershed (21°N). In corroboration of earlier work, we relate dust flux minima to penetration of the African summer monsoon front to the north of the central Saharan watershed. This would have enhanced soil humidity and vegetation cover in the source regions, in agreement with results from green Sahara climate models. Our results indicate that this northward monsoon penetration recurred during insolation maxima throughout the last 3 million years. As would be expected, this orbital precession-scale mechanism is modulated on both short (100-kyr) and long (400-kyr) eccentricity time scales. We also observe a strong expression of the 41-kyr (obliquity) cycle, which we discuss in terms of high- and low-latitude mechanisms that involve Southern Hemisphere meridional temperature contrasts and shifts in the latitudes of the tropics, respectively. We also observe a marked increase in sub-Milankovitch variability around the mid-Pleistocene transition (0.95 Ma), which suggests a link between millennial-scale climate variability, including monsoon dynamics, and the size of northern hemisphere ice sheets.     

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.     

Aerosols in Alaskan air masses

Results from measurements of the composition and size distribution of aerosol particles advected into central Alaska are reported. It is argued that the aerosol predominant in number, but not necessarily in mass, consists of submicron droplets of sulfuric acid. The major aerosol by mass in arctic air is a removal-resistant accumulation mode (radius 0.3 m) probably to large extent originating from pollution sources 10³ km upstream (mostly in central Eurasia) from the site in Alaska. The accumulation mode aerosol disappears when arctic air masses are replaced with relatively warmer air masses flowing in from the northern Pacific. The latter air mass systems have been strongly scavenged by clouds and precipitation associated with the Aleutian low pressure system and with forced orographic uplifting over the Alaska Mountain Range; nevertheless the Pacific air masses contain substantial (i.e., 500–1000 cm^-3) quantities of small (several hundredths of a micron in radius) particles. Arctic-derived air masses are enriched in large (i.e, 0.3 ) particles compared to Pacific Marine air masses, whereas the opposite trend is found for smaller, Aitken, particles. The smaller particles are found in greatest abundance in warmer air mass systems, presumably because of the relatively brief time since such air masses were last exposed to sunlight with attendant production of small particles from the gas phase.     

Gas-Particle Partitioning of Nitric Acid Modulated by Alkaline Aerosol

The role of alkaline mineral aerosol in controlling HNO₃ partitioning between gas and aerosol phases is explored using a comprehensive, process oriented three-dimensional model. Simulation results for March 1994, a period from the PEM West B experiment, are presented. It is found that in the dust impacted regions of the boundary layer and free troposphere, more than 50% of HNO₃ ispartitioned onto dust particles; while 1050% of HNO₃ in the boundarylayer and 10 30% of HNO₃ in the free troposphere is partitionedonto sea-salt particles. This higher capacity of mineral dust to uptake HNO₃ is due to the fact that carbonate in the dust particles is more volatile (thus easily replaced by nitrate) than chloride in the sea-salt particles. When this process of nitric acid partitioning onto alkaline particles is included in the analysis, model predicted HNO₃-to-NO_x ratios are much closer to observed valuesthat typically range between 1 and 9.     

Relative optical mass functions for air, water vapour, ozone and nitrogen dioxide in atmospheric models presenting different latitudinal and seasonal conditions

Summary A study of the dependence features of the relative optical mass functions for air, water vapour, ozone and nitrogen dioxide on the apparent solar zenith angle was performed by calculating these optical parameters by means of the well-known computer code LOWTRAN 7 at several values of and for nine atmospheric models characterized by different latitudes and seasons. Moreover, other investigations were performed on the dependence features of (i) the relative optical air mass on the thermal characteristics of the low troposphere, (ii) the relative optical water vapour mass on the vertical distribution characteristics of absolute humidity in the troposphere, and (iii) the relative optical mass function for ozone and nitrogen dioxide on the shape characteristics of the vertical profiles of the two gaseous concentrations and the concentration peak altitudes. The results are compared with the values given by the two simple formulas proposed by Kasten (1966) for air and water vapour and the formulas defined by Young (1969) and Staehelin et al. (1995) for ozone and nitrogen dioxide. From this comparison, a wide set of correction factors were obtained which can be conveniently used in the analysis of multispectral sun-radiometric measurements for calculating, with a very high precision, the values of the four optical mass functions at all the angles in the 0° to 87° range, corresponding to the various latitudinal and seasonal conditions described by the nine atmospheric models.With 9 Figures     

High Acetone Concentrations throughout the 0–12 km Altitude Range over the Tropical Rainforest in Surinam

Airborne measurements of acetone were performed overthe tropical rainforest in Surinam(2°–7° N, 54°–58° W, 0–12 kmaltitude) during the LBA-CLAIRE campaign in March1998, using a novel proton transfer reaction massspectrometer (PTR-MS) that enables the on-linemonitoring of volatile organic compounds (VOC) with ahigher proton affinity than water. The measuredacetone volume mixing ratios ranged from 0.1 nmol/molup to 8 nmol/mol with an overall average of 2.6nmol/mol and a standard deviation of 1.0 nmol/mol. Theobserved altitude profile and correlations with CO,acetonitrile, propane and wind direction are discussedwith respect to potential acetone sources. No linearcorrelation between acetone and CO mixing ratios wasobserved, at variance with results of previousmeasurement campaigns. The mean acetone/CO ratio(0.022) was substantially higher than typical valuesfound before. The abundance of acetone appears to beinfluenced, but not dominated, by biomass burning,thus suggesting large emissions of acetone and/oracetone precursors, such as possibly 2-propanol, fromliving plants or decaying litter in the rainforest.     

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.     

PV morphology of a frontal-wave development

Summary A case study is performed of a frontal-wave development on a trailing cold front in the Atlantic. The data base comprises principally the analysis and forecast fields of the global operational weather prediction model of the ECMWF, and the development itself is viewed from a potential vorticity (PV) perspective. It is shown that the ambient atmosphere contained three distinct and salient PV features: at the surface a frontal baroclinic zone; in the lower troposphere a co-aligned, moisture laden elongated band (2000 km long and 400 km wide) of enhanced PV; and at upper-levels a richly structured, southward extending PV pool. In the developments first phase a large-scale undulation of the surface frontal zone was accompanied by an in-phase movement of the upper-level anomaly. In a second phase two low-level wave features developed around 1000 km apart, and the resulting wave depressions were accompanied by a distortion of the baroclinic zone and the break-up of the low-level PV-band. In the subsequent mature phase the dominant secondary cyclone attained 500 km scale in the horizontal and acquired a coherent PV structure in the vertical.A PV-based diagnostic analysis provides evidence of both the self development of the PV features and their synergetic interplay. It also forms the basis for a comparison of the event with traditional and recent hypotheses for frontal-wave development.On the basis of the diagnosed relationship between the customarily depicted surface frontal-wave cups and the low-level PV-band, it is suggested that the segmentation of the latter provides a useful tool for monitoring and forecasting secondary developments. Also in the context of numerical weather prediction brief consideration is given to the sensivity of the frontal-wave development and structure to the spatial resolution of the associated forecast model and the specification of the initial fields.With 12 Figures     

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.     

Grid transformation for incorporating the Arctic in a global ocean model

A grid transformation is described which isolates the Arctic and North Atlantic, rotates the spherical grid to pass an equator up the Atlantic through the north pole and remaps the Coriolis parameter. Boundary condition information is exchanged along the equatorial Atlantic so that the Arctic-Atlantic model is dynamically coupled to a model of the rest of the global ocean (which remains on the geographic spherical grid). The transform produces a more regular grid over the Arctic and eliminates the need for filtering or special treatment at the pole. The transform has been implemented in the GFDL Modular Ocean Model. After testing with idealized geometry, a 300 y global integration is compared to an integration using the geographic spherical grid and Fourier filtering. Results are similar, with differences in the Arctic and western North Atlantic regions leading to smaller air-sea heat flux near the Gulf Stream separation latitude for the transform case. Use of the transform also leads to a reduction in computation time.     

Tropical atmospheric stability and wind structures as inferred from the Indian MST radar observations

Summary The MST (Mesosphere-Stratosphere-Tropospher) Radar Facility at Gadanki (13.47° N, 79.18° E), near Tirupati, Andhra Pradesh, India has been operated over seven diurnal cycles—three in November 1994, one in September 1995 and three in January–February 1996 with an objective to study the wind and stability characteristics in the troposphere and lower-stratosphere. The radar-measured height profiles of both zonal (EW) and meridional (NS) wind components and near-simultaneous radiosonde measurements from Madras (13.04° N, 80.7° E) and Bangalore (12.85° N, 77.58° E), the two stations close to either side of the radar site, have been compared and they are found to be in gross agreement within the limitations of the sensing techniques.The results of the study also indicated multiple stable and turbulent structures/stratification throughout the height region from about 4 to 30 km. It is noticed that the stable layers are well marked around the altitudes 4 km, 12 km and the tropopause while the turbulent layers exist a few kilometers below the tropopause. These stable and turbulent layer structures showed good correspondence with the radar-measured wind gradients and also with the radiosonde-derived temperature and wind distributions over Madras. The maximum positive gradient in the signal-tonoise ratio (SNR) which corresponds to radar tropopause is found to coincide with the greater potential temperature gradient and smaller wind gradient. The time evolution of atmospheric stability structure, derived from the SNR, spectral width and vertical wind revealed a diffused tropopause or tropopause weakening which is found to be associated with broader spectral width and larger gradients of winds. This feature is considered to be due either to the instability associated with large vertical gradients in horizontal winds (dynamical instability) or to the instability generated by the convection (convective instability).With 6 Figures     

Radiative Heat Transfer and Hydrostatic Stability in Nocturnal Fog

We have performed a one-dimensional and transient radiative heat transfer analysis in order to investigate interaction between atmospheric radiation and convective instability within a nocturnal fog. The radiation element method using the Ray Emission Model (REM²), which is a generalized numerical method, in conjunction with a line-by-line (LBL) method, is employed to attain high spectral resolution calculations for anisotropically scattering fog. The results show that the convective instability has a strong dependence on radiative properties of the fog. For the condition of a 20-m droplet diameter and liquid water content of 0.1 × 10^–3 kg m^–3;, the temperature profile within the fog becomes S shaped, and a convective instability layer forms in the middle or lower level of the fog. However, for the same water content and a 40-m diameter droplet, no strong convective instability layer forms, whereas for a 10-m diameter droplet a strong convective instability is observed.     

Numerical Investigation of the Influence of Mineral Dust on the Tropospheric Chemistry of East Asia

An investigation of the influence of mineral dust ontrace gas cycles in the troposphere is carried out inthis study. A 3D regional scale atmospheric chemistrymodel (STEM-III) which includes aerosol processes isused for the numerical simulations for May 1987.Heterogeneous interactions between gaseous species(SO₂, N₂O₅, HNO₃, HO₂andH₂O₂) and the dust particles are considered.Emissions of dust behind convective cold fronts aremodeled. The transport and distribution of mineraldust predicted from the model is compared withsatellite measurements (aerosol index from TOMS). Themodel is shown to capture the synoptic variability inthe observed aerosol index. Calculations show twomajor dust events in May 1987, during which thedust levels close to the source reach more than500 g/m³. The transport of dust is mostlyrestricted towards the north, with the net continentaloutflow of 6 Tg for the entire month. Results showthat the presence of mineral aerosol can greatlyimpact sulfate and nitrate distributions. Averagedover the month of May, the presence of dust isestimated to increase particulate sulfate and nitratelevels in east Asia by 40%. Furthermore, the sulfateand nitrate on the dust particles are predicted to beassociated with the coarse mode (3–5 m particlediameter), consistent with observations over Japan.The influence of mineral dust on the photochemicaloxidant cycle is also investigated. For the entiremonth, a5–10% decrease in boundary layer ozone ispredicted by the model closer to regions of higherdust levels. The ratio of nitric acid to NO_x overmarine regions is reduced by a factor between 1 and 2in the boundary layer to more than 2 in the freetroposphere as a result of aerosol processes.     

On the turbulence structure in the stable boundary layer over the Greenland ice sheet

Turbulence measurements from a 30 m tower in the stably stratifiedboundary layer over the Greenland ice sheet are analyzed. The observationsinclude profile and eddy-correlation measurements at various levels. Atfirst, the analysis of the turbulence data from the lowest level (2 m aboveground) shows that the linear form of the non-dimensional wind profile(m) is in good agreement with the observations for z/L <0.4, whereL represents the Obukhov length. A linear regression yieldsm=1+5.8z/L. The non-dimensional temperature profile (h) at the2m level shows no tendency to increase with increasing stability. The datafrom the upper levels of the tower are analyzed in terms of both localscaling and surface-layer scaling. The m and the h values show atendency to level off at large stability (z/>0.4) where represents the local Obukhov length. Hence, the linear form of the functions is no longer appropriate under such conditions. The bestcorrespondence to the data can be achieved when using the expression ofBeljaars and Holtslag for m and h. The vertical profiles of theturbulent fluxes, the wind velocity variances and temperature variance arealso determined. The momentum flux profile and the profiles of wind speedvariances are in general agreement with other observations if a welldeveloped low-level wind maximum occurs, and the height of this maximum isused as a height scale.