1

1

April-May 2010 Eyjafjallajökull volcanic fallout over Rimini, Italy 2

3

Paolo Rossinia, Emanuela Molinaroli

b,*, Giovanni De Falco

c, Federica Fiesoletti

a, Stefano 4

Papad, Elena Pari

a, Alberto Renzulli

d, Pierpaolo Tentoni

a, Alessio Testoni

a, Laura Valentini

d, 5

Gabriele Matteuccia 6

7 a Istituto di Ricerca Gruppo C.S.A., via Al Torrente 22, 47923 Rimini, Italy 8

b Dipartimento di Scienze Ambientali, Informatica e Statistica, Università Ca’ Foscari Venezia, 9

Dorsoduro 2137, 30123 Venezia, Italy 10 c IAMC-CNR, Località Sa’ Mardini, 09072 Torregrande - Oristano, Italy 11

d Dipartimento di Scienze della Terra, della Vita e dell'Ambiente, Università degli Studi di Urbino 12

"Carlo Bo", Campus Scientifico, 61029 Urbino, Italy 13 14 15 *Corresponding author. Tel. and fax: +39-041-2348583. 16 E-mail address: molinaro@unive.it (Emanuela Molinaroli) 17 18 prossini@csaricerche.com (Paolo Rossini) 19 giovanni.defalco@cnr.it (Giovanni De Falco) 20 ffiesoletti@csaricerche.com (Federica Fiesoletti) 21 stefano.papa@uniurb.it (Stefano Papa) 22 epari@csaricerche.com (Elena Pari) 23 alberto.renzulli@uniurb.it (Alberto Renzulli) 24 ptentoni@csaricerche.com (Pierpaolo Tentoni) 25 atestoni@csaricerche.com (Alessio Testoni) 26 laura.valentini@uniurb.it (Laura Valentini) 27 gmatteucci@csaricerche.com (Gabriele Matteucci) 28 29

30

Abstract 31

Located at a distance of approximately 3200 Km from Iceland, where the Eyjafjallajökull 32

volcano erupted, Italy was affected by volcanic ash transported by middle altitude air masses 33

across Europe. Volcanic emissions from the Eyjafjallajökull eruption in April 2010 were 34

detected in Rimini (44° 2' 28" N, 12° 34' 3" E) (Italy) by means of in-situ measurements 35

(sampling of bulk depositions). Sampling was carried out during the period April-August 36

2010, and the following parameters were determined: grain-size, TSP, mineralogy, particle 37

morphology and chemical content in terms of Br-, Cl

-, F

-, SO4

2-, Al, As, Ba, Be, Ca, Cd, Ce, 38

Co, Cr, Cu, Fe, Hg, K, Li, Lu, Mg, Mn, Mo, Na, Ni, P, Pb, S, Sb, Sc, Se, Si, Sn, Sr, Tb, Te, 39

Ti, Tl, U, V, Y, Zn and Zr. Information from the Hysplit-NOAA back trajectory helped to 40

identify the origin of the air mass. 41

2

The results obtained from the observations are in good agreement with similar studies carried 42

out by other European scientists, confirming that the Eyjafjallajökull ash plume also had a 43

surface impact in Italy. The findings of our study support observations made by researchers of 44

the CNR-IMAA Atmospheric Observatory at the EARLINET station in Southern Italy and 45

enlarge the geographical area known to have been affected by fallout from the April-May 46

2010 eruption of the Eyjafjallajökull volcano. 47

48

Keywords: Eyjafjallajökull ash cloud, Icelandic tephra, atmosperic bulk deposition chemistry, 49

grain-size, mineralogy 50

51

52

1. Introduction 53

Eyjafjallajökull is an ice-capped stratovolcano with a maximum height of about 1660 metres 54

above sea level located near the southern coast of Iceland. The volcano started erupting on 55

April 14th

2010 sending an ash cloud into the troposphere at over 9 km of altitude (Schumann 56

et al., 2010). The eruption produced profuse quantities of fine-grained silicic ash, and the 57

strong north-westerly winds over Iceland at that time carried this south-eastwards into the 58

crowded airspace of the UK and continental Europe (Petersen, 2010). 59

Samples taken at ground level near Eyjafjallajökull by the researchers of the Nordic 60

Volcanological Center Institute of Earth Sciences indicate particle sizes of up to 300 µm, with 61

more than 44% by mass of the particles larger than 50 µm, varying during the eruption period 62

(Thorsteinsson, unpublished results). Moreover, as reported by Petersen (2010), about 24% of 63

the sample was smaller than 10 μm, which is in the range of aerosols, and about 33% in the 64

10–50μm range. 65

3

An ash leaching experiment carried out by the researchers of the Institute of Earth Sciences 66

indicated that the main elements in the leachate of the ash were Si (as SiO2), P, Mn and Al 67

(Eiriksdottir and Alfredsson, unpublished results). 68

Microtephra were identified in Bergen, Norway, by the Department of Earth Science of the 69

University of Bergen. Ash traps (25 µm sieves) were placed beneath roof gutter outlets (April 70

15th

) and collected the following day after a night of persistent rain. Approximately 2 cm3 of 71

dark grey sediment was collected, sieved at 80 µm to remove coarse particles and then 72

microscopically examined for ash. The 25 µm fraction revealed the presence of numerous 73

yellow-brown coloured volcanic glass shards of intermediate type, with an average size of 74

~50 µm. No shards were retrieved from the >80 µm size fraction. Shard morphology was 75

vesicular with numerous microlithic inclusions (Sean Pyne-O’Donnell, personal 76

communication, Open meeting on the Ejyafjallajökull eruption, Oxford, April 30th

, 2010). 77

The volcanic ash was detected over the Netherlands and Northern Germany on April 16th

and 78

in Southern Germany on April 17th

. It then moved southwards, reaching Italy on April 19th

79

and Greece on April 21st (Madonna et al., 2010; Balis et al., 2010). Over several days starting 80

on April 15th

2010, the radar antenna of the CNR-IMAA Atmospheric Observatory in 81

Potenza, Southern Italy, observed signatures characterized by a clear spectral behaviour that 82

was attributed to the detection of ultragiant aerosol particles. The aerosol layers observed by 83

the multi-wavelength Raman lidar were classified by combining lidar measurements with 84

Lagrangian dispersion models to trace the path followed by the observed air masses, revealing 85

that they originated in the region surrounding the Eyjafjallajökull volcanic area (Madonna et 86

al., 2010). 87

From April 16th

to 24th

2010, pronounced volcanic ash layers were also observed throughout 88

the free troposphere at heights of up to about 10 km by lidars in Leipzig and Munich 89

(Ansmann et al., 2010). As reported by Labazuy et al. (2010), the back trajectory calculated 90

4

from the Hysplit-NOAA model clearly showed that ash observed above Clermont-Ferrand at 91

an altitude of 3000 m on April 19th

was related to ash emitted by Eyjafjallajökull on April 92

16th

, reaching an altitude of 5000-5500 m above the vent as deduced from the simulation 93

model, which is in good accordance with in-situ radar observations. After that, the Hysplit-94

NOAA back trajectory calculated for April 20th

shows that the air masses passed over 95

Northern Italy (Fig. 1). In May, the volcanic plume was observed over Portugal and Spain and 96

then over Italy, Greece and Southern Germany again (Madonna et al., 2010). 97

In order to provide more data on the impact of volcanic fallout over Europe and the related 98

changes induced in deposition chemistry, the total atmospheric deposition in Rimini, Italy 99

during the period April-August 2010 was studied. This paper describes the data from analyses 100

of particle size, mineralogy, morphology and chemical composition carried out on bulk 101

samples collected at ground level in order to characterise the atmospheric depositions and 102

provide a long-term context for the distribution patterns associated with the April-May 2010 103

Eyjafjallajökull eruption. 104

105

2. Material and methods 106

A total atmospheric deposition sampling station was set up in Rimini from April 19th

to 107

August 11th

, 2010. Atmospheric depositions were collected every 29±1 days in the period 108

April-August, 2010. 109

Atmospheric depositions were collected by a bulk sampler consisting of a cylindrical polymer 110

container, with a ring and a net protecting it from possible damage by birds and other animals, 111

clamped to a 60-mm pole. Details of the instrument are fully described in Rossini et al. 112

(2005). 113

Inorganic micropollutants were collected in a polyethylene bottle with a polyethylene funnel 114

placed inside the PVC container. Sampling was carried out according to Rossini et al. (2005). 115

5

Two samples were processed: the first from April 19th

to May 17th

, 2010 (RN1), when the air 116

masses associated with the ash emissions from Eyjafjallajökull volcano were present over 117

Rimini (Fig. 1), and a second from July 15th

to August 11th

, 2010 (RN2), i.e. ~2 months after 118

the end of volcanic activity. 119

Equivalent sub-samples were obtained by means of a Hach-Lange Sigma 900 automatic 120

sampler previously treated with 2% HNO3 solution overnight. Keeping them constantly mixed 121

with an orbital mixer, samples were subdivided by the automatic sampler into three equivalent 122

sub-samples of 1000 ml, which were treated as follows: 123

i) one sub-sample was filtered through pre-weighed 0.22 µm pore-size Nuclepore™ 124

polycarbonate filters and analysed by Environmental Scanning Electron Microscope (SEM) 125

with Energy-Dispersive Spectroscopy (EDS). Scanning electron microscopy was carried out 126

using a Quanta 200 FEI scanning microscope equipped with an energy dispersive X-ray 127

micro-analytical system. Accelerated voltage of 20 or 30 kV was used and the probe current 128

was 264 μA. The elemental composition was determined using the prepared gold-coated 129

polycarbonate filters, which were bombarded with a strong, accelerated and focalised electron 130

beam in a vacuum (5.0 e-6 mbar) prior to observation by SEM for mineralogical, 131

morphological and chemical identification; 132

ii) another sub-sample was filtered through pre-weighed 0.22 µm pore-size Nuclepore™ 133

polycarbonate filters. In order to obtain total particulate concentrations (TSP), the 134

insoluble fraction was dried in a dry-box and re-weighed. The particles were then re-135

suspended in 6‰ Na-Hexametaphosphate solution in an ultrasonic bath for 30 minutes. This 136

solution is typically used to avoid the formation of particle aggregates (Molinaroli et al., 137

2000). Samples were analysed after 24 hours by the Galai Cis 1 technique (2×105 to 3×10

5 138

counts), Galai Production Ltd, (now owned by Ankersmid B.V., Oosterhout, the Netherlands) 139

to determine grain-size distribution. The principle of the device is based on a rotating laser 140

6

and the relationship between the size and transition time of particles moving in a photodefined 141

zone. A focused laser beam scans an area 600 µm in diameter with a beam size of 1.2 µm; 142

when a particle is detected, a photodiode produces a signal proportional to the size of the 143

particle. The Galai system has been used to analyse aerosols, distinguishing desert-dominated 144

from European background particles (Molinaroli and De Falco, 1995; De Falco et al., 1996 ); 145

iii) a third sub-sample was digested in Teflon bottles in a microwave digestion unit, after the 146

addition of 5 ml of 65% HNO3, 1.5 ml of 30% H2O2 and 0.5 ml of 40% HF. 147

The samples were analysed for Br-, Cl

-, F

-, SO4

2-, Al, As, Ba, Be, Ca, Cd, Ce, Co, Cr, Cu, Fe, 148

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, 149

Zn and Zr by ICS 3000 ionic chromatograph (Dionex), ICP-MS 7500CE (Agilent 150

Technologies), ICP-AES 720S (Varian) and Advanced Mercury Analyzer AMA-254 (Altec, 151

Czech Republic). 152

Uncertainties in flux measurements were estimated at ± 18%. This value was determined by 153

considering the variability arising from sampling blanks (± 6 %), repetition of samples (± 7 154

%) and method blanks (± 5 %). Quality control was carried out in accordance with UNI CEI 155

EN ISO/IEC 17025 and with reference to certified standard materials (HISS1, NIST1648, 156

NIST2583, PACS1) treated as bulk samples. All procedures were conducted in a clean room 157

equipped with a laminar flow bench. 158

159

3. Results and discussion 160

3.1. Particle size distribution 161

Fig. 2 shows the grain size frequency plots and cumulative distributions of four monthly bulk 162

deposition samples. The RN1 sample contains a high proportion of coarse particles with 163

bimodal distribution. The coarser mode is in the range of 44-63 µm and the finer mode 4-5.5 164

µm (median: 42 µm). The RN2 sample contains a higher proportion of fine particles (median 165

7

27.5 µm) and shows a slightly bimodal distribution; we consider it to be the background 166

atmospheric deposition of the area. Indeed, samples of atmospheric fall-out obtained by 167

sampling monthly bulk depositions collected in June-July 2010 (RN3), and bulk depositions 168

representing the regional coastal background (Northern Adriatic Sea), have a similar 169

proportion of fine particles to sample RN2. Both RN3 and the regional coastal background 170

show the finer mode at 4-5.5 µm and the coarser mode between 16 and 22 µm. The higher 171

proportion of coarse particles at 44-63 µm seen in RN1 demonstrates that is indeed 172

anomalous. 173

The presence of the coarser particles in RN1 may be related to the volcanic ash, also observed 174

over several days by Madonna et al. (2010) in Potenza, Southern Italy, characterized by a 175

clear spectral behaviour that was attributed to the detection of ultragiant aerosol particles. 176

To evaluate and characterise the RN1 samples we made a comparison with samples taken at 177

ground level on April 15th

and 17th

at 55 km and 20 km respectively from the Eyjafjallajökull 178

volcano. Estimates of particle grain size from the Eyjafjallajökull plume provided by the 179

Icelandic Institute of Earth Sciences (Thorsteinsson, unpublished data 2010, available from 180

the Nordic Volcanological Center, http://earthice.hi.is/page/ies_EYJO2010_Grain) indicate 181

that particle size is greater closer to the eruption site. The particle size of samples taken at 20 182

km ranged from 1.5 to 500 µm, and at 55 km ranged from 1.5 to 300 µm. The RN1 sample, 183

taken at ~3200 Km, is finer, with particle size ranging from 0.5 to 88 µm. This supports a 184

possible aging effect on the ash particles collected in Rimini. 185

Observations of large aerosol particles injected into the atmosphere and undergoing long-186

range transport have been reported in the literature on the transport of desert dust, particularly 187

from the Sahara Desert to the Mediterranean area and Europe (Molinaroli, 1996; Guerzoni et 188

al., 1997) and to the Atlantic and Caribbean regions (Schütz et al., 1981). Evidence of long-189

range transport of Icelandic ash has been detected in marine sediments and glacier ice 190

8

(Lacasse, 2001). In the present study the significance of the grain size data was checked 191

against independent information, i.e., geological signatures in terms of morphological, 192

mineralogical and geochemical characteristics. 193

194

3.2. Morphological and mineralogical characteristics 195

During the analysis of the samples, several particles were investigated using an SEM with an 196

attached energy-dispersive EDS detector to determine the aspect ratio, morphology, and 197

chemical composition of each single particle. Based on the listed characteristics, we tried to 198

identify the pyroclastic material (volcanic fragments, crystals and glass shards) in sample 199

RN1. 200

Preliminary analysis of the particles from the bulk sample collected in April revealed the 201

presence of glass shards. Figure 3 shows an SEM image of a typical ash particle (glass shard), 202

with a size of ~65 µm. The frequency of the glass shards in the particle population is 203

approximately 5% and that of the volcanic fragments is ~ 25%. 204

Our data were compared with the morphology of ash collected closer to the Eyjafjallajökull 205

volcano, as referenced in Schumann et al. (2010), Davies et al. (2010) and Dawson et al. 206

(2011). Schumann et al. (2010) collected volcanic ash particle samples with impactor-207

sampling devices inside a fuselage placed in a Falcon aircraft. These samples were taken over 208

the North Atlantic in volcanic ash clouds from different eruption periods (7–12 h age). The 209

glass shard shown in Fig. 4A is ~ 20 µm and has a stocky shape. Dawson et al. (2011) studied 210

the impact of volcanic ash fallout on Scottish natural resources. They collected surface snow 211

samples from the Cairngorm plateau on April 18th

in which they found volcanic glass shards 212

(Fig. 4B). Analysis of dust from vehicle surfaces and rainwater samples obtained by Davies et 213

al. (2010) revealed the presence of long-fluted volcanic glass particles in Belfast, Northern 214

Ireland (Fig.4C). 215

9

The glass shards from the North Atlantic, Scotland, Northern Ireland and Rimini show 216

morphological variations due to the different transport distances and temporal scale of 217

collections (from a few hours to a few days after the eruption). 218

SEM studies of the RN1 sample showed that most particles were crystalline, i.e. not glass 219

shards. For the larger particles, silicates and mixed particles were the most abundant groups 220

(Figs. 5 and 6). It is clear from the observations that these particles are characterised by sharp 221

morphology despite the aeolian transport, which normally produces dissolution, alteration and 222

abrasion of the grains. Our observations support the hypothesis put forward by Madonna et al. 223

(2010) that the non-spherical ultragiant tephra particles injected into the upper troposphere 224

during the Eyjafjallajökull eruption could have been transported over more than 4000 km and 225

on a longer temporal scale than 72 hours, possibly up to 120 hours. The aggregates of 226

particles mostly consisted of silicates with biological particles and other crystalline phases 227

(Fig. 6). 228

In agreement with Schumann et al. (2010) sample RN1 shows silicate grains in mixtures of 229

various minerals. Based on chemical composition, the mixtures predominantly consist of 230

feldspars, amphiboles/pyroxenes, and quartz minerals in variable proportions. 231

The size distribution of the two samples (RN1 and RN2) was bimodal in both cases, with one 232

size peak corresponding to the particles which fell singly (5.5-8 µm) and are assumed to be of 233

regional and local origin. The second mode (44-63 µm) is more pronounced in sample RN1 234

(see Fig. 2), reflecting both smaller particles which fell as aggregates (Fig. 6) and single 235

coarse particles (Fig. 5). The sample contains lithic and crystalline volcanic ash particles as 236

well as vitric material. 237

The SEM analysis of sample RN2 showed differences in morphological and mineralogical 238

composition. Fig. 7 shows small particles, predominantly rounded, of clay and biological 239

material. 240

10

The results of the grain-size and mineralogical analyses carried out on our samples confirm 241

the evidence of Madonna et al. (2010), who observed ultragiant particles using a Ka-Band 242

Doppler radar in Southern Italy from April 19th

to May 13th

2010. 243

244

3.3. Chemistry of bulk depositions 245

The atmospheric bulk deposition fluxes observed during the study period are shown in Table 246

1. 247

The concentrations of Br-, F

-, Be, Sc, Te, U, Y were below the detection limits (0.2, 0.05 mg l

-248

1 and 0.005, 0.5, 0.005, 0.05, 0.5 µg l

-1 respectively) in both bulk samples and are not 249

reported. 250

In order to compare the deposition profiles of samples collected in this study with others 251

arising from the Eyjafjallajökull eruption, the results obtained by researchers from the Nordic 252

Volcanological Center Institute of Earth Sciences (Oskarsson, unpublished results; 253

Eiriksdottir and Alfredsson, unpublished results) and by Schumann et al. (2010) from 254

different types of samples were compared with data from the atmospheric bulk samples 255

collected in Rimini. In detail, these reference samples reveal: 256

i) the chemical composition of volcanic ash and scoria from the Eyjafjallajökull eruption; 257

ii) the concentration of dissolved elements that were leached from the Eyjafjallajökull ash in 258

the ash-leaching experiment carried out by the researchers of the Nordic Volcanological 259

Center Institute of Earth Sciences; 260

iii) the composition of the silicates within the volcanic ash clouds of different eruption periods 261

and different plume ages. 262

As can be seen in Table 1, the bulk fluxes of TSP, SO42-

, Al, Ce, Fe, Hg, K, Li, P, Si and Ti 263

reached significantly high values in the period April 19th

- May 17th

, 2010 (sample RN1), 3 to 264

4 times higher than the period July 15th

- August 11th

, 2010 (sample RN2). Fig. 8 shows the 265

11

comparison between the observed deposition fluxes and the Regional coastal deposition 266

background (Rossini et al., 2001; Rossini et al., 2005). The figure shows that whereas the 267

deposition fluxes observed in the period July 15th

- August 11th

, 2010 (sample RN2) are 268

comparable with the Northern Adriatic Sea deposition background, during the period April 269

19th

- May 17th

, 2010 (sample RN1) there is an enrichment of Si, K, Al, Fe, P, Ti, Mn, Cr and 270

Ni. 271

These results agree with data reported for the Eyjafjallajökull eruption fingerprint by other 272

European researchers. 273

The Institute of Earth Sciences observed that the main elements seen in the dissolution of ash 274

from Eyjafjallajökull were Si (as SiO2), P, Mn and Al (Eiriksdottir and Alfredsson, 275

unpublished results). 276

As reported by Schafer et al. (2011), the elements Mn, P, Sc, Sr, Ti, Y and Zr were more than 277

twice as rich in the Eyjafjallajökull ashes as the average composition of the Earth’s crust; by 278

using these elements as indicators, the authors conclude that the increased concentrations of 279

Ti, Mn, Sr, Y and Zr in Southern Germany on April 19th

and 20th

were evidently a result of 280

the impact of the volcanic plume on PM10 concentrations. 281

Moreover, as reported by Schumann et al. (2010), the elements characterising the volcanic 282

emissions were mainly Si, Al, Fe and Ca, although they varied with time within the ash 283

plumes, reflecting the varying proportions of the different silicate minerals. The Si/Al ratio 284

detected in sample RN1 (3.4) fell within the 2.8-3.6 range reported by Schumann et al. 285

(2010), thus indicating similar feldspar components, whereas in sample RN2 the observed 286

ratio (3.9) was higher, probably due to the prevalence of local coastal particles. 287

Furthermore, for the same period, Colette et al. (in press) observed an increase and 288

subsequent decrease of Al, Fe and Ti during the eruption in Mulhouse (France), quite unusual 289

12

in ambient air, which they associated with the impact of the Eyjafjallajökull plume on the 290

surface. 291

Since the deposition fluxes observed during July 15th

- August 11th

, 2010 (sample RN2) are 292

comparable to the Regional deposition background, we can consider this sample as 293

representative of the normal study period deposition conditions in Rimini. Based on this 294

assumption, we calculated the deposition surplus by subtracting from sample RN1 the values 295

obtained for RN2. Fig. 9 compares the relative abundances of Si, Al, Fe, Ti, Mn, Sr and Zr in 296

the Rimini deposition surplus and in the Eyjafjallajökull SRG2b ash sample (Sigmundsson et 297

al., 2010). As can be seen, the anomalous profile corresponding to the deposition surplus is 298

very similar to the elemental profile of the SRG2b sample, which was collected on April 15th

299

from the ash layer on Mýrdalssandur, Iceland (Sigmundsson et al., 2010). 300

Based on these observations we can conclude, in agreement with other European researchers, 301

that the increased atmospheric deposition fluxes of Si, K, Al, Fe, P, Ti, Mn, Cr and Ni 302

observed in Rimini during the period April 19th

- May 17th

2010 were due to the impact of the 303

Eyjafjallajökull volcanic plume. 304

305

306

4. Conclusions 307

Although all these estimates carry uncertainties, the significance of the present study is 308

supported by the diversification of the proxies, since its multidisciplinary approach combines 309

many independently modelled or measured parameters (Hysplit-NOAA back trajectory 310

modelling, particle size distribution, mineralogical and morphological characteristics and 311

chemical determinations). The results obtained from all observations are in good agreement 312

with similar studies carried out by other European scientists. As far as we know, our in-situ 313

13

measurements are the only available data reported for deposition from the Eyjafjallajökull 314

eruption in Italy. 315

The findings of our study support the observations made by the researchers of the CNR-316

IMAA Atmospheric Observatory at the EARLINET station in Southern Italy and enlarge the 317

geographical area affected by fallout from the April-May 2010 Eyjafjallajökull volcanic 318

eruption. 319

320

321

Acknowledgements 322

This is contribution n° 144 of the Istituto di Ricerca Gruppo CSA. George Metcalf revised the 323

English text. 324

325

326

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Figure captions 406

407

Fig. 1. Hysplit-NOAA back trajectories calculated for air masses passing over Rimini on 408

April 20th, 2010. Back trajectories are at low altitude (about 750 m above sea level) and 409

high altitude (about 3000 m above sea level); symbols mark every 6 h along wind path. 410

Back trajectories validate and confirm source information such as start date of ash cloud 411

emission at Eyjafjallajökull volcano. 412

Fig. 2. Comparison of representative frequencies and cumulative distributions of grain size 413

particles in bulk samples. 414

Fig. 3. SEM image of glass shard observed in RN1 sample. 415

Fig. 4. Volcanic ash particles from three different areas: A) North Atlantic (Schumann et al., 416

2010); B) Cairngorm plateau, Scotland (Dawson et al., 2011; C) Belfast, Northern 417

Ireland (Davies et al., 2010). 418

Fig. 5. SEM image showing crystal pyroclasts from sample RN1. Energy-dispersive analyses 419

show that A is pyrogenic K-feldspar and B is pyroxene. 420

Fig. 6. SEM image of aggregate of large and small particles, of both inorganic and organic 421

origin, from sample RN1. Particle in centre is K-feldspar. 422

Fig. 7. SEM image showing inorganic and organic particles from sample RN2. Large particle 423

in centre is organic. 424

Fig. 8. Comparison of atmospheric deposition fluxes with Regional coastal deposition 425

background (Rossini et al., 2001; Rossini et al., 2005). 426

Fig. 9. Relative abundance of key elements in Rimini deposition surplus and Eyjafjallajökull 427

SRG2b ash sample (Sigmundsson et al., 2010). 428

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