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Overview of the field measurement campaign in Hyytiälä, August 2001 in the framework of the EU project OSOA

As part of the OSOA (Origin and formation of Secondary Organic Aerosols) project, two intensive field campaigns were conducted in Melpitz, Germany and Hyytiälä, Finland. This paper gives an overview of the measurements made during the Hyytiälä campaign, which was held between 1 and 16 August 2001. Various instrumental techniques were used to achieve physical and chemical characterisation of aerosols and to investigate possible precursor gases. During the OSOA campaign in Hyytiälä, particle formation was observed on three consecutive days at the beginning of the campaign (1 to 3 August 2001) and on three days later on. The investigation of the meteorological situation divided the campaign into two parts. During the first three days of August, relatively cold and clean air masses from northwest passed over the station (condensation sink – CS: <0.002 s-1, NOx: <0.5 ppb). Daily particle bursts of one fraction of the nucleation mode aerosols (3–10 nm) with number concentrations between 600–1200 particles cm-3 were observed. After this period, warmer and more polluted air from south-west to south-east arrived at the station (CS: 0.002–0.01 s-1, NOx: 0.5–4 ppb) and during these 13 days only three events were observed. These events were not as apparent as those that occurred during the earlier period of the campaign. The chemical analyses from different institutes of PM2, PM2.5 and PM10 particles confirmed the assumption that organic matter from the oxidation of various terpenes contributed to the formation of secondary organic aerosols (SOA). Concerning these conclusions among others, the ratio between formic (oxidation product of isoprene and monoterpenes by ozone) and acetic acid (increased by anthropogenic emissions) (ratio=1 to 1.5) and concentration of different carboxylic acids (up to 62 ngm-3) were investigated. Gas/particle partitioning of five photo-oxidation products from α- and β-pinene resulted in higher concentrations of pinonic, nor pinonic and pinic acids in the particle phase than in the gas phase, which indicates a preference to the particle phase for these compounds. The average growth factors (GF) from 100 nm particles in water vapour gave a diurnal pattern with a maximum during daytime and values between 1.2 and 1.7. On average, the amount of secondary organic carbon reached values around 19% of the sampled aerosols and we speculate that formation of SOA with the influence of photo-oxidation products from terpenes was the reason for the observed particle bursts during the campaign. However, correlations between the precursor gases or the favourable condensing species with the monitored nucleation mode particles were not found. For the investigated time period other factors like the condensation sink of newly formed particles to the pre-existing aerosols, temperature and solar irradiance seem to be more important steering parameters for the production of new aerosols. Another open question concerns the vertical distribution of the formation of SOA. For this reason measurements were conducted at different altitudes using a tethered balloon platform with particle sampling and particle counting equipment. They were incorporated with eddy covariance (EC) flux measurements made at 23 m above ground level. The results give first indications that production of new aerosols happens throughout the planetary boundary layer (PBL), whereby different parameters e.g. temperature, CS, solar irradiance or concentration of monoterpenes are responsible for the location of the vertical maximum.
Nitrogen oxides measurements in an Amazon site and enhancements associated with a cold front

An intensive atmospheric chemistry study was carried out in a pristine Amazonian forest site (Balbina), Amazonas state, Brazil during the 2001 wet season, as part of the LBA/CLAIRE 2001 (The Large Scale Biosphere Atmosphere Experiment in Amazonia/Cooperative LBA Airborne Regional Experiment) field campaign. Measurements of nitrogen oxide (NO), nitrogen dioxide (NO2) and ozone (O3) were performed simultaneously with aerosol particles and black carbon concentrations and meteorological parameters observations. Very low trace gases and aerosol concentrations are typically observed at this pristine tropical site. During the measurement period, there was a three-day episode of enhancement of NO2 and black carbon concentration. NO2 concentration reached a maximum value of 4 ppbv, which corresponds to three times the background concentration observed for this site. Black carbon concentration increased from the approximated 100 ng/m3 average value to a 200 ng/m3 maximum during the same period. Biomass burning spots were detected southward, between latitudes 15 to 10° S, 5–6 days before this episode from GOES-8 WF_ABBA (Wildfire Automated Biomass Burning Algorithm). An atmospheric numerical simulation of the whole measurement period was carried out using the RAMS model coupled to a biomass burning emission and transport model. The simulation results pictured a smoke transport event from Central Brazil associated to an approach of a mid-latitude cold front, reinforcing the hypothesis of biomass burning products being long-range transported from the South by the cold front and crossing the Equator. This transport event shows how the pristine atmosphere pattern in Amazonia is impacted by biomass burning emissions from sites very far away.
Sudden increases in the NO2 column caused by thunderstorms: a case study in the northern subtropical region

A long-term program for NO2 column measurements started in 1993 at the subtropical Izaña Observatory (28° N, 16° W). Seasonal evolution shows a small day-to-day variability as compared with higher latitudes. Sharp increases in the column appear occasionally superimposed on the annual cycle. The origin of these spikes is explored by considering the possibility of tropospheric transport from polluted areas, stratospheric intrusions, meridional transport in the stratosphere and production by lightning, in a case study. From radiative transfer calculations and meteorological information available, it is shown that the NO2 increase takes place in the upper troposphere with values of 300–400 pptv. Back-trajectories reveal that, for the case studied, the air masses came from an area of thunderstorms located upwind. After the analysis of the various possibilities, the NO2 increase by lightning production appears to be the most feasible cause. Annual distribution of spikes displays a maximum in late winter and spring during the shift from midlatitude winter tropopause to summer tropopause.
Aspect sensitivity of VHF echoes from field aligned irregularities in meteor trails and thin ionization layers

The aspect sensitivity of VHF echoes from field aligned irregularities (FAI) within meteor trails and thin ionization layers is studied using numerical models. Although the maximum power is obtained when a radar is pointed perpendicular to the field line (<IMG WIDTH="15" HEIGHT="14" ALIGN="BOTTOM" BORDER="0" src="acp-4-685-img1.gif" ALT="$bot$">B), substantial power can be obtained off the <IMG WIDTH="15" HEIGHT="14" ALIGN="BOTTOM" BORDER="0" src="acp-4-685-img1.gif" ALT="$bot$">B direction if the ionization trail/layer is thin. When the FAI length along B is 20 m, the power observed 6° off <IMG WIDTH="15" HEIGHT="14" ALIGN="BOTTOM" BORDER="0" src="acp-4-685-img1.gif" ALT="$bot$">B is about 10 db below that perpendicular to the B direction. Meteoric FAI echoes can potentially be used to determine the diffusion rate in the mesopause region. Based on the aspect sensitivity analysis, we conclude that the range spread trail echoes far off <IMG WIDTH="15" HEIGHT="14" ALIGN="BOTTOM" BORDER="0" src="acp-4-685-img1.gif" ALT="$bot$">B observed by powerful VHF radars are likely due to overdense meteors. Our simulation also shows that ionospheric FAI echoes can have an altitude smearing effect of about 4 km if the vertical extension of a FAI-layer is around 100 m, which has often been observed at Arecibo. The altitude smearing effect can account for the fact that the Es-layers observed by the Arecibo incoherent scatter radar are typically much narrower than FAI-layers and the occurrence of double spectral peaks around the Es-layer altitude in FAI echoes.
The impact of anthropogenic chlorine emissions, stratospheric ozone change and chemical feedbacks on stratospheric water

Mixing ratios of water (H2O) in the stratosphere appear to increase due to increased input of H2O and methane from the troposphere and due to intensified oxidation of CH4 in the stratosphere, but many of the underlying mechanisms are not yet understood. Here we identify and quantify three chemical mechanisms which must have led to more efficient oxidation of CH4 in the stratosphere over the past several decades: 1) The increase in stratospheric chlorine levels due to anthropogenic CFC emissions, 2) the thinning of the stratospheric ozone column and 3) enhanced OH levels in the stratosphere due to increasing H2O levels themselves. In combination with the increase in tropospheric CH4 mixing ratios and with solar cycle related variations of upper stratospheric ozone, these effects can explain about 50% of the additional conversion of CH4 to H2O as observed throughout the stratosphere. The relative contributions from the individual processes have varied over the past decades.
Canadian Meteor Orbit Radar (CMOR)

The radar system described here (CMOR) comprises a basic 5-element receiving system, co-located with a pulsed transmitter, specifically designed to observe meteor echoes and to determine their position in space with an angular resolution of ~1° and a radial resolution of ~3 km. Two secondary receiving sites, a few km distant and arranged to form approximately a right angle with the base station, allow the determination of the velocity (speed and direction) of the meteor that, together with the time of occurrence, lead to an estimate of the orbit of the original meteoroid. Some equipment details are presented along with a method used to determine the orbits. Representative echoes are shown and observations on the 2002 Leonid shower presented.
Cloud chemistry at the Puy de Dôme: variability and relationships with environmental factors

The chemical composition of cloud water was investigated during the winter-spring months of 2001 and 2002 at the Puy de Dôme station (1465 m above sea level, 45°46′22′′ N, 2°57′43′′ E) in an effort to characterize clouds in the continental free troposphere. Cloud droplets were sampled with single-stage cloud collectors (cut-off diameter approximately 7 µm) and analyzed for inorganic and organic ions, as well as total dissolved organic carbon. Results show a very large variability in chemical composition and total solute concentration of cloud droplets, ranging from a few mg l-1 to more than 150 mg l-1. Samplings can be classified in three different categories with respect to their total ionic content and relative chemical composition: background continental (BG, total solute content lower than 18 mg l-1), anthropogenic continental (ANT, total solute content from 18 to 50 mg l-1), and special events (SpE, total solute content higher than 50 mg l-1). The relative chemical composition shows an increase in anthropogenic-derived species (NO3-, SO42- and NH4+) from BG to SpE, and a decrease in dissolved organic compounds (ionic and non-ionic) that are associated with the anthropogenic character of air masses. We observed a high contribution of solute in cloud water derived from the dissolution of gas phase species in all cloud events. This was evident from large solute fractions of nitrate, ammonium and mono-carboxylic acids in cloud water, relative to their abundance in the aerosol phase. The comparison between droplet and aerosol composition clearly shows the limited ability of organic aerosols to act as cloud condensation nuclei. The strong contribution of gas-phase species limits the establishment of direct relationships between cloud water solute concentration and LWC that are expected from nucleation scavenging.
Technical Note: A diagnostic for ozone contributions of various NOx emissions in multi-decadal chemistry-climate model simulations

Nitrogen oxide (NOx=NO+NO2) emissions from various sources contribute to the ozone budget. The identification of these contributions is important, e.g. for the assessment of emissions from traffic. The non-linear character of ozone chemistry complicates the online diagnosis during multi-decadal chemistry-climate simulations. A methodology is suggested, which is efficient enough to be incorporated in multi-decadal simulations. Eight types of NOx emissions are included in the model. For each a NOy (=all N components, except N2 and N2O) tracer and an ozone tracer is included in the model, which experience the same emissions and loss processes like the online chemistry fields. To calculate the ozone changes caused by an individual NOx emission, the assumption is made that the NOx relative contributions from various sources are identical to the NOy relative contributions. To evaluate this method each NOx emission has been increased by 5% and a detailed error analysis is given. In the regions of the main impact of individual sources the potential error of the calculated contribution is significantly smaller than the contribution. Moreover, the changes caused by an increase of the emissions of 5% were detected with a higher accuracy than the potential error of the absolute contribution.
Evaporation of high speed sporadic meteors

Recent measurements conducted at the Arecibo Observatory report high-speed sporadic meteors having velocities near 50 km/s. The results seem to indicate a bimodal velocity distribution in the sporadic meteors (maxima at ~20 km/s and ~50 km/s). The particles have a maximum mass of ~1µg. This paper will present an analysis of the ablation of 1µg meteoroids having velocities of 20, 30, 50, and 70 km/s. The calculations show that there is fractionation even for the fast meteoroids, the effect being particularly noticeable for the 1µg sporadic particles, and less so for the heavier particles. The relevance of the calculations to the radar observations of the sporadic meteors will be discussed.
Tracing troposphere-to-stratosphere transport above a mid-latitude deep convective system

Within the project SPURT (trace gas measurements in the tropopause region) a variety of trace gases have been measured in situ in order to investigate the role of dynamical and chemical processes in the extra-tropical tropopause region. In this paper we report on a flight on 10 November 2001 leading from Hohn, Germany (52ºN) to Faro, Portugal (37ºN) through a strongly developed deep stratospheric intrusion. This streamer was associated with a large convective system over the western Mediterranean with potentially significant troposphere-to-stratosphere transport. Along major parts of the flight we measured unexpectedly high NOy mixing ratios. Also H2O mixing ratios were significantly higher than stratospheric background levels confirming the extraordinary chemical signature of the probed air masses in the interior of the streamer. Backward trajectories encompassing the streamer enable to analyze the origin and physical characteristics of the air masses and to trace troposphere-to-stratosphere transport. Near the western flank of the intrusion features caused by long range transport, such as tropospheric filaments characterized by sudden drops in the O3 and NOy mixing ratios and enhanced CO and H2O can be reconstructed in great detail using the reverse domain filling technique. These filaments indicate a high potential for subsequent mixing with the stratospheric air. At the south-western edge of the streamer a strong gradient in the NOy and the O3 mixing ratios coincides very well with a sharp gradient in potential vorticity in the ECMWF fields. In contrast, in the interior of the streamer the observed highly elevated NOy and H2O mixing ratios up to a potential temperature level of 365 K and potential vorticity values of maximum 10 PVU cannot be explained in terms of resolved troposphere-to-stratosphere transport along the backward trajectories. Also mesoscale simulations with a High Resolution Model reveal no direct evidence for convective H2O injection up to this level. Elevated H2O mixing ratios in the ECMWF and HRM model are seen only up to about tropopause height at 340 hPa and 270hPa, respectively, well below flight altitude of about 200 hPa. However, forward tracing of the convective influence as identified by satellite brightness temperature measurements and counts of lightning strokes shows that during this part of the flight the aircraft was closely following the border of an air mass which was heavily impacted by convective activity over Spain and Algeria. This is evidence that deep convection at mid-latitudes may have a large impact on the tracer distribution of the lowermost stratosphere reaching well above the thunderstorms anvils as claimed by recent studies using cloud-resolving models.