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Atmospheric Environment 48 (2012) 122e128

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Atmospheric Environment

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AprileMay 2010 Eyjafjallajökull volcanic fallout over Rimini, Italy

Paolo Rossini a, Emanuela Molinaroli b,*, Giovanni De Falco c, Federica Fiesoletti a,Stefano Papa d, Elena Pari a, Alberto Renzulli d, Pierpaolo Tentoni a, Alessio Testoni a,Laura Valentini d, Gabriele Matteucci a

a Istituto di Ricerca Gruppo C.S.A., via Al Torrente 22, 47923 Rimini, ItalybDipartimento di Scienze Ambientali, Informatica e Statistica, Università Ca’ Foscari Venezia, Dorsoduro 2137, 30123 Venezia, Italyc IAMC-CNR, Località Sa’ Mardini, 09072 Torregrande, Oristano, ItalydDipartimento di Scienze della Terra, della Vita e dell’Ambiente, Università degli Studi di Urbino "Carlo Bo", Campus Scientifico, 61029 Urbino, Italy

a r t i c l e i n f o

Article history:Received 23 February 2011Received in revised form2 May 2011Accepted 5 May 2011

Keywords:Eyjafjallajökull ash cloudIcelandic tephraAtmosperic bulk deposition chemistryGrain sizeMineralogy

* Corresponding author. Tel./fax: þ39 041 2348583E-mail addresses: prossini@csaricerche.com (P.

(E. Molinaroli), giovanni.defalco@cnr.it (G. De Facom (F. Fiesoletti), stefano.papa@uniurb.it (S. Pa(E. Pari), alberto.renzulli@uniurb.it (A. Renzulli)(P. Tentoni), atestoni@csaricerche.com (A. Teston(L. Valentini), gmatteucci@csaricerche.com (G. Ma

1352-2310/$ e see front matter � 2011 Elsevier Ltd.doi:10.1016/j.atmosenv.2011.05.018

a b s t r a c t

Located at a distance of approximately 3200 km from Iceland, where the Eyjafjallajökull volcano erupted,Italy was affected by volcanic ash transported by middle altitude air masses across Europe. Volcanicemissions from the Eyjafjallajökull eruption in April 2010 were detected in Rimini (44� 20 28" N, 12� 340

3" E) (Italy) by means of in-situ measurements (sampling of bulk depositions). Sampling was carried outduring the period AprileAugust 2010, and the following parameters were determined: grain size, TSP,mineralogy, particle morphology and chemical content in terms of Br�, Cl�, F�, SO2�

4 , Al, As, Ba, Be, Ca, Cd,Ce, Co, Cr, Cu, Fe, Hg, K, Li, Lu, Mg, Mn, Mo, Na, Ni, P, Pb, S, Sb, Sc, Se, Si, Sn, Sr, Tb, Te, Ti, Tl, U, V, Y, Zn andZr. Information from the Hysplit-NOAA back trajectory helped to identify the origin of the air mass. Theresults obtained from the observations are in good agreement with similar studies carried out by otherEuropean scientists, confirming that the Eyjafjallajökull ash plume also had a surface impact in Italy. Thefindings of our study support observations made by researchers of the CNR-IMAA Atmospheric Obser-vatory at the EARLINET station in Southern Italy and enlarge the geographical area known to have beenaffected by fallout from the AprileMay 2010 eruption of the Eyjafjallajökull volcano.

� 2011 Elsevier Ltd. All rights reserved.

1. Introduction

Eyjafjallajökull is an ice-capped stratovolcano with a maximumheight of about 1660 m above sea level located near the southerncoast of Iceland. The volcano started erupting on April 14th 2010sending an ash cloud into the troposphere at over 9 km of altitude(Schumann et al., 2010). The eruption produced profuse quantitiesof fine-grained silicic ash, and the strong north-westerly windsover Iceland at that time carried this south-eastwards into thecrowded airspace of the UK and continental Europe (Petersen,2010).

Samples taken at ground level near Eyjafjallajökull by theresearchers of the Nordic Volcanological Center Institute of Earth

.Rossini), molinaro@unive.itlco), ffiesoletti@csaricerche.pa), epari@csaricerche.com, ptentoni@csaricerche.comi), laura.valentini@uniurb.ittteucci).

All rights reserved.

Sciences indicate particle sizes of up to 500 mm,withmore than 44%by mass of the particles larger than 50 mm, varying during theeruption period (Thorsteinsson, 2010). Moreover, as reported byPetersen (2010), about 24% of the sample was smaller than 10 mm,which is in the range of aerosols, and about 33% in the 10e50 mmrange.

An ash-leaching experiment carried out by the researchers ofthe Institute of Earth Sciences indicated that the main elements inthe leachate of the ash were Si (as SiO2), P, Mn and Al (Eiriksdottirand Alfredsson, 2010).

Microtephra were identified in Bergen, Norway, by the Depart-ment of Earth Science of the University of Bergen. Ash traps (25 mmsieves) were placed beneath roof gutter outlets (April 15th) andcollected the following day after a night of persistent rain.Approximately 2 cm3 of dark grey sediment was collected, sieved at80 mm to remove coarse particles and then microscopically exam-ined for ash. The 25 mm fraction revealed the presence of numerousyellow-brown coloured volcanic glass shards of intermediate type,with an average size ofw50 mm. No shards were retrieved from the>80 mm size fraction. Shard morphology was vesicular withnumerous microlithic inclusions (Sean Pyne-O’Donnell, personal

P. Rossini et al. / Atmospheric Environment 48 (2012) 122e128 123

communication, Open meeting on the Eyjafjallajökull eruption,Oxford, April 30th, 2010).

The volcanic ash was detected over the Netherlands andNorthern Germany on April 16th and in Southern Germany on April17th. It then moved southwards, reaching Italy on April 19th andGreece on April 21st (Madonna et al., 2010; Balis et al., 2010). Overseveral days starting on April 15th 2010, the radar antenna of theCNR-IMAA Atmospheric Observatory in Potenza, Southern Italy,observed signatures characterized by a clear spectral behaviourthat was attributed to the detection of ultragiant aerosol particles.The aerosol layers observed by the multi-wavelength Raman lidarwere classified by combining lidar measurements with Lagrangiandispersion models to trace the path followed by the observed airmasses, revealing that they originated in the region surroundingthe Eyjafjallajökull volcanic area (Madonna et al., 2010).

From April 16th to 24th 2010, pronounced volcanic ash layerswere also observed throughout the free troposphere at heights ofup to about 10 km by lidars in Leipzig and Munich (Ansmann et al.,2010). As reported by Labazuy et al. (2010), the back trajectorycalculated from the Hysplit-NOAA model clearly showed that ashobserved above Clermont-Ferrand at an altitude of 3000m on April19th was related to ash emitted by Eyjafjallajökull on April 16th,reaching an altitude of 5000e5500 m above the vent as deducedfrom the simulation model, which is in good accordance with in-situ radar observations. After that, the Hysplit-NOAA back trajec-tory calculated for April 20th shows that the air masses passed overNorthern Italy (Fig. 1). In May, the volcanic plume was observedover Portugal and Spain and then over Italy, Greece and SouthernGermany again (Madonna et al., 2010).

Fig. 1. Hysplit-NOAA back trajectories calculated for air masses passing over Rimini onApril 20th, 2010. Back trajectories are at low altitude (about 750 m above sea level) andhigh altitude (about 3000 m above sea level); symbols mark every 6 h along wind path.Back trajectories validate and confirm source information such as start date of ashcloud emission at Eyjafjallajökull volcano.

In order to provide more data on the impact of volcanic falloutover Europe and the related changes induced in deposition chem-istry, the total atmospheric deposition in Rimini, Italy during theperiod AprileAugust 2010 was studied. This paper describes thedata from analyses of particle size, mineralogy, morphology andchemical composition carried out on bulk samples collected atground level in order to characterise the atmospheric depositionsand provide a long-term context for the distribution patternsassociated with the AprileMay 2010 Eyjafjallajökull eruption.

2. Material and methods

A total atmospheric deposition sampling station was set up inRimini from April 19th to August 11th, 2010. Atmospheric deposi-tions were collected every 29 � 1 days in the period AprileAugust,2010.

Atmospheric depositions were collected by a bulk samplerconsisting of a cylindrical polymer container, with a ring and a netprotecting it from possible damage by birds and other animals,clamped to a 60 mm pole. Details of the instrument are fullydescribed in Rossini et al. (2005).

Inorganic micropollutants were collected in a polyethylenebottle with a polyethylene funnel placed inside the PVC container.Sampling was carried out according to Rossini et al. (2005).

Two samples were processed: the first from April 19th to May17th, 2010 (RN1), when the air masses associated with the ashemissions from Eyjafjallajökull volcano were present over Rimini(Fig. 1), and a second from July 15th to August 11th, 2010 (RN2), i.e.w2 months after the end of volcanic activity.

Equivalent sub-samples were obtained by means of a Hach-Lange Sigma 900 automatic sampler previously treated with 2%HNO3 solution overnight. Keeping them constantly mixed with anorbital mixer, samples were subdivided by the automatic samplerinto three equivalent sub-samples of 1000 ml, which were treatedas follows:

i) One sub-sample was filtered through pre-weighed 0.22 mmpore-size Nuclepore� polycarbonate filters and analysed byEnvironmental Scanning Electron Microscope (SEM) withEnergy-Dispersive Spectroscopy (EDS). Scanning electronmicroscopy was carried out using a Quanta 200 FEI scanningmicroscope equipped with an energy-dispersive X-ray micro-analytical system. Accelerated voltage of 20 or 30 kVwas usedand the probe current was 264 mA. The elemental composi-tion was determined using the prepared gold-coatedpolycarbonate filters, which were bombarded with a strong,accelerated and focalised electron beam in a vacuum(5.0 e�6mbar) prior to observation by SEM for mineralogical,morphological and chemical identification;

ii) Another sub-sample was filtered through pre-weighed0.22 mm pore-size Nuclepore� polycarbonate filters. Inorder to obtain total particulate concentrations (TSP),the insoluble fraction was dried in a dry-box and re-weighed.The particles were then re-suspended in 6& Na-Hexametaphosphate solution in an ultrasonic bath for30 min. This solution is typically used to avoid the formationof particle aggregates (Molinaroli et al., 2000). Samples wereanalysed after 24 h by the Galai Cis 1 technique (2 � 105 to3 � 105 counts), Galai Production Ltd, (now owned byAnkersmid B.V., Oosterhout, the Netherlands) to determinegrain-size distribution. The principle of the device is based ona rotating laser and the relationship between the size andtransition time of particles moving in a photodefined zone.A focused laser beam scans an area 600 mm in diameter witha beam size of 1.2 mm; when a particle is detected,

P. Rossini et al. / Atmospheric Environment 48 (2012) 122e128124

a photodiode produces a signal proportional to the size of theparticle. The Galai system has been used to analyse aerosols,distinguishing desert-dominated from European backgroundparticles (Molinaroli and De Falco, 1995; De Falco andMolinaroli, 1996);

iii) A third sub-sample was digested in Teflon bottles ina microwave digestion unit, after the addition of 5 ml of 65%HNO3, 1.5 ml of 30% H2O2 and 0.5 ml of 40% HF. The sampleswere analysed for Br�, Cl�, F�, SO2�

4 , Al, As, Ba, Be, Ca, Cd, Ce,Co, Cr, Cu, Fe, Hg, K, Li, Lu, Mg, Mn, Mo, Na, Ni, P, Pb, S, Sb, Sc,Se, Si, Sn, Sr, Tb, Te, Ti, Tl, U, V, Y, Zn and Zr by ICS 3000 IonicChromatograph (Dionex), ICP-MS 7500CE (Agilent Technol-ogies), ICP-AES 720S (Varian) and Advanced MercuryAnalyzer AMA-254 (Altec, Czech Republic). Uncertainties influx measurements were estimated at � 18%. This value wasdetermined by considering the variability arising fromsampling blanks (�6%), repetition of samples (�7%) andmethod blanks (�5%). Quality control was carried out inaccordance with UNI CEI EN ISO/IEC 17025 and with refer-ence to certified standard materials (HISS1, NIST1648,NIST2583, PACS1) treated as bulk samples. All procedureswere conducted in a clean room equipped with a laminarflow bench.

3. Results and discussion

3.1. Particle size distribution

Fig. 2 shows the grain size frequency plots and cumulativedistributions of four monthly bulk deposition samples. The RN1

Fig. 2. Comparison of representative frequencies and cumulative distributions of grainsize particles in bulk samples.

sample contains a high proportion of coarse particles with bimodaldistribution. The coarser mode is in the range of 44e63 mm and thefiner mode 4e5.5 mm (median: 42 mm). The RN2 sample containsa higher proportion of fine particles (median 27.5 mm) and showsa slightly bimodal distribution; we consider it to be the backgroundatmospheric deposition of the area. Indeed, samples of atmosphericfallout obtained by sampling monthly bulk depositions collected inJuneeJuly 2010 (RN3), and bulk depositions representing theregional coastal background (Northern Adriatic Sea), have a similarproportion of fine particles to sample RN2. Both RN3 and theregional coastal background show the finer mode at 4e5.5 mm andthe coarser mode between 16 and 22 mm. The higher proportion ofcoarse particles at 44e63 mm seen in RN1 demonstrates that isindeed anomalous.

The presence of the coarser particles in RN1 may be related tothe volcanic ash, also observed over several days by Madonna et al.(2010) in Potenza, Southern Italy, characterized by a clear spectralbehaviour that was attributed to the detection of ultragiant aerosolparticles.

To evaluate and characterise the RN1 samples we madea comparisonwith samples taken at ground level on April 15th and17th at 55 km and 20 km respectively from the Eyjafjallajökullvolcano. Estimates of particle grain size from the Eyjafjallajökullplume provided by the Icelandic Institute of Earth Sciences(Thorsteinsson, 2010) indicate that particle size is greater closer tothe eruption site. The particle size of samples taken at 20 km rangedfrom 1.5 to 500 mm, and at 55 km ranged from 1.5 to 300 mm. TheRN1 sample, taken atw3200 km, is finer, with particle size rangingfrom 0.5 to 88 mm. This supports a possible aging effect on the ashparticles collected in Rimini.

Observations of large aerosol particles injected into the atmo-sphere and undergoing long-range transport have been reported inthe literature on the transport of desert dust, particularly from theSahara Desert to the Mediterranean area and Europe (Molinaroli,1996; Guerzoni et al., 1997) and to the Atlantic and Caribbeanregions (Schütz et al., 1981). Evidence of long-range transport ofIcelandic ash has been detected in marine sediments and glacier ice(Lacasse, 2001). In the present study the significance of the grainsize data was checked against independent information, i.e.,geological signatures in terms of morphological, mineralogical andgeochemical characteristics.

3.2. Morphological and mineralogical characteristics

During the analysis of the samples, several particles wereinvestigated using an SEM with an attached energy-dispersiveEDS detector to determine the aspect ratio, morphology,and chemical composition of each single particle. Based on thelisted characteristics, we tried to identify the pyroclastic mate-rial (volcanic fragments, crystals and glass shards) in sampleRN1.

Preliminary analysis of the particles from the bulk samplecollected in April revealed the presence of glass shards. Fig. 3 showsan SEM image of a typical ash particle (glass shard), with a sizeof w65 mm. The frequency of the glass shards in the particlepopulation is approximately 5% and that of the volcanic fragmentsis w25%.

Our data were compared with the morphology of ash collectedcloser to the Eyjafjallajökull volcano, as referenced in Schumannet al. (2010), Davies et al. (2010) and Dawson et al. (2011).Schumann et al. (2010) collected volcanic ash particle samples withimpactor-sampling devices inside a fuselage placed in a Falconaircraft. These samples were taken over the North Atlantic involcanic ash clouds from different eruption periods (7e12 h age).The glass shard shown in Fig. 4A isw20 mm and has a blocky shape.

Fig. 3. SEM image of glass shard observed in RN1 sample.

P. Rossini et al. / Atmospheric Environment 48 (2012) 122e128 125

Dawson et al. (2011) studied the impact of volcanic ash fallout onScottish natural resources. They collected surface snow samplesfrom the Cairngorm plateau on April 18th in which they foundvolcanic glass shards (Fig. 4B). Analysis of dust from vehicle

Fig. 4. Volcanic ash particles from three different areas: A) North Atlantic (Schumann et al.,(Davies et al., 2010).

surfaces and rainwater samples obtained by Davies et al. (2010)revealed the presence of long-fluted volcanic glass particles inBelfast, Northern Ireland (Fig. 4C).

The glass shards from the North Atlantic, Scotland, NorthernIreland and Rimini show morphological variations due to thedifferent transport distances and temporal scale of collections(from a few hours to a few days after the eruption).

SEM studies of the RN1 sample showed that most particles werecrystalline, i.e. not glass shards. For the larger particles, silicates andmixed particles were the most abundant groups (Figs. 5 and 6). It isclear from the observations that these particles are characterised bysharp morphology despite the aeolian transport, which normallyproduces dissolution, alteration and abrasion of the grains. Ourobservations support the hypothesis put forward byMadonna et al.(2010) that the non-spherical ultragiant tephra particles injectedinto the upper troposphere during the Eyjafjallajökull eruptioncould have been transported over more than 4000 km and ona longer temporal scale than 72 h, possibly up to 120 h. Theaggregates of particles mostly consisted of silicates with biologicalparticles and other crystalline phases (Fig. 6).

In agreement with Schumann et al. (2010) sample RN1 showssilicate grains in mixtures of various minerals. Based on chemicalcomposition, the mixtures predominantly consist of feldspars,amphiboles/pyroxenes, and quartz minerals in variableproportions.

The size distribution of the two samples (RN1 and RN2) wasbimodal in both cases, with one size peak corresponding to theparticles which fell singly (5.5e8 mm) and are assumed to be of

2010); B) Cairngorm plateau, Scotland (Dawson et al., 2011; C) Belfast, Northern Ireland

Fig. 5. SEM image showing crystal pyroclasts from sample RN1. Energy-dispersive analyses show that A is pyrogenic K-feldspar and B is pyroxene.

P. Rossini et al. / Atmospheric Environment 48 (2012) 122e128126

regional and local origin. The second mode (44e63 mm) is morepronounced in sample RN1 (see Fig. 2), reflecting both smallerparticles which fell as aggregates (Fig. 6) and single coarse particles(Fig. 5). The sample contains lithic and crystalline volcanic ashparticles as well as vitric material.

The SEM analysis of sample RN2 showed differences inmorphological and mineralogical composition. Fig. 7 shows smallparticles, predominantly rounded, of clay and biological material.

The results of the grain size and mineralogical analyses carriedout on our samples confirm the evidence of Madonna et al. (2010),who observed ultragiant particles using a Ka-Band Doppler radar inSouthern Italy from April 19th to May 13th 2010.

3.3. Chemistry of bulk depositions

The atmospheric bulk deposition fluxes observed during thestudy period are shown in Table 1.

The concentrations of Br�, F�, Be, Sc, Te, U, Y were below thedetection limits (0.2, 0.05 mg l�1 and 0.005, 0.5, 0.005, 0.05,0.5 mg l�1 respectively) in both bulk samples and are not reported.

Fig. 6. SEM image of aggregate of large and small particles, of both inorganic andorganic origin, from sample RN1. Particle in centre is K-feldspar.

In order to compare the deposition profiles of samples collectedin this study with others arising from the Eyjafjallajökull eruption,the results obtained by researchers from the Nordic VolcanologicalCenter Institute of Earth Sciences (Oskarsson, 2010; Eiriksdottir andAlfredsson, 2010) and by Schumann et al. (2010) from differenttypes of samples were compared with data from the atmosphericbulk samples collected in Rimini. In detail, these reference samplesreveal:

i) The chemical composition of volcanic ash and scoria from theEyjafjallajökull eruption;

ii) The concentration of dissolved elements that were leachedfrom the Eyjafjallajökull ash in the ash-leaching experimentcarried out by the researchers of the Nordic VolcanologicalCenter Institute of Earth Sciences;

iii) The composition of the silicates within the volcanic ashclouds of different eruption periods and different plume ages.

As can be seen in Table 1, the bulk fluxes of TSP, SO2�4 , Al, Ce, Fe,

Hg, K, Li, P, Si and Ti reached significantly high values in the periodApril 19theMay 17th, 2010 (sample RN1), 3e4 times higher than

Fig. 7. SEM image showing inorganic and organic particles from sample RN2. Largeparticle in centre is organic.

Table 1Atmospheric bulk deposition fluxes observed in Rimini during the study period.

Sample RN1 RN2

Start 19/04/2010 17.45 15/07/2010 12.10

Stop 17/05/2010 12.00 11/08/2010 14.12

Rain mm 182.2 96.4TSP mg m�2 d�1 45380 � 8168 11387 � 2050Cl� mg m�2 d�1 12864 � 2316 7366 � 1326SO4¼ mg m�2 d�1 11814 � 2126 3914 � 705Al mg m�2 d�1 2769 � 498 697 � 125As mg m�2 d�1 0.74 � 0.13 0.26 � 0.05Ba mg m�2 d�1 52 � 9 29 � 5Ca mg m�2 d�1 13924 � 2506 9622 � 1732Cd mg m�2 d�1 0.35 � 0.06 0.14 � 0.03Ce mg m�2 d�1 3.67 � 0.66 0.76 � 0.14Co mg m�2 d�1 0.86 � 0.16 0.38 � 0.07Cr mg m�2 d�1 7.81 � 1.41 3.76 � 0.68Cu mg m�2 d�1 20 � 4 21 � 4Fe mg m�2 d�1 1638 � 295 497 � 89Hg mg m�2 d�1 0.036 � 0.007 0.010 � 0.002K mg m�2 d�1 2313 � 416 668 � 120Li mg m�2 d�1 2.40 � 0.43 0.78 � 0.14Lu mg m�2 d�1 0.84 � 0.15 0.43 � 0.08Mg mg m�2 d�1 1852 � 333 935 � 168Mn mg m�2 d�1 64 � 11 30 � 5Mo mg m�2 d�1 0.95 � 0.17 0.54 � 0.10Na mg m�2 d�1 8607 � 1549 4446 � 800Ni mg m�2 d�1 11.01 � 1.98 4.72 � 0.85P mg m�2 d�1 425 � 77 116 � 21Pb mg m�2 d�1 230 � 41 398 � 72S mg m�2 d�1 4600 � 828 1948 � 351Sb mg m�2 d�1 5.07 � 0.91 1.92 � 0.34Se mg m�2 d�1 0.39 � 0.07 0.27 � 0.05Si mg m�2 d�1 9510 � 1712 2714 � 488Sn mg m�2 d�1 3.21 � 0.58 2.26 � 0.41Sr mg m�2 d�1 41 � 7 28 � 5Tb mg m�2 d�1 0.30 � 0.05 0.87 � 0.16Ti mg m�2 d�1 175 � 32 50 � 9Tl mg m�2 d�1 0.07 � 0.01 0.05 � 0.01V mg m�2 d�1 6.45 � 1.16 2.30 � 0.41Zn mg m�2 d�1 94 � 17 54 � 10Zr mg m�2 d�1 4.72 � 0.85 1.63 � 0.29

P. Rossini et al. / Atmospheric Environment 48 (2012) 122e128 127

the period July 15the August 11th, 2010 (sample RN2). Fig. 8 showsthe comparison between the observed deposition fluxes and theRegional coastal deposition background (Rossini et al., 2001, 2005).The figure shows that whereas the deposition fluxes observedin the period July 15th e August 11th, 2010 (sample RN2) arecomparable with the Northern Adriatic Sea deposition background,

Fig. 8. Comparison of atmospheric deposition fluxes with Regional coast

during the period April 19th e May 17th, 2010 (sample RN1) thereis an enrichment of Si, K, Al, Fe, P, Ti, Mn, Cr and Ni.

These results agree with data reported for the Eyjafjallajökulleruption fingerprint by other European researchers.

The Institute of Earth Sciences observed that the main elementsseen in the dissolution of ash from Eyjafjallajökull were Si (as SiO2),P, Mn and Al (Eiriksdottir and Alfredsson, 2010).

As reported by Schafer et al. (2011), the elements Mn, P, Sc, Sr, Ti,Y and Zr were more than twice as rich in the Eyjafjallajökull ashesas the average composition of the Earth’s crust; by using theseelements as indicators, the authors conclude that the increasedconcentrations of Ti, Mn, Sr, Y and Zr in Southern Germany on April19th and 20th were evidently a result of the impact of the volcanicplume on PM10 concentrations.

Moreover, as reported by Schumann et al. (2010), the elementscharacterising the volcanic emissions were mainly Si, Al, Fe andCa, although they varied with time within the ash plumes,reflecting the varying proportions of the different silicateminerals. The Si/Al ratio detected in sample RN1 (3.4) fell withinthe 2.8e3.6 range reported by Schumann et al. (2010), thus indi-cating similar feldspar components, whereas in sample RN2 theobserved ratio (3.9) was higher, probably due to the prevalence oflocal coastal particles.

Furthermore, for the same period, Colette et al. (2011) observedan increase and subsequent decrease of Al, Fe and Ti during theeruption in Mulhouse (France), quite unusual in ambient air, whichthey associated with the impact of the Eyjafjallajökull plume on thesurface.

Since the deposition fluxes observed during July 15th e August11th, 2010 (sample RN2) are comparable to the Regional depositionbackground, we can consider this sample as representative of thenormal study period deposition conditions in Rimini. Based on thisassumption, we calculated the deposition surplus by subtracting fromsample RN1 the values obtained for RN2. Fig. 9 compares the relativeabundances of Si, Al, Fe, Ti, Mn, Sr and Zr in the Rimini depositionsurplus and in the Eyjafjallajökull SRG2b ash sample (Sigmundssonet al., 2010). As can be seen, the anomalous profile corresponding tothe deposition surplus is very similar to the elemental profile of theSRG2b sample,whichwas collectedonApril 15th fromtheash layeronMýrdalssandur, Iceland (Sigmundsson et al., 2010).

Based on these observations we can conclude, in agreementwith other European researchers, that the increased atmosphericdeposition fluxes of Si, K, Al, Fe, P, Ti, Mn, Cr and Ni observed inRimini during the period April 19th e May 17th 2010 were due tothe impact of the Eyjafjallajökull volcanic plume.

al deposition background (Rossini et al., 2001; Rossini et al., 2005).

Fig. 9. Relative abundance of key elements in Rimini deposition surplus and Eyjafjallajökull SRG2b ash sample (Sigmundsson et al., 2010).

P. Rossini et al. / Atmospheric Environment 48 (2012) 122e128128

4. Conclusions

Although all these estimates carry uncertainties, the signifi-cance of the present study is supported by the diversification of theproxies, since its multidisciplinary approach combines manyindependently modelled or measured parameters (Hysplit-NOAAback trajectory modelling, particle size distribution, mineralogicaland morphological characteristics and chemical determinations).The results obtained from all observations are in good agreementwith similar studies carried out by other European scientists. As faras we know, our in-situ measurements are the only available datareported for deposition from the Eyjafjallajökull eruption in Italy.

The findings of our study support the observations made by theresearchers of the CNR-IMAA Atmospheric Observatory at theEARLINET station in Southern Italy and enlarge the geographicalarea affected by fallout from the AprileMay 2010 Eyjafjallajökullvolcanic eruption.

Acknowledgements

This is contribution n 144 of the Istituto di Ricerca Gruppo CSA.George Metcalf revised the English text. Authors thank Mr. Tadeofor his technical support.

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