ALBERT

Description: On 14 January 2001, the four Cluster spacecraft passed through the northern magnetospheric mantle in close conjunction to the EISCAT Svalbard Radar (ESR) and approached the post-noon dayside magnetopause over Green-land between 13:00 and 14:00 UT. During that interval, a sudden reorganisation of the high-latitude dayside convection pattern occurred after 13:20 UT, most likely caused by a direction change of the Solar wind magnetic field. The result was an eastward and poleward directed flow-channel, as monitored by the SuperDARN radar network and also by arrays of ground-based magnetometers in Canada, Greenland and Scandinavia. After an initial eastward and later poleward expansion of the flow-channel between 13:20 and 13:40 UT, the four Cluster spacecraft, and the field line footprints covered by the eastward looking scan cycle of the Söndre Strömfjord incoherent scatter radar were engulfed by cusp-like precipitation with transient magnetic and electric field signatures. In addition, the EISCAT Svalbard Radar detected strong transient effects of the convection reorganisation, a poleward moving precipitation, and a fast ion flow-channel in association with the auroral structures that suddenly formed to the west and north of the radar. From a detailed analysis of the coordinated Cluster and ground-based data, it was found that this extraordinary transient convection pattern, indeed, had moved the cusp precipitation from its former pre-noon position into the late post-noon sector, allowing for the first and quite unexpected encounter of the cusp by the Cluster spacecraft. Our findings illustrate the large amplitude of cusp dynamics even in response to moderate solar wind forcing. The global ground-based data proves to be an invaluable tool to monitor the dynamics and width of the affected magnetospheric regions.Key words. Magnetospheric cusp, ionosphere, reconnection, convection flow-channel, Cluster, ground-based observations

Description: This paper presents strong experimental evidence for a major perturbation in ozone concentrations over large parts of the North Atlantic Ocean from the surface to 8 km associated with continental pollutants. The evidence was gathered in the course of 7 flights by the UK Meteorological Office C-130 aircraft based on the Azores, and 4 ferry flights between the UK to the Azores in spring and summer 1997 as a component of the NERC-funded ACSOE project. The total latitude range covered was approximately 55°N–25°N, and the longitude range was approximately 0° to 40°W. Many profiles were made between the sea surface and altitudes up to 9 km to survey the composition of the marine atmosphere. The C-130 aircraft was comprehensively equipped to measure many chemical and physical parameters along with standard meteorological instrumentation. Thus it was able to measure ozone and speciated NOy, along with tracers including water vapour, carbon monoxide and condensation nuclei, in near real time. The overall "picture" of the troposphere over large parts of the North Atlantic is of layers of pollution from the continents of different ages interspersed with layers of air uplifted from the marine boundary layer. The lowest ozone concentrations were recorded in the marine boundary layer where there is evidence for extensive ozone destruction in summer. Flights were made to penetrate the outflow of hurricane Erica, to determine the southerly extent of polluted air in summer, to examine the impact of frontal systems on the composition of remote marine air, and to trace long-range pollution from the west coast of the USA interspersed with air with a stratospheric origin. In one of the spring flights it is possible that a plume of polluted air with high ozone and NOy, and with an origin in southeast Asia, was intercepted off the coast of Portugal. The concentrations of NOx, in this plume were sufficient for ozone formation to be continuing along its track from west to east. The instrument to measure NOy almost certainly was only measuring the sum of organic nitrates (mostly in the form of PAN) plus NOx. The high correlation between NOy and ozone under these conditions strongly suggests a non-stratospheric source for most of the ozone encountered over large parts of the atmosphere upwind of Europe. There was a marked seasonal variation in the NOy with about twice as much present in the spring flights than in the summer flights. The overall ozone levels in both spring and summer were somewhat similar although the highest ozone concentration encountered (~100 ppbv) was observed in summer in some polluted layers in mid Atlantic with an origin in the boundary layer over the southeastern USA. The bulk of the pollutants, ozone, CO, and NOy, were in the free troposphere at altitudes between 3 and 8 km. The only instances of pollution at lower levels were in the form of ship plumes, which were encountered several times. The data therefore strongly support the need for more in-situ aircraft experiments to quantify and understand the phenomenon of long-range transport of pollution from continent to continent. Observations at ground-based stations are inadequate for this purpose and satellite data is incomplete both in terms of its altitude detail and in the extent of chemical speciation, particularly for ascertaining whether chemical production and destruction processes for ozone are occurring.

Description: We report values of the columnar tropospheric aerosol optical depth at UV wavelengths based on experimental measurements of the direct spectral irradiances carried out by a commercial spectroradiometer (Li1800 of Licor company) covering the range from 300–1100 nm at two stations with different climate characteristics in Spain. The first station is located in a rural site in north central Spain with continental climate. The data extend from March to the end of October of 1995. The other station is a coastal site in the Gulf of Cádiz (southwest Spain) of maritime climate type. This study is mainly focused on the capability of estimating aerosol optical depth values in the UV region based on the extracted information in the visible and near infrared ranges. A first method has been used based on the Ångström turbidity parameters. However, since this method requires detailed spectral information, a second method has also been used, based on the correlation between wavelengths. A correlation has been established between the experimental aerosol optical depth values at 350 nm and 500 nm wavelengths. Although the type of aerosol seems to be the key factor that determines the quality of these estimations, the evaluation of the associated error is necessary to know the behaviour of these estimations in each area of study.Key words. Atmospheric composition and structure (aerosols and particles; transmission and scattering of radiation; troposphere – composition and chemistry)

Description: Chemical ozone loss in the Arctic stratosphere was investigated for the twelve years between 1991 and 2003 employing the ozone-tracer correlation method. For this method, the change in the relation between ozone and a long-lived tracer is considered for all twelve years over the lifetime of the polar vortex to calculate chemical ozone loss. Both the accumulated local ozone loss in the lower stratosphere and the column ozone loss were derived consistently, mainly on the basis of HALOE satellite observations. HALOE measurements do not cover the polar region homogeneously over the course of the winter. Thus, to derive an early winter reference function for each of the twelve years, all available measurements were additionally used; for two winters climatological considerations were necessary. Moreover, a detailed quantification of uncertainties was performed. This study further demonstrates the interaction between meteorology and ozone loss. The connection between temperature conditions and chlorine activation, and in turn, the connection between chlorine activation and ozone loss, becomes obvious in the HALOE HCl measurements. Additionally, the degree of homogeneity of ozone loss within the vortex was shown to depend on the meteorological conditions. Results derived here are in general agreement with the results obtained by other methods for deducing polar ozone loss. Differences occur mainly owing to different time periods considered in deriving accumulated ozone loss. However, very strong ozone losses as deduced from SAOZ for January in winters 1993-1994 and 1995-1996 cannot be identified using available HALOE observations in the early winter. In general, strong accumulated ozone loss was found to occur in conjunction with a strong cold vortex containing a large volume of possible PSC existence (VPSC), whereas moderate ozone loss was found if the vortex was less strong and moderately warm. Hardly any ozone loss was calculated for very warm winters with small amounts of VPSC during the entire winter. This study supports the linear relationship between VPSC and the accumulated ozone loss reported by Rex et al. (2004) if VPSC was averaged over the entire winter period. Here, further meteorological factors controlling ozone loss were additionally identified if VPSC was averaged over the same time interval as that for which the accumulated ozone loss was deduced. A significant difference in ozone loss (of ≈36DU) was found due to the different duration of solar illumination of the polar vortex of at maximum 4 hours per day in the observed years. Further, the increased burden of aerosols in the atmosphere after the Pinatubo volcanic eruption in 1991 significantly increased the extent of chemical ozone loss.

Description: During the Mediterranean Intensive Oxidant Study MINOS in August 2001, 87 air samples were collected at the ground-based station Finokalia (35°19'N, 25°40'E) on the north coast of Crete and subsequently analysed by GC-MS. The analysis includes various hydrocarbons, organo-halogens, HCFCs and CFCs. These compounds have a wide variety of sources and sinks and a large range of atmospheric lifetimes. We evaluated the characteristics of the sampling site in terms of proximity to individual sources by plotting the measured variability of these species against lifetime. The resulting linear relationship suggests that the sampling site is representative of intermediate conditions between a remote site and one that is in the vicinity of a wide variety of sources. Our analysis of air mass origin and chemical ratios also shows that several distinct anthropogenic sources influenced the atmospheric composition over Crete. Propane observations are compared to a global model to assess the fossil fuel related emission inventory. Although the model reproduces the general pattern of the propane variations, the model mixing ratios are systematically too low by a factor of 1.5 to 3, probably due to an underestimation of the propane emissions from east European countries in the underlying global database EDGAR. Another important finding was that methyl chloroform, a compound banned under the Montreal protocol, showed significant enhancements from background, which were well correlated with CFC-113. This suggests continued use and emission of methyl chloroform by one or more European countries. We also discuss the observed variations of methyl bromide and suggest that the significant peak observed on 12 August 2001 reflects heavy agricultural use as a soil fumigant in Italy.

Description: A recent World Meteorological Organisation report discussed the importance of continued study of the effect of clouds on the solar UV radiation reaching the earth's surface. The report mentions that the use of all-sky imagery offers the potential to understand and quantify cloud effects more accurately. There are an increasing number of studies investigating the enhancement of surface solar, UV irradiance, and UV actinic flux, using automated CCD and sky imagers. This paper describes new algorithms applicable to a commercially available all-sky imager (TSI-440), for research investigating cloud enhanced spectral UV irradiance. Specifically, these include three new algorithms relating to cloud amount at different spatial positions from 1) zenith and 2) from the solar position and 3) the visible brightness of clouds surrounding the sun. A possible relationship between UV enhancement and the occurrence of near-sun cloud brightness is reported based on this preliminary data. It is found that a range of wavelength dependent intensities, from 306 to 400 nm, can occur in one day for UV enhancements. Evidence for a possible decreasing variation of intensity with longer wavelengths is also presented.

Description: Following recent observations of molecular iodine (I2) in the coastal marine boundary layer (MBL) (Saiz-Lopez and Plane, 2004), it has become important to determine the absolute absorption cross-section of I2 at reasonably high resolution, and also to evaluate the rate of photolysis of the molecule in the lower atmosphere. The absolute absorption cross-section (σ) of gaseous I2 at room temperature and pressure (295K, 760Torr) was therefore measured between 182 and 750nm using a Fourier Transform spectrometer at a resolution of 4cm-1 (0.1nm at λ=500nm). The maximum absorption cross-section in the visible region was observed at λ=533.0nm to be σ=(4.24±0.50)x10-18cm2molecule-1. The spectrum is available as supplementary material accompanying this paper. The photo-dissociation rate constant (J) of gaseous I2 was also measured directly in a solar simulator, yielding J(I2)=0.12±0.03s-1 for the lower troposphere. This is in excellent agreement with the value of 0.12±0.015s-1 calculated using the measured absorption cross-section, terrestrial solar flux for clear sky conditions and assuming a photo-dissociation yield of unity. A two-stream radiation transfer model was then used to determine the variation in photolysis rate with solar zenith angle (SZA), from which an analytic expression is derived for use in atmospheric models. Photolysis appears to be the dominant loss process for I2 during daytime, and hence an important source of iodine atoms in the lower atmosphere.

Description: Aerosol number size distributions have been measured since 5 May 1997 in Helsinki, Finland. The presented aerosol data represents size distributions within the particle diameter size range 8-400nm during the period from May 1997 to March 2003. The daily, monthly and annual patterns of the aerosol particle number concentrations were investigated. The temporal variation of the particle number concentration showed close correlations with traffic activities. The highest total number concentrations were observed during workdays; especially on Fridays, and the lowest concentrations occurred during weekends; especially Sundays. Seasonally, the highest total number concentrations were observed during winter and spring and lower concentrations were observed during June and July. More than 80% of the number size distributions had three modes: nucleation mode (30nm), Aitken mode (20-100nm) and accumulation mode (90nm). Less than 20% of the number size distributions had either two modes or consisted of more than three modes. Two different measurement sites were used; in the first (Siltavuori, 5.5.1997-5.3.2001), the arithmetic means of the particle number concentrations were 7000cm, 6500cm, and 1000cm respectively for nucleation, Aitken, and accumulation modes. In the second site (Kumpula, 6.3.2001-28.2.2003) they were 5500cm, 4000cm, and 1000cm. The total number concentration in nucleation and Aitken modes were usually significantly higher during workdays than during weekends. The temporal variations in the accumulation mode were less pronounced. The lower concentrations at Kumpula were mainly due to building construction and also the slight overall decreasing trend during these years. During the site changing a period of simultaneous measurements over two weeks were performed showing nice correlation at both sites.

Description: The cycling of inorganic bromine in the marine boundary layer (mbl) has received increased attention in recent years. Bromide, a constituent of sea water, is injected into the atmosphere in association with sea-salt aerosol by breaking waves on the ocean surface. Measurements reveal that supermicrometer sea-salt aerosol is substantially depleted in bromine (often exceeding 50%) relative to conservative tracers, whereas marine submicrometer aerosol is often enriched in bromine. Model calculations, laboratory studies, and field observations strongly suggest that the supermicrometer depletions reflect the chemical transformation of particulate bromide to reactive inorganic gases that influence the processing of ozone and other important constituents of marine air. Mechanisms for the submicrometer enrichments are not well understood. Currently available techniques cannot reliably quantify many Br containing compounds at ambient concentrations and, consequently, our understanding of inorganic Br cycling over the oceans and its global significance are uncertain. To provide a more coherent framework for future research, we have reviewed measurements in marine aerosol, the gas phase, and in rain. We also summarize sources and sinks, as well as model and laboratory studies of chemical transformations. The focus is on inorganic bromine over the open oceans outside the polar regions. The generation of sea-salt aerosol at the ocean surface is the major tropospheric source producing about 6.2 Tg/a of bromide. The transport of Br from continents (as mineral aerosol, and as products from biomass-burning and fossil-fuel combustion) can be of local importance. Transport of degradation products of long-lived Br containing compounds from the stratosphere and other sources contribute lesser amounts. Available evidence suggests that, following aerosol acidification, sea-salt bromide reacts to form Br2 and BrCl that volatilize to the gas phase and photolyze in daylight to produce atomic Br and Cl. Subsequent transformations can destroy tropospheric ozone, oxidize dimethylsulfide (DMS) and hydrocarbons in the gas phase and S(IV) in aerosol solutions, and thereby potentially influence climate. The diurnal cycle of gas-phase Br and the corresponding particulate Br deficits are correlated. Higher values of Br in the gas phase during daytime are consistent with expectations based on photochemistry. We expect that the importance of inorganic Br cycling will vary in the future as a function of both increasing acidification of the atmosphere (through anthropogenic emissions) and climate changes. The latter affects bromine cycling via meteorological factors including global wind fields (and the associated production of sea-salt aerosol), temperature, and relative humidity.

Description: The European-funded MOZAIC programme (Measurements of ozone and water vapour by Airbus in-service aircraft) has been operational since 1994 aboard 5 commercial Airbus A340. It has gathered ozone and water vapour data between the ground and an altitude of 12 km from more than 20 000 long-range flights. A new infrared carbon monoxide analyser has been developed for installation on the MOZAIC equipped aircraft. Improvements in the basic characteristics of a commercial CO analysers have achieved performance suitable for routine aircraft measurements : ±5 ppbv, ±5% precision for a 30 s response time. The first year of operation on board 4 aircraft with more than 900 flights has proven the reliability and the usefulness of this CO analyser. The first scientific results are presented here, including UTLS exchange events and pollution within the boundary layer.