Small-particle concentration fluctuations at a coastal site

Aerosol size spectra (d=10 nm–10 μm) were measured with an electrical aerosol spectrometer (EAS) at Mace Head on the west coast of Ireland. Several small aerosol particle (diameter 10–32 nm) concentration bursts were observed during the measurement period. Relationships between the events, air mass trajectories, tide height, and meteorological parameters are examined. Series of bursts were observed when a spectral transformation due to subsequent particle growth from 10 to 56–100 nm can be identified in an Eulerian experiment. Particle growth rates of between 1 and 3 nm/h were determined. These bursts appear in cold and comparatively clean arctic or polar air masses with temperature and relative humidity fluctuations, and do not correlate with low tide in some cases. These episodes, similar to those frequently found in the continental boundary layer, are thought to occur over a wide area and, for clear detection, require stable airflow for a few days. Elevated small-particle concentration events are more common during low tide or shortly after, and are typically associated with low wind speeds. Here, the increased shore exposure during low tide is thought to influence the nucleation and the subsequent growth of these aerosol particles. The occurrences of the bursts are found to depend on local wind direction. The highest d=10–32 nm particle concentrations appeared for wind sectors furthest from the tidal regions when the wind direction was 150–160°(south-easterly). Most of the events occurred during daytime when solar irradiation is most intense.     

Statistical properties of optical refractive index fluctuations in the marine boundary layer

The optical refractive index fluctuation has been determined from measurements of turbulent temperature and humidity fluctuations in the atmospheric surface layer over the ocean. Probability density, spectral density and even- and odd-order structure functions of the refractive index fluctuation are presented. The spectral density exhibits a significant -5/3 inertial subrange as a result of the existence of a -5/3 subrange in the spectra of temperature and humidity fluctuations and in the temperature-humidity co-spectrum. The behaviour in the inertial subrange of fourth- and sixth-order structure functions of the refractive index is in reasonable agreement with that predicted by the analysis of Antonia and Van Atta (1975, 1978). The third-order structure functions of the refractive index exhibit an approximately linear dependence on separation in the inertial subrange, in agreement with a ramp model for the large coherent structure of the motion.     

Seasonal characteristics of tropical marine boundary layer air measured at the Cape Verde Atmospheric Observatory

Observations of the tropical atmosphere are fundamental to the understanding of global changes in air quality, atmospheric oxidation capacity and climate, yet the tropics are under-populated with long-term measurements. The first three years (October 2006–September 2009) of meteorological, trace gas and particulate data from the global WMO/Global Atmospheric Watch (GAW) Cape Verde Atmospheric Observatory Humberto Duarte Fonseca (CVAO; 16° 51′ N, 24° 52′ W) are presented, along with a characterisation of the origin and pathways of air masses arriving at the station using the NAME dispersion model and simulations of dust deposition using the COSMO-MUSCAT dust model. The observations show a strong influence from Saharan dust in winter with a maximum in super-micron aerosol and particulate iron and aluminium. The dust model results match the magnitude and daily variations of dust events, but in the region of the CVAO underestimate the measured aerosol optical thickness (AOT) because of contributions from other aerosol. The NAME model also captured the dust events, giving confidence in its ability to correctly identify air mass origins and pathways in this region. Dissolution experiments on collected dust samples showed a strong correlation between soluble Fe and Al and measured solubilities were lower at high atmospheric dust concentrations. Fine mode aerosol at the CVAO contains a significant fraction of non-sea salt components including dicarboxylic acids, methanesulfonic acid and aliphatic amines, all believed to be of oceanic origin. A marine influence is also apparent in the year-round presence of iodine and bromine monoxide (IO and BrO), with IO suggested to be confined mainly to the surface few hundred metres but BrO well mixed in the boundary layer. Enhanced CO₂ and CH₄ and depleted oxygen concentrations are markers for air-sea exchange over the nearby northwest African coastal upwelling area. Long-range transport results in generally higher levels of O₃ and anthropogenic non-methane hydrocarbons (NMHC) in air originating from North America. Ozone/CO ratios were highest (up to 0.42) in relatively fresh European air masses. In air heavily influenced by Saharan dust the O₃/CO ratio was as low as 0.13, possibly indicating O₃ uptake to dust. Nitrogen oxides (NO_x and NO_y) show generally higher concentrations in winter when air mass origins are predominantly from Africa. High photochemical activity at the site is shown by maximum spring/summer concentrations of OH and HO₂ of 9?×?10⁶ molecule cm^?3 and 6?×?10⁸ molecule cm^?3, respectively. After the primary photolysis source, the most important controls on the HO_x budget in this region are IO and BrO chemistry, the abundance of HCHO, and uptake of HO_x to aerosol.     

Properties of pressure fluctuations in an atmospheric boundary layer

From experimental data it is shown that there is a relationship between measured wind speed and associated micropressure levels. It is also shown that turbulent eddies associated with the wind vanish within distances of five to six times their size, and that these eddies exhibit normal dispersion. These results confirm, at the atmospheric scales, results previously observed only in model experiments.     

A complete dynamical ozone budget measured in the tropical marine boundary layer during PASE

The Pacific Atmospheric Sulfur Experiment (PASE) was a field mission that took place aboard the NCAR C-130 airborne laboratory over the equatorial Pacific Ocean near Christmas Island (Kirimati, Republic of Kiribati) during August?CSeptember, 2007. Eddy covariance measurements of the ozone fluxes at various altitudes above the ocean surface, along with simultaneous mapping of the horizontal gradients provided a unique opportunity to observe all of the dynamical components of the ozone budget in this remote marine environment. The results of six daytime and two sunrise flights indicate that vertical transport into the marine boundary layer from above and horizontal advection by the tradewinds are both important source terms, while photochemical destruction consisting of 82% photolysis (leading to OH production), 11% reaction with HO₂, and 7% reaction with OH provides the main sink. The overall photochemical lifetime of ozone in the marine boundary layer was found to be 6.5 days. Ocean uptake of ozone was observed to be fairly slow (mean deposition velocity of 0.024?±?0.014 cm s^?1) accounting for a diurnally averaged loss rate that was ??30% as large as the net photochemical destruction. From the measurement of deposition velocity an ozone reactivity of ??50 s^?1 in seawater is inferred. Due to the unprecedented measurement accuracy of the dynamical budget terms, unobserved photochemistry was able to be deduced, leading to the conclusion that 3.9?±?3.0 ppt (parts per trillion by volume) of NO is present on average in the daytime tropical marine boundary layer, broadly consistent with several previous studies in similar environments. It is estimated, however, that each ppt of BrO hypothetically present would counter each ppt of NO above the requisite 3.9 ppt needed for budget closure. The long-term budget of ozone is further analyzed in the buffer layer, between the boundary layer and free troposphere, and used to derive an entrainment velocity across the trade wind inversion of 0.51 ± 0.38 cm s^?1.     

Similarity functions in the tropical marine boundary layer

Mean profiles of virtual potential temperature, specific humidity, and the wind velocity components are obtained from aircraft data taken during the NORPAX trans-equatorial shuttle over the Pacific Ocean. The resulting parameters are used to calculate the similarity functions A,B,C, and D. These agree well with similarity functions obtained for the tropical Atlantic Ocean using GATE data (Fitzjarrald and Garstang, 1981). The similarity function A for wind speed over the tropical oceans is in good agreement with values obtained over land at higher latitudes. The tropical temperature and humidity functions, C and D, are lower than those obtained at higher latitudes, becoming negative as h/(-L) → 0.     

Factors influencing the marine boundary layer during a cold-air outbreak

The model for the cloud-topped marine boundary layer during a cold air outbreak developed by Stage and Businger (1981a) is used in conjunction with a test profile based on a fall outbreak episode over Lake Ontario to study factors influencing marine boundary-layer evolution. Sensitivity tests are done which show changes in layer evolution resulting from variation of wind speed, radiative sky temperature, water surface temperature, humidity of the shoreline sounding and divergence. The behavior of the layer in the presence of a region of cold-water upwelling near the shore is also investigated. It is found that the main effect of the upwelling region is to delay modification of the boundary-layer air.     

A study of temperature fluctuations in the atmospheric boundary layer

The spectral density of temperature fluctuations in the boundary layer has been studied in the range 0.2 to 2 Hz. It is shown that the temperature spectrum is strongly variable from one minute to the next and that the spectral slope tends to increase with the standard deviation of temperature fluctuations and with the stability of the medium. It is shown that C _T ² values computed from short time series (30 s) tend to be smaller than the C _T ² values computed from several minutes of record.Formerly at Laboratoire de Météorologie Dynamique du C.N.R.S. (Paris).     

Correlated humidity and temperature measurements in the urban atmospheric boundary layer

Summary To investigate the effect of atmospheric turbulence on microwave communication links, temperature and water vapor pressure have been measured and radio refractivity has been computed, during different meteorological conditions, in the atmospheric boundary layer of an urban site. The cospectra between temperature (T) and water vapor pressure (e) have been found to be either negative over the whole range of frequencies, or the low-frequency end of the cospectrum is of opposite sign relative to higher frequency end. In both cases cospectra follow a–5/3 law in the inertial subrange, in agreement with the theoretical predictions. The coherence spectra clearly show that the temperature and humidity fluctuations are highly coherent within the inertial subrange under both convective and stable conditions. The relative contribution ofC _T ² ,C _eT andC _e ² to the real refractive index structure parameterC _n ² is examined and discussed.With 4 Figures     

Radon daughter disequilibria in the lower marine boundary layer

Radon daughters are produced as free ions, but they become attached to aerosol particles at a rate depending on the particle concentration. In the lower marine boundary layer, most of those which do not become attached plate out on the ocean surface. In this paper a simple model is used to examine the influence of several parameters on radon/radon daughter disequilibria in maritime air. The model is compared with experimental data from Cape Grim.The radon daughter to radon ratio, f, decreases from 0.86 to 0.1 as the particle concentration falls from 1000 to 10 cm^-3. Estimates of radon concentration at sea level, based on daughter measurements may therefore be in error by as much as a factor of 10 unless allowance is made for particle concentration. At 100 cm^-3, the standard deviation of the distribution of measured f values is about 30%, indicating that the particle concentration is not the only factor influencing the loss of radon daughters. The implication is that radon daughters can be used to measure radon concentrations at sea level with an accuracy of about 30%, provided the particle concentration is known.The measurements show that there is a very low proportion of unattached daughers in the air between about 30 and 165 m above sea level. According to the model, this implies that mixing of air up to about 200 m is usually rapid enough to result in plate-out of radon daughters on the ocean on a time scale of less than 100 s.     

Characterization of concentration fluctuations of a surface plume in a neutral boundary layer

We describe a new high-resolution sampling technique which can be used to measure concentration fluctuations simultaneously at several points in space. The technique has been used to measure the probability distribution function as a function of the detector location relative to a continuous and steady source. Results are compared to previous experiments and theoretical predictions. The spectra of the concentration fluctuations are analyzed and their behaviour as a function of downwind distance from the source is described.     

A note on vertical coherence of wind measured in an urban boundary layer

The coherence, γ, between levels of the horizontal components of wind velocity are examined for data obtained on a 118-m tower at Victoria Dock, an urban site in Melbourne, Australia. The coherence is analysed to determine the influence of various parameters on its variation; it is found to be strongly dependent on f=n δz/U (n frequency, δz interlevel spacing and U the mean wind speed), and to a lesser degree on thermal stability and wind component. The empirical relation γ=exp(?af) is found to be reasonable and estimates of a are given. The data conform to observations reported at other sites.     

RETRACTED ARTICLE: Validation of mean and turbulent parameters measured from the aircraft in the marine atmospheric boundary layer

The SEMAPHORE (Structure des Echanges Mer-Atmosphère, Propriétés Océaniques/ Recherche Expérimentale) experiment, which took place between 04 Oct. and 17 Nov. 1993, was conducted over the oceanic Azores current located in the Azores basin. The SST (Sea Surface Temperature) field was characterized in the SEMAPHORE area (31°–38°N; 21°–28°W) by a large meander with a SST gradient of about 1°C per 100 km. In order to study the evolution of the MABL (Marine Atmospheric Boundary Layer) over the ocean, the mean and the turbulent data were evaluated by the measurement with two aircraft and a ship in different meteorological conditions. Three cases of low pressure and three cases of high pressure are mainly presented here. For the six cases, the satellite images (NOAA) did not show any relation between the SST field and the cloud cover. At each flight level, the decrease of the SST with the altitude due to the divergence of the infrared radiation flux from the ocean is 0.25°C per 100 m. For the comparison between the two aircraft, the mean thermodynamic and dynamic parameters show a good agreement except for the temperature. The dispersion of the sensible heat flux is larger than that of the latent heat flux due to the weak sensible heat flux over the ocean both in the intercomparison between two aircraft and in the comparison between the aircraft and the ship.     

Generation and dissipation of microwave refractive-index fluctuations in the boundary layer

The index of refraction and its short-term variations have been measured on a 152-m meteorological tower at three fixed levels and on a moveable platform. Analysis of the data reveals that the time rates of production and dissipation of refractivity fluctuations are approximately in balance under a variety of meteorological conditions, and that changes in the rate of dissipation usually coincide with comparable changes in the rate of production. Under reasonably stationary conditions, terms corresponding to the rate of change and vertical diffusion of refractivity variance are found to be negligible. Power spectral densities of the variations increase when the rate of generation (and dissipation) increase, and conversely. Comparison of the results with simultaneous acoustic sounder returns provides a valuable insight into the mechanisms responsible for changes in the rates of production and dissipation.     

Measurements of peroxyacetylnitrate in the marine boundary layer over the Atlantic

The atmospheric concentration of peroxyacetylnitrate (PAN) was measured during a cruise of the R.S. Polarstern from Bremerhaven (Germany) to Rio Grande do Sul (Brazil) in September/ October 1988. The measurements were made in-situ by a combination of electron capture gaschromatography with a cryogenic preconcentration step. The theoretical lower limit of detection (3) was 0.4 ppt. The mixing ratios of PAN varied by more than three orders of magnitude from 2000 ppt in the English Channel to less than 0.4 ppt south of the Azores (38° N). South of 35° N, PAN levels were below the detection limit, except at 30–31° S off the eastern coast of South America. Here, PAN mixing ratios of 10 to 100 ppt were detected in continentally influenced air masses. Detectable levels of PAN were mostly observed in air masses of continental or high northern origin. Changes in the wind directions were usually associated with substantial changes in the PAN mixing ratios.     

Micromixing modelling of concentration fluctuations in inhomogeneous turbulence in the convective boundary layer

The micromixing technique, widely used in engineering calculations of mixing and chemical reaction, is extended to atmospheric boundary-layer flows. In particular, a model based on the interaction-by-exchange-with-the-conditional-mean (IECM) micromixing approach is formulated to calculate concentration fluctuation statistics for a line source and a point source in inhomogeneous and non-Gaussian turbulence in the convective boundary layer. The mixing time scale is parameterised as a linear function of time with the intercept value determined by the source size at small times. Good agreement with laboratory data for the intensity of concentration fluctuations is obtained with a value of 0.9 for the coefficient of the linear term in the time-scale parameterisation for a line source, and a value of 0.6 for a point source. Calculation of higher-order moments of the concentration field for a line source shows that non-Gaussian effects persist into the vertically well-mixed region. The cumulative distribution function predicted by the model for a point source agrees reasonably well with laboratory data, especially in the far field. In the limit of zero mixing time scale, the model reduces to a meandering plume model, thus enabling the concentration variance to be partitioned into meandering and relative components. The meandering component is shown to be more persistent for a point source than for a line source.     

Mean horizontal wind profiles measured in the atmospheric boundary layer about a simulated block building

Instrumented wind towers are used to measure the three components of wind about a simulated block building. The mean horizontal wind profiles over the building are compared with wind profiles measured in the absence of the building and the wind speed deficit in the wake of the building is correlated.Horizontal mean wind speeds measured in the natural atmospheric boundary layer with and without the presence of a simulated building show excellent reproducibility and agreement with fundamental concepts of fluid mechanics. The data possess all the characteristic features reported from wind-tunnel studies of building flows. In the present study the turbulence intensity is of the order of 20% in the undisturbed flow whereas the free stream turbulence intensity of wind-tunnel studies is generally not more than 5%. The effect of smaller averaging periods and the structure of the turbulence will be reported at a later time.The velocity profiles measured in the undisturbed flow zones support the representation of a neutrally stable atmospheric boundary layer with a logarithmic wind profile.     

Field study of dimethylsulfide oxibation in the boundary layer: Variations of dimethylsulfide,methanesulfonic acid,sulfur dioxide,non-sea-salt sulfate and aitken nuclei at a coastal site

Measurements of atmospheric dimethylsulfide (DMS) and its oxidation products, sulfur dioxide (SO₂), methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO₄ ^2-) were monitored during the period June 9–26, 1989 at a coastal site in Brittany. As indicated by the radon (Rn-222) activities and the high concentrations of NOx the air masses, for most of the experiment, were continental in origin. The observed concentrations range from 1.9 to 65 nmol/m³ for DMS (n=157), 0.6 to 94.2 nmol/m³ for SO₂ (n=50), 0.6 to 11.6 nmol/m³ for MSA (n=44) and 42 to 350 nmol/m³ for nss-SO₄ ^2- (n=44). Aitken nuclei reached values as high as 4.5 × 10⁵ particles/m³. When continental conditions predominated, the measured SO₂ concentrations were lower than those expected from a consideration of the observed DMS concentrations and the existence of SO₂ background of the continental air masses. Similarly, compared to the MSA/DMS ratio in the marine atmosphere, higher concentrations of MSA were observed than those expected from the measured levels of DMS. The presence of enhanced levels of MSA was also endorsed by the observation that the measured mean MSA/nss-SO₄ ^2- ratio of 6±3% was similar to the mean value of 6.9% observed in the marine atmosphere. These above observations are in line with recent laboratory findings by Barnes et al. (1988), which show an increase of the MSA/DMS yield with a simultaneous decrease of the SO₂/DMS yield in the presence of NOx.