Bull Volcanol (2004) 66:226–242 DOI 10.1007/s00445-003-0306-x RESEARCH ARTICLE Martin G. Wiesner · Andreas Wetzel · Sandra G. Catane · Eddie L. Listanco · Hannah T. Mirabueno Grain size, areal thickness distribution and controls on sedimentation of the 1991 Mount Pinatubo tephra layer in the South China Sea Received: 16 April 2002 / Accepted: 16 June 2003 / Published online: 6 September 2003 Springer-Verlag 2003 Abstract The June 15, 1991 climactic eruption of Mt. Pinatubo produced an extensive, largely co-ignimbritederived airfall ash layer on Luzon Island and across the central South China Sea. The layer covers an area of ~4105 km2 with a volume of 5.5 km3. Near the coast of Luzon, the deposit consists of two units: a normally graded basal ash bed, unimodal in grain size, and a finergrained, internally structureless upper ash bed showing grain size bimodality. With increasing distance from the source, the coarse particle populations of the two units merge and migrate towards a near-constant fine population (~11 mm); the distal region is covered by a fine-mode dominated, virtually ungraded single ash layer. The reversal of the winds from easterly directions at uppertropospheric and stratospheric levels to westerly directions in the middle and lower troposphere indicates that both the coarse- and fine-mode components fell out from high-altitude eruption clouds. The high-velocity upperlevel winds, however, would have transported finegrained ash particles far beyond the South China Sea, which suggests that their settling was accelerated by aggregation. The boundary between the units thus marks a change from fallout of predominantly discrete pyroclasts Editorial responsibility: R. Cioni M. G. Wiesner ()) Institute of Biogeochemistry and Marine Chemistry, University of Hamburg, Bundesstrasse 55, 20146 Hamburg, Germany e-mail: [email protected] Fax: +49-40-428387081 A. Wetzel Geological-Paleontological Institute, University of Basel, Bernoullistrasse 32, 4056 Basel, Switzerland S. G. Catane · E. L. Listanco National Institute of Geological Sciences, University of the Philippines, Diliman, Quezon City 1101, Philippines H. T. Mirabueno Philippine Institute of Volcanology and Seismology, C.P. Garcia Avenue, Diliman, Quezon City 1101, Philippines to simultaneous fallout of aggregated fines and freely falling, coarse-grained particles. The particle populations composing the upper ash bed were almost completely removed from the proximal areas by the upper-level winds. At lower elevations, the counterclockwise circulation of a typhoon over the coastal area advected the ash south and eastward, producing a thickness maximum in the medial region (at about 160 km from source). The strong displacement of fines, possibly aided by wind turbulence, led to a break in bulk tephra thinning rates close to the coastline. In the distal region, outside the influence of the typhoon, southwest monsoonal winds caused a distinct lobe axis inflection and thickness asymmetry. Within this region, at about 420 km from source, fallout of particle aggregates created a second thickness maximum. Comparison of the field data with previous experimental observations and tephra flux records in the deep sea (Wiesner et al. 1995; Carey 1997; McCool 2002) implies that the transport of ash in the water column was largely determined by vertical density currents. Differences in the reaction of coarse and fine particles to turbulence in the descending plumes probably suppressed the segregation of fines but allowed the coarser pyroclasts to maintain their initial order of arrival at the sea surface. Considering typical fall rates of convective plumes, modifications of the initial fallout position of the particles by the South China Sea current system are on the order of only a few kilometers. The results suggest that convective sedimentation processes ensure the preservation of atmospheric particle transport directions, distances, and fallout modes in the deep sea. Keywords Mt. Pinatubo · 1991 Tephra fallout · South China Sea · Grain size · Thickness · Volume · Sedimentation processes Introduction The grain size and thickness of deep-sea ash layers derived from subaerial eruptions are principally con- 227 Fig. 1 Thickness contours (in mm) of the June 15, 1991 Mt. Pinatubo ash fall deposit in the South China Sea (isobaths in m) and on Luzon Island (unlabeled isopach is 200 mm). On-land thicknesses (layer C) were taken from Paladio-Melosantos et al. (1996) and E. Listanco (unpublished data 1991). Marine core sites are denoted as follows: circles R/V Sonne cruises SO-132 in 1998 and SO-140 in 1999 (this study); triangles SO-95 in 1994 (Wiesner and Wang 1996); squares SO-114 and R/V Ocean Researcher 1 cruise OR-455, both in 1996 (Kuhnt et al. 1996; Wiesner et al. 1997; Wang 1999); pentagons SO-115 in 1996/1997 (Stattegger et al. 1997); diamonds 1997 cruises of R/V Explorer (F. Siringan, personal communication 1998); inversed triangles 1998 cruises of R/V Xiangyanghong-14 (R. Chen, personal communication 1999); cross 1990–1992 sediment trap mooring station SCS-C (Wiesner et al. 1995). Filled symbols ash thickness measured; half-filled symbols ash observed, thickness not reliable due to core disturbance or postdepositional redistribution; open symbols no macroscopically visible ash. Numerals at core sites refer to those tephra sections that were analyzed by sieving/pipetting and correspond with the last two digits of the station labels given in Table 1 and Figs. 3, 4, 5, and 6 trolled by eruptive column height, initial size range of ejected particles, and prevailing wind strength (e.g., Kennett 1981). Despite the very low settling velocities of fine-grained tephra in seawater (Cashman and Fiske 1991), distinct modifications of the fallout distribution by ocean currents have rarely been observed (Ninkovich and Shackleton 1975). Recent experimental studies suggest that the major mechanism counteracting subaqueous lateral advection is that ash particles can become entrained into highly accelerated vertical density currents (Carey 1997). The currents were shown to form as a result of convective instabilities in the near-surface boundary layer when the particle concentration becomes large; the increase in solids concentration is a consequence of the abrupt decrease in the settling velocity of tephra as it crosses the air-sea interface. Support for this mechanism comes from times-series particle flux studies in the deep sea, which documented tephra sinking speeds several orders of magnitude higher than predicted by Stokes’ law (Wiesner et al. 1995). Laboratory experiments have also shown that, apart from particle loading, convective sedimentation depends on turbulence and water-column stratification. Turbulent motions can create large inhomogeneities in particle concentration fields (e.g., Eaton and Fessler 1994), initiating convective plume formation at even very low initial volume fractions of solids (McCool 2002). Additionally, turbulence-induced preferential concentration can cause the finer particles to be the first convectively settling out from stratified polydisperse suspensions 228 (McCool 2002; McCool and Parsons 2002). Stratification by temperature or salinity in turn can provide levels of neutral buoyancy along which particle-laden currents spread out laterally (Carey 1997; Parsons et al. 2001). These factors may thus modify the initial order and location of ash particles arriving at the sea surface. The actual implications of convective sedimentation for interpreting tephra deposits in terms of eruptive source signal and atmospheric conditions still need to be assessed (Manville and Wilson 2002). A necessary first step is to obtain information on the character and dispersal patterns of deep-sea ash layers for which the initial conditions are largely known. Such an opportunity has been provided by the 1991 eruptions of Mt. Pinatubo in the island of Luzon (Fig. 1), which generated a series of stratospheric tephra plumes that drifted across the South China Sea (e.g., Koyaguchi and Tokuno 1993; Lynch and Stevens 1996; Holasek et al. 1996). Wiesner and Wang (1996) and Wang (1999) have shown that the tephra falls formed a widespread submarine deposit extending from Luzon across the central South China Sea basin towards the shelf break off central Vietnam. Attempts to trace out processproduct relationships failed, however, because of the lack of sediment cores to reliably define downwind and acrosslobe grain size and thickness variations. This paper presents a comprehensive set of new deep-sea core data on the stratigraphy, distribution, and characteristics of the ash layer, including an estimate of the tephra volume. The results are compared with the timing and style of the eruption, syn-eruptive wind vectors, and ocean currents. The major processes controlling the tephra sedimentation are discussed. Sequence of Pinatubo eruptive events and products The 1991 volcanic activities at Mt. Pinatubo began to intensify on early June 12, when a brief sub-Plinian event generated an eruption column of at least 19 km in height (Hoblitt et al. 1996). Tephra falls were recorded mainly southwest of the vent and produced a normally graded layer of lapilli- to sand-sized andesite scoriae with minor dacite pyroclasts (layer A; Paladio-Melosantos et al. 1996). Another three vertical eruptions occurred between late June 12 and the early afternoon of June 14, followed by numerous pyroclastic-surge-producing explosions which continued for nearly 24 h (Hoblitt et al. 1996). Ash clouds were lifted to altitudes of 5 to >24 km and largely moved to the west and southwest (Lynch and Stevens 1996; Holasek et al. 1996). The resulting fallout deposits consist of a finely laminated layer of predominantly silt-sized tephra (layer B; Paladio-Melosantos et al. 1996). Upward in the layer, the proportion of dacite to andesite pyroclasts increases, reflecting the progressive replacement of the limited volume of andesitic magma in the conduit by dacitic magma (Hoblitt et al. 1996). In the early afternoon on June 15, shortly before 13:41 (GMT+8), the eruptive activity escalated into a 9-h-long climactic phase (Holasek et al. 1996; Fig. 2). During the Fig. 2 Velocity-height section of mean zonal (solid line) and meridional (dashed line) winds on June 15, 1991, combined with the timing and plume top altitudes (bold curved line) of the June 15–16 Pinatubo eruptions. Wind velocities were obtained from ECMWF ERA-40 reanalysis data sets (for reference, see European Center for Medium-Range Weather Forecasts 2000) and averaged over the area 10.25–18.75N, 109.25–120.25E; positive (negative) values indicate westerly (easterly) flow for the zonal component and northerly (southerly) flow for the meridional component. Chronology of eruptive plume events was adapted from Holasek et al. (1996) first hour, the eruption column rapidly rose to about 40 km altitude and a massive umbrella plume intruded between 25 and 35 km, expanding in all directions (Koyaguchi and Tokuno 1993). The total column height then gradually lowered by 7 km until 16:41 (Fig. 2), at which time the dome-shaped overshoot of the plume top reduced its height from about 17 to 3 km (Holasek et al. 1996). A large plume, re-attaining 35 km in altitude, was sustained over the vent for the following 2–3 h (Fig. 2). Subsequently, the eruption column continuously decreased in height, diminishing to pre-climactic levels shortly after 22:41 (Fig. 2). During the first 4–5 h after the onset of the eruption, the stratospheric umbrella plume spread nearly symmetrically to about 750 km in diameter (Holasek et al. 1996). The plume was then sheared out by the upper-level winds and started to drift to the westsouthwest at altitudes in middle stratosphere down to the upper troposphere (Self et al. 1996). By early June 16, when its leading edge had approached the east coast of Vietnam, the ash cloud covered the entire South China Sea between 7 and 18N (Lynch and Stevens 1996; Holasek et al. 1996). On Luzon Island, the climactic fallout deposited a normally graded lapilli- to sand-sized tephra bed (layer C; Paladio-Melosantos et al. 1996). The layer contains white, phenocryst-rich and tan, phenocrystpoor dacite pumice, with the former (dominant) type closely resembling the one present in the pre-climactic deposits (Hoblitt et al. 1996; Pallister et al. 1996). 229 From June 16 onward, energetic ash emissions further declined in both number and magnitude (Fig. 2) and virtually stopped by the end of September (Pinatubo Volcano Observatory Team 1991). Low-level post-climactic ash clouds were predominantly advected to the northeast, while those that rose into upper troposphere or penetrated the tropopause (~17 km) were carried to the southwest. Ash falls related to this phase formed a laminated, fine-sand- to silt-sized dacitic tephra bed (layer D; Paladio-Melosantos et al. 1996). On-land tephra thickness contours reflect both the major atmospheric transport directions and changes in the dispersive power of the eruptions. Layer A, B, and C ash lobes trend southwestward, ever-widening from A to C, whereas layer D stretches in a narrow band to the northeast with a subsidiary lobe oriented to the southwest (Paladio-Melosantos et al. 1996). Near-vent maximum thicknesses of layers A, B, C, and D are 9, 46, 33, and 94 cm, respectively; along the lobe axes the thicknesses decrease to 0.7, 1.5, 16, and 0.4 cm at the west coast of Luzon over a distance of ~50 km (Koyaguchi and Tokuno 1993; Paladio-Melosantos et al. 1996). Based on an extrapolation of the isopachs, the bulk volume of tephrafall deposits (layers A to D) was estimated at 3.8–4.8 km3 (1.8–2.2 km3 dense-rock equivalent, DRE) (PaladioMelosantos et al. 1996). Adding the dense-rock volume of the June 15 pyroclastic flow deposits (2.1–3.3 km3; Scott et al. 1996), the total magma volume would approximate 3.9–5.5 km3. Holasek et al. (1996) calculated a total magma volume of 4.8–7.8 km3 on the basis eruption rates derived from plume altitude measurements made with satellite and radar data. Sampling and methods Investigations in the South China Sea were conducted by R/V Sonne (cruises SO-132, June–July 1998, and SO-140, April–May 1999) at a total of 89 stations and water depths between 500–4,500 m (Wiesner et al. 1998, 1999; see Fig. 1). Sea-bottom cores were obtained by a Wuttke standard box-corer (equipped with a 505060 cm spade box) and a Wuttke multi-corer (equipped with 12 plastic tubes each 65 cm in length and 9.5 cm in diameter). The thickness of the ash layer was determined at various points by direct observations on split cores (using a yardstick or caliper) and by a Northwest Metasystems microresistivity probe which was inserted into the cores immediately after retrieval. The probe was similar to the system described by Andrews and Bennett (1981) and consisted of a 4-mm-wide pin with a <0.1-mm-thick edge at its vertex, mounted on a rack-and-pinion gear, with a calibrated scale of 0.1 mm accuracy. Resistivities varied with particle grain-size and packing, and significant breaks in values occurred at the ash-nepheloid layer interface and at the boundary between the ash and underlying siliciclastic sediments (clay) (for further details, see Berner 2001). The probe was inserted in 1mm steps or less and the thickness values were directly read from the scale. Measurements were carried out at positions that visually showed no signs of bioturbation, which was later cross-checked by inspection of X-ray radiographs. At least nine positions per box-core and five positions per multi-core-tube were selected. Thickness values were averaged per core and the arithmetic mean of all thickness averages per station was used for isopach construction. Contouring was performed with a PC-based program that was also used to calculate isopach areas. All thickness data refer to uncompacted ash beds as the X-ray radiographs did not exhibit any evidence for dewatering of the deposits such as elutriation pipes, dish structures or convolute bedding (Wiesner et al. 1998, 1999). Tephra grain size spectra were obtained by wet-sieving (<4.33f) and pipette analysis (>3.66f) at 1/3-phi intervals (particle populations >9f were not further fractionated). The overlapping range was used to reduce possible errors due to misclassified material as sieve and hydraulic size distributions are joined (Matthews 1991). This was attained by subjecting the sieve fraction >4.33f to the pipette method and starting the analyses at 3.66f. The material hydraulically coarser than the sieve aperture it passed through was then added to the quantity retained in the appropriate interval of the wet-sieving method. Since at a variety of stations the amounts of ash recovered from the cores were insufficient to fully perform the sieving/ pipetting procedure, all ash samples were subjected to a Galai CIS-100 Laser Particle Sizer. Analyses were performed at steps of 2 and 12 mm over the size ranges 2–600 and 12–3,600 mm, respectively. Particle counts were arithmetically combined on the basis of their size range overlap and normalized to reflect a 100% volume distribution between 2–3,600 mm. Maximum, median, and mean grain sizes were calculated as f1, f50, and (f16+f50+f84)/3, respectively; sorting was taken as [(f84f16)/4]+[(f95f5)/6.6] (Folk and Ward 1957). For the particle populations <9f, the correlation between the mean grain diameter obtained by the Laser method (ML) and sieving/pipetting (MS) was MS=1.13+1.03 ML (r2=0.96) at ML=1–5f; the MS-intercept largely reflects the bias of the former technique toward producing coarser-grained size spectra relative to conventional settling methods (Agrawal et al. 1991; Syvitski et al. 1991). The standard deviation of the mean grain diameter ranged between €0.01f at 1.33f and €0.06f at 5.03f for the Laser method (triplicate analyses per ash sample), and between €0.14f at 2.30f and €0.18f at 6.24f for the combined sieve/pipette method (duplicate analyses). Unless otherwise indicated, all grain size data presented in the text and figures are those obtained by the latter procedure. Point counting of the modal constituents was performed with standard petrographic and stereo-microscopes. Counts were converted to weight percent by using the densities for the Pinatubo glass and phenocrysts given in Luhr and Melson (1996). Herein the major microscope observations are described, while a detailed presentation of the modal data will be given in Wiesner et al. (in preparation). Bulk grain densities (Dg) of the ash samples 230 Fig. 3 Stratigraphy and grain size distributions of the submarine Mt. Pinatubo ash fall deposit in four representative cores downwind along the main dispersal axis (distance from source is given in brackets; see inset for core locations). Open bars unit I; black bars unit II; grey bars single ash layer were measured gas-pycnometrically using a Micromeritics 1305 Multivolume Pycnometer. Bulk ash densities (Db) were calculated as Db=Dg(1P/100), where P is the total porosity (porosity values were taken from Haeckel et al. 2001). Electron microprobe analyses were carried out on a Philips Camebax 724. To obtain information on the composition of the very fine particles, all fractions >9f were analyzed by a Philips PW 3710 X-ray diffractometer. In the following sections, the terms proximal, medial and distal are used to designate downwind ash deposits at distances of <50 (on-land tephra), 50–340, and >340 km, respectively, from the volcano. sharp contact to unit II. Particle populations are unimodal in grain-size with maximum clast and median diameters around 0.4f and 2.2f, respectively, and a fine tail that extends into the clay fraction (Fig. 3 and Table 1). Downwind along the axis, the thickness decreases to 1 mm southeast of the Scarborough seamounts (station 132-13; Fig. 4a) over a distance of 250 km. This is paralleled by the following textural changes: (1) maximum clast and coarse particle median grain sizes decrease; (2) the percentage of fines increases producing a secondary mode at around 6.5f; and (3) particle sorting becomes poorer (Figs. 3, 5; Table 1). Unit II is a finer-grained, virtually ungraded greyish tan layer (Fig. 3), showing a southward displacement of its isopachs relative to the position of the lobe axis of unit I (Fig. 4b). The greatest near-coast thickness of the unit occurs west of Lubang Island (27 mm at station 132-37; Fig. 4b and Table 1). There, the particle populations are poorly sorted (1.5f) and distinctly bimodal with modes at around 3.6 and 6.8f, and a maximum clast size of about 2.8f (Table 1). Upsection in the layer, the coarse ash component fines, whereas the fine mode remains nearly constant (which typifies all coastal deposits of unit II; Fig. 3). From station 132-37 towards the west-northwest the thickness of the unit decreases, passes through a minimum of 11 mm at 118.2E, and then increases again to 29 mm at station 132-13 (Fig. 4b). Concurrently, the Grain size and dispersal characteristics of the submarine tephra The submarine Pinatubo airfall deposit consists of two units in the medial areas, referred to as unit I (base) and unit II (top), whereas the distal region is covered by a single ash layer. Unit I is a coarse-grained, ‘salt-andpepper’-colored tephra (Fig. 3) which displays a regular west-southwesterly directed dispersal pattern up to the Manila Trench; beyond the trench the lobe axis curves to the west-northwest (Fig. 4a). In the on-axis core closest to the coast (station 140-25, 88 km from the volcano), the unit is 72 mm thick and distinctly normally graded with a 231 Table 1 Grain size data (in f-units) of the 1991 Mount Pinatubo tephra layer and its stratigraphic units in the South China Sea. The position of the core stations is shown in Fig. 1. For the formulas Core station number Distancea (km) SO-140-25 88 SO-132-41 111 SO-132-37 134+ SO-132-29 213 SO-132-28 248 SO-132-13 SO-132-14 SO-140-04 SO-132-07 SO-140-03 SO-132-05 341 418 496 594 644 768d used in calculating the statistical grain size parameters, refer to the Sampling and Methods section Stratigraphic section Thickness (mm) Maximum clast size Bulk ash Unit II Unit I Bulk ash Unit II Unit I Bulk ash Unit II Unit I Bulk ash Unit II Unit I Bulk ash Unit II Unit I Bulk ash Bulk ash Bulk ash Bulk ash Bulk ash Bulk ash 88 16 72 61 14 47 41 27 14 52 16 36 47 14 33 31 32 33 15 7 4 0.39 2.05 0.35 0.68 2.14 0.61 2.34 2.84 1.69 1.67 2.53 1.51 1.96 2.41 1.85 2.39 2.73 3.28 3.22 3.38 4.07 Median diameter Fine mode Coarse mode 6.49 6.46 6.75 6.82 6.76 6.79 6.76 6.56 6.56 6.47 6.56 6.62 6.48 6.76 6.65 6.59 6.60 5.83 6.15 2.22 3.29 2.19 2.44 3.52 2.37 3.90 4.30 3.64 3.14 4.08 2.95 3.40 3.78 3.31 3.69 4.02 4.22 4.44 - Meanb Sorting >4fc (wt%) >5f (wt%) 2.81 5.54 2.30 2.84 5.41 2.41 5.29 5.93 4.47 4.44 5.73 3.85 4.67 5.66 4.30 5.66 5.78 6.21 6.09 5.88 6.24 1.64 1.87 1.16 1.51 1.94 0.99 1.64 1.48 1.56 1.88 1.62 1.65 1.82 1.77 1.70 1.83 1.67 1.44 1.42 1.43 1.21 19.28 77.88 9.73 18.94 68.33 8.15 72.81 87.73 48.45 50.48 84.18 31.47 53.88 78.72 41.65 76.94 83.28 94.24 93.29 94.05 99.25 16.76 68.22 8.41 15.81 57.91 6.61 57.40 72.81 32.25 40.02 69.00 23.77 41.95 66.11 30.04 65.90 69.19 82.21 78.29 73.14 85.96 a On axis downwind from vent; bmean (M) is correlated with the coarse mode median (MdC) by M=1.23+1.74 MdC (r2=0.90); cwt% of particles >0f is >99.7 in all deposits; dProjected onto lobe axis (see Fig. 5) maximum clast size and coarse-mode median shift to coarser levels (with a relatively stationary fine mode) and gradually merge with the ones of unit I (Fig. 5). As a consequence, the contact between the units becomes gradational (Fig. 3) and therefore the thickening of unit II (thinning out of unit I) in the area of station 132-13 is not well defined. Specific mineralogical or geochemical signatures serving to distinguish between the two units were not detected (see next section and Wang 1999) and, hence stratigraphic correlation with the distal ash bed cannot be established. This bed consists of a single, internally structureless pale-grey layer, which is characterized by the dominance of the fine ash component (Fig. 3). Figure 4 shows that the mean grain sizes of the layer cover the same range of values as the majority of unit II (~5.2–6.3f), while the respective values of unit I plot at 2.5–5.1f. On the basis of these data and the striking similarity in structural appearance (Fig. 3), the distal deposits were combined with unit II (Fig. 4b). The joined isopachs produce two discrete thickness maxima: one off Lubang Island around station 132-37 (henceforth referred to as the Lubang maximum) and a second one centered southwest of the Scarborough seamount chain (Fig. 4b). The second maximum (31–33 mm) stretches to the west-northwest over a distance of 160 km, beyond which the layer thins regularly towards the east coast of Vietnam (Fig. 1). In the same direction, maximum clast and coarse-mode median diameters continuously fine, whereas the fine mode maintains relatively uniform values (Fig. 5). The thickness distribution of the total submarine deposit defines a tephra lobe extending from Luzon across the South China Sea from 11.5 to 16.5N and 111.5 to 120E (Fig. 1). Proximal to the coast, the thickness contours are dominated by unit I and the lobe is nearly symmetric about its dispersal axis which trends to the west-southwest. At about 230 km from the volcano, the axis swings to the west-northwest, accompanied by a pronounced asymmetry of the lobe with a north-northeastward biased thickness distribution perpendicular to the axis. South of the Macclesfield Bank, the orientation of the axis becomes obscure because of the limited amount of across-lobe thickness data (Fig. 1). Along the dispersal axis, the total deposit thins exponentially from 88 mm near the coast to 35 mm at 118.2E (~280 km from source). Farther downwind, the bulk ash isopachs do not contour a discrete second thickness maximum but a narrow, spur-like structure south of the Scarborough seamounts. Beyond this structure (referred to as the ‘Scarborough spur’ in Fig. 5), the bulk deposit continuously thins to the 1-mm isopach at ~980 km from the vent (Fig. 1). The bulk ash on-axis grain size distributions exhibit a medially dominant coarse mode that migrates toward and eventually merges with a relatively constant fine mode with increasing distance away from the coast (Figs. 5, 6). Beyond 640 km, the particle populations are 232 Fig. 4 Thickness contours (in mm) of a unit I (unlabeled isopach is 50 mm) and b unit II (*combined with the single ash layer to show the total distribution of fine ash). Core site symbols are as in Fig. 1 but filled where the boundary between unit I and II is sharp, halffilled where boundary is gradual, and open where no boundary is present. Numbers in italics at core sites are mean grain sizes (in funits) for the particle populations <9f. Values were obtained by the Laser method and converted to sieve/pipette particle means on the basis of the equation given in the section on Sampling and Methods (bracketed values denote sites where contamination of the ash section by particles from above and beneath was difficult to avoid during sampling). Bold dashed line represents the bulk ash lobe axis (see Fig. 1) unimodal and tail off towards the 9f-level (Fig. 6). However, the quantity of particles >9f (~10 wt%; Fig. 6) is too large to be expressed as a continuing fining tail, which suggests the existence of a second mode in the very fine size range of the distal deposits. X-ray powder diffractograms of the >9f fractions (not shown) were all characterized by a large, unresolved baseline hump. This typically occurs in the presence of substantial amounts of amorphous silica (e.g., Poulsen et al. 1995), indicating that these fractions are dominated by glass shards. Fig. 5 Downwind variations in a thickness, b maximum clast size, and c median diameter of the submarine Mt. Pinatubo tephra layer and its stratigraphic units as a function of distance from source along the bulk ash dispersal axis. Short-dashed thickness line in a indicates diffuse contact between unit I and II. Bracketed data in b and c refer to core sites located south of the lobe axis (their source distance was orthogonally projected onto the center line; see Fig. 1 for core positions). Note that stations 132-37, -28, -29, -13, and -14 plot along a line which connects the thickness maximum of unit II with the one of the distal ash layer (cf. Figs. 1, 4) Correlation with the subaerial tephra fall deposits Unit I contains white (and very rarely tan) pumice and vitric shards totaling up to a glass content of 24–36 wt%. The remaining fraction consists of 38–52 wt% plagioclase (mean An=35 mol%); 20–23 wt% hornblende, occasionally rimmed by cummingtonite (mean Mg#=67); 3–5 wt% 233 Fig. 6 Bulk ash grain size distributions of the submarine Mt. Pinatubo tephra layer at increasing distance downwind along the main dispersal axis. Also shown is the percentage of ash in the >9f size range as a function of distance from source. Size spectra of unit I (open bars) and unit II (black bars) are stacked and normalized to the bulk ash deposit on the basis of unit thickness and unit bulk density (averaging 1.3 and 1.1 g/cm3, respectively); grey bars single ash layer. Note that at station SO-132-13 unit I was too thin (1 mm) to be analyzed separately by sieving/pipetting; also note that the distal station SO-132-05 is positioned south of the center line (cf. Figs. 1, 5, 6) iron-titanium oxides; and <1 wt% biotite, quartz, zircon, and lithic fragments. In unit II and the distal ash layer, the content of glass is significantly increased (70–79 wt%), while the phenocrysts essentially comprise the same assemblage as in unit I (see also Wiesner et al. 1995 and Wang 1999). Throughout the deposits, glass compositions are rhyolitic (76–79% SiO2) and compatible to the highly evolved matrix glasses of the dacitic ejecta deposited during the June 1991 events on land (Pallister et al. 1996). The absence of clinopyroxene (Mg#=75–85) and cooccurring low-silica glasses (68–73% SiO2) indicates that layer A and the majority of layer B ash falls did not contribute to the submarine tephra (see Pallister et al. 1996 and Hoblitt et al. 1996 for the composition of the pre-climactic deposits). Discrete ash beds underlying unit I were not observed. Glass shards disseminated in the first 2–3 mm of the pelagic sediments beneath the base of the unit were found to be almost entirely andesitic (53–58% SiO2). These shards are identical to those reported by Yang and Fan (1990) in the pre-Pinatubo surface sediments of the eastern and central South China Sea (55–59% SiO2). However, among the mineral phases present few juvenile phenocrysts were detected, consisting of clinopyroxene (Mg#=82), plagioclase (An37), and hornblende (Mg#=68), all surrounded by clear vesiculated glass (69–76% SiO2). Pre-climactic ash plumes must therefore have crossed the eastern South China Sea, which is also seen from satellite images (Lynch and Stevens 1996; Oswalt et al. 1996). Late B ash falls produced in the morning and early afternoon of June 15 were devoid of clinopyroxene (Hoblitt et al. 1996) and hence are indistinguishable in composition from the submarine tephra. Yet, the dispersal of the June 12–14 tephra falls in combination with the following observations suggest that, if at all, only small quantities of the late B ash settled out over the offshore stations: (1) the injection heights of the ash did not exceed the plume altitudes attained during the June 12–14 eruptions (Holasek et al. 1996); (2) the strength and direction of the high-altitude winds did not vary significantly during the pre-climactic phase, while the low- and mid-level winds shifted to more westerly directions on June 15 (see Gibson et al. 1997 for data sets); and (3) the late B particle populations were similar in grain size to those ejected during the preceding layer B eruptive events (Koyaguchi and Tokuno 1993; Paladio-Melosantos et al. 1996) and, hence, should not have been wind-transported to greater distances. Nonetheless, some of this ash could have been carried to great heights and advected far to the west as the early paroxysmal eruption column rose through the previous plume (Holasek et al. 1996). Regardless of this complexity, the base of unit I marks the onset of the climactic fallout because those particle sizes composing layer B (>4f; see Koyaguchi and Tokuno 1993) are almost absent (Fig. 3). The post-climactic ash falls plot in the range of unit II in terms of both grain size and composition (PaladioMelosantos et al. 1996; Pierson et al. 1996), but are unlikely to have contributed significantly to the unit. This is deduced from two observations: (1) the dispersal pattern of layer D is inconsistent with the vast areal extent and southward displacement of unit II; and (2) the rate of thinning of the layer to the west is distinctly higher and its thickness along the coast of Luzon is much lower than the ones of layers A and B (see section on Sequence of Eruptive Events and Products). Taken collectively, the above data lead to the conclusion that the bulk of the deep-sea tephra is the product of the climactic eruption phase. Accordingly, the isopachs of the submarine ash layer were combined with the ones of layer C (Fig. 1). The course of the thickness contours of the two units suggests that the lower bed extends onto Luzon Island, whereas the upper bed appears to be largely restricted to the South China Sea (Fig. 4). In the climactic fall deposits on land, the clear textural bipartition is lacking (PaladioMelosantos et al. 1996). Around the volcano, the normal grading of layer C is interrupted by thin pyroclastic flow and ash cloud deposits (Scott et al. 1996). This was initially taken as evidence that during the 9-h climactic 234 Fig. 7 Wind vector fields on June 15, 1991 at 14:00 local time (GMT+8) in a the lower stratosphere (70 hPa, ~19 km), b the upper troposphere (250 hPa, ~11 km), c the middle troposphere (600 hPa, ~4.5 km), and d the lower troposphere (925 hPa, ~0.8 km). Vectors were calculated from ECMWF ERA-15 reanalysis data sets (for reference see Gibson et al. 1997). Scales of velocity vectors are 10 and 20 m/s. Pinatubo tephra thickness contour intervals (in mm) are as in Fig. 1 phase Plinian pumice fall and (co-)ignimbrite activity were at least partly concurrent (Scott et al. 1996). Integrating new stratigraphic data with earlier eyewitness accounts, Rosi et al. (2001) arrived at the following results: (1) layer C accumulated during the first 3 h of the eruption; and (2) a large part of pyroclastic flow activity occurred thereafter, unaccompanied by ash falls on Luzon. The authors considered that the large plume above the vent following the initial 3-h peak (Fig. 2) was co-ignimbrite. This implies that downwind-displaced ash falls from this high-altitude plume may have generated unit II, while unit I represents the submarine counterpart of layer C. Recently, Dartevelle et al. (2002) inferred that even layer C was substantially derived from co-ignimbrite clouds, with lesser Plinian input than previously thought, based on two findings: (1) the distinctly finer-grained nature of the layer compared to fall deposits produced by Plinian eruptions of similar intensity; and (2) the strong water enrichment in the ash plumes (indicated by satellite data), which was not expected for a Plinian column. Atmospheric controls on the tephra dispersal During the climactic eruption, the winds at stratospheric and upper tropospheric levels were vectored to azimuths between 250 and 290 at speeds of 15–32 m/s; maximum wind velocities were attained at heights between 30 and 35 km (Figs. 2, 7). At lower levels, a drastic departure from the climatological mean summer wind regime was induced by Typhoon Yunya which approached eastern Luzon in the early morning of June 15 (Oswalt et al. 1996). Upon landfall, Yunya downgraded to a tropical storm and passed about 75 km northeast of Mt. Pinatubo during the initial stage of the climactic eruption. The storm then tracked north-northwestward, entered the South China Sea at approximately 20:00, and finally dissipated west of northern Luzon in the early morning of June 16 (Oswalt et al. 1996). Its counterclockwise circulation was about 500 km across, extending over Luzon, Mindoro and the eastern South China Sea from the surface up to the 400 hPa (~7.6 km) level, with wind 235 velocities of up to 12 m/s (UN Economic and Social Commission for Asia and the Pacific 1992; Figs. 2, 7). Outside the influence of Yunya’s circulation, westerly winds (1–8 m/s) prevailed at mid-tropospheric levels; in the lower troposphere winds were mainly directed to the northeast (southwest monsoon) at speeds of 10–13 m/s (Fig. 7). In Fig. 7a–d, representative wind vector fields illustrating the major changes in the flow regime with altitude were superimposed on the thickness contours of the bulk ash deposit. The plots show a clear congruence of the stratospheric and upper tropospheric wind directions with the lobe axis of the medial bulk ash deposit and hence with the lobe axis of unit I (cf. Figs. 4a, 7a, b). The southward shift of unit II, on the other hand, is in line with the northwesterly-to-westerly flow components of Yunya’s outer circulation off Luzon (cf. Figs. 4b, 7c, d). Figure 7c and d further reveal that the western boundary of Yunya’s flow system roughly coincides with the inflection point of the bulk lobe axis. Beyond that point, both the orientation of the centerline and the lobe asymmetry indicate that ash falls released from the west-southwestward drifting plume were strongly redistributed by the southwest monsoon (Fig. 7d). For the particle populations that settled out over the South China Sea, Wiesner et al. (1995) have shown that the presence of the ash components finer than about 5f is unexpected. If these particles fell freely in the June 15 wind profile from the observed height of the major eruption plumes, they would have arrived at sea level at distances of > 2,500 km downwind from the volcano. The calculations presented by the authors suggest that the finemode particles should have fallen out from lower tropospheric levels in order to accumulate in the offshore regions individually. At these levels, however, fine and coarse pyroclasts would have been transported in the opposite direction (Fig. 7c and d). Co-settling of coarse, low-density and fine, high-density individual pyroclasts can be considered to have been, if at all, of minor significance in producing the grain size bimodality. First, throughout the tephra bed, discrete phenocrysts of both plagioclase and hornblende are present in both modes (see also Wiesner et al. 1995 and Wang 1999 for the modal composition of the tephra). Secondly, in unit II and the distal ash, the coarse mode is dominated by pumice shards (70%) while the fine mode is largely composed of bubblewall shards (73%), and the density contrast between these types of shards is small (2.46 and 2.34 g/ cm3, respectively; Fisher 1965). Furthermore, the limited westward dispersal of the pre- and post-climactic ash falls argues against the possibility that the widespread occurrence of bimodal spectra is due to coarse particles overtaking fines from earlier eruptions. Consequently, both the coarse and fine ash must have been derived from high altitude (above Yunya’s flow system), and their codeposition requires a process accelerating the settling of fines. Observational and numerical evidence exist for several historical eruptive events that this process is subaerial particle aggregation (Carey and Sigurdsson 1982; Brazier et al. 1983; Cornell et al. 1983; Varekamp et al. 1984). Vapor condensation, electrostatic attraction, physical interlocking, and turbulence have been proposed as the principal mechanisms inducing aggregation (Sorem 1982; Gilbert et al. 1991; Riley et al. 2001). Basically two types of clusters are produced: (1) single-grain clusters composed of a large particle with adhering fines (settling at grain-specific rates of the largest particle); and (2) multiple-particle clusters composed of fine ash and a few larger grains (settling at aggregate-specific rates) (Schumacher 1994). The boundary between the units can thus be explained by a change from fallout of predominantly single-grain clusters to simultaneous fallout of aggregated fines and freely falling, coarse-grained particles. Multiparticle aggregates then became an increasingly important component of the two units as the individually settling particles attained lower terminal velocities. This is suggested from the general increase in the proportion of particles >5f with the fining of the coarse-mode median downwind along the lobe axis and southward to Lubang Island (Table 1 and Figs. 3, 6). The secondary thickening in the distal region and the dominance of the fine mode in the associated deposits are strikingly similar to the dispersal characteristics of two on-land ash layers: the 1980 Mount St. Helens and the 1991 Mount Hudson tephra (Sarna-Wojcicki et al. 1981; Scasso et al. 1994). For the Mount St. Helens tephra, Carey and Sigurdsson (1982) numerically reproduced the second thickness maximum by allowing all ash particles >4f to fall as aggregates; the terminal settling velocity of the aggregates was assumed to correspond to the one attained by those particles that compose the coarse-mode median of the deposits at the maximum. In the Pinatubo case, the co-deposited coarse mode at the second thickness maximum southwest of Scarborough has a median diameter of around 4.1f (Table 1). Notably, however, in the area of the Lubang maximum the coarsemode median of unit II is at about the same level (4.3f; Table 1). In both cases, the coarse particle populations were found to be dominated by glass shards and plagioclase. Hence, if the coarse-mode median is indicative of the settling velocity class of the fine-mode particles, then the two thickness maxima have to be attributed to fallout of ash aggregates of similar settling behavior. Numerical models have shown that such a case requires a considerable fraction of the total mass of particles having the same settling velocity to be present across the layer where the wind strength is highest (Armienti et al. 1988). Accordingly, the ash clusters may have fallen out from different (but great) heights, with a large proportion of aggregated fines transported at levels of the easterly (stratospheric) wind maximum. The dispersal effects of the wind regime in the middle and lower troposphere can be evaluated on the basis of the lateral variations in particle mean diameter (note that the mean diameter is positively correlated with the coarsemode median; see Table 1). In unit I, the particle mean regularly shifts to finer levels not only downwind along the lobe axis but also from the axis towards the northern 236 and southern lobe margins (Fig. 4a). In contrast, the particle means of the upper unit tend to fine from north to south across the lobe and from west to east towards Lubang Island (Fig. 4b). These trends indicate that (1) the fallout of the coarse particles generating the lower unit was not significantly affected by Yunya’s flow system; (2) the finer-grained particles and co-settling ash aggregates were sorted by size or density by the storm’s crosswinds; and (3) part of this ash was transported back toward the coast by Yunya’s westerly components. The position of the Lubang thickness maximum thus reflects overall lower effective settling velocities of the particle populations of unit II at all wind levels compared to unit I. In the distal region, the mean diameter varies irregularly across the lobe despite the strong northeasterly winds (cf. Figs. 4b, 7d). Considering the dominance of the finemode in that region, the likely reason is that the bulk of the particles were transported in aggregates; any winnowing would therefore not significantly change the granulometry of the deposits left behind. Further information on the atmospheric transport of the ash is obtained from the plot of the logarithm of thickness versus square root of isopach area in Fig. 8. The bulk ash isopach data 10 mm yield two straight best-fit lines which intercept at a thickness of 77 mm (area1/276 km); the thickness half-distances are 33 km for the proximal segment and 98 km for the medial-to-distal segment. This denotes a significant change in dispersal mechanism over the coastal area of western Luzon. The break-in-slope is too far from source to be explained by the transition from column margin to umbrella cloud sedimentation. The distance between the column corner and the central plume axis is typically less than 30% of the column height (e.g., Sparks et al. 1992). In the Pinatubo case, the height of the climactic column would imply that this transition occurs at distances of 8–11 km from the volcano. Such a break in thinning rates has not been observed, but data on nearvent localities where this feature would be expected to be seen are scarce (Paladio-Melosantos et al. 1996). The two segments are, therefore, related to fallout from the umbrella cloud. Bonadonna et al. (1998) have shown that breaks in thinning rates at greater distances from source can be a consequence of the change in sedimentation law from intermediate to low Reynolds number. The deposits comprising the proximal segment (i.e., layer C) are unimodal in grain size, with a median diameter ranging from 1 to 1f (Paladio-Melosantos et al. 1996). Such particles would settle at intermediate Reynolds numbers from the height of the ash cloud to sea level (Bonadonna et al. 1998); particles >4f in size, which are expected to fall at low Reynolds numbers, account for less than 5% of the particle populations on land (Paladio-Melosantos et al. 1996). Close to the break-in-slope, in the bulk ash deposit at station 140-25 (88 km from source), the proportion of particles >4f is about 19% and then increases to >50% farther downwind (Table 1). However, since more than 78% of the >4f-fractions are finer than 5f (Table 1), the majority of the low Reynolds number particles did not Fig. 8 Logarithm of thickness versus square root of isopach area for the June 15, 1991 Mt. Pinatubo ash-fall deposit along with two straight-line approximations for the isopach ranges 30–1 cm (T1 and T2) and 30–0.1 cm (T1 and T3) (see Fig. 1 for data source). Open symbols denote isopachs that could not be closed with confidence. Inset lists the regression equations for T1, T2, and T3. Numerals in boxes are bulk volumes in km3 calculated for the two straight-line segments T1-T2 and T1-T3 according to the method of Fierstein and Nathenson (1992). Tmax is the extrapolated thickness at the vent; bt1, bt2, and bt3 are the thickness half-distances for the segments T1, T2, and T3. Dotted lines mark the point of interception of the regression lines T1 and T2, with Tip=7.7 cm and A1/2ip= 76.3 km settle individually. Assuming again that the co-occurring coarse-mode median provides an approximation for aggregate settling behavior, neither unit I nor unit II exhibit median values plotting in the low Reynolds number regime (except at the Lubang thickness maximum); only beyond about 450 km on-axis from source do the median diameters clearly increase above the 4f-level (Table 1). This transition is too large to explain the breakin-slope in terms of particle Reynolds number. A first-order contribution to the break in thinning rates is the almost complete removal of the fine ash from the proximal areas and fallout beyond the coastline. The distal overthickening of this ash can be assumed to have provided only a second-order contribution as this process causes a decrease in tephra dispersal (e.g., Hildreth and Drake 1992). Another factor known to lower thinning rates is atmospheric turbulence, causing finer particles to be sustained aloft longer and wind-dispersed to greater distances (Fierstein and Hildreth 1992; Hildreth and Drake 1992). Aggregated ash may react similarly because of the generally highly porous nature and, consequently, low density of such clusters (Sorem 1982; Varekamp et al. 1984; Schumacher 1994). To approximate the segment of unit I and of the combined deposit of unit II and the distal ash (not shown), their isopachs 10 mm were closed by a straight line at their eastern termination. This yields decay constants of 0.004 km1 for the combined deposit and 0.010 km1 for unit I. The flatter slope 237 indicates that turbulence may have indeed influenced the dispersal of the fine ash. Subaqueous tephra sedimentation Information on the current systems that prevailed in the South China Sea in June 1991 is not available. Possible effects of subaqueous advection on the tephra distribution have, therefore, to be evaluated on the basis of long-term monthly means and modeled data. The passage of Yunya is not expected to have caused significant anomalies in upper-ocean flow because of the storm’s relatively low wind speed and short residence time (<1 day) over the South China Sea (see Behara et al. 1998 for oceanic response to typhoon forcing). Fig. 9a shows that in June the surface currents generally flow to the northeast and east-northeast at 0.18–0.22 m/s, forced by the southwestmonsoon and Ekman transport. Below the Ekman layer, the essential feature during the summer season is an anticyclonic gyre centered at 11N, 113E; off Vietnam, currents are vectored to the north-northeast, then turn to the east at 13N and finally recurve into a southsoutheasterly flow in the eastern South China Sea (Fig. 9b). The gyre gradually diffuses downdepth, paralleled by an exponential decay in maximum current velocities from 0.1 m/s at 50 m to less than 0.001 m/s below 2,000 m water depth (Shaw and Chao 1994; Chao et al. 1996). In Fig. 9 two representative current vector fields (surface and 900 m water depth) were superimposed on the thickness contours of the bulk ash deposit. The plots reveal that if particle residence times were sufficiently long, the flow regime could have contributed to both northeastward advection of fines in the distal region and southward advection off Luzon. An approximation of the mean settling velocity attained by the tephra components in the water column was obtained by Wiesner et al. (1995). The authors recorded distal fallout of Pinatubo ash in time-series sediment traps that were fixed to a bottom-tethered mooring array deployed in the central South China Sea at 4,300 m water depth; the trap depths were 1,200 and 3,700 m below sea level (see Fig. 1 for trap system position). Settling rates were determined from a trajectory analysis of the arrival of the main ash cloud over the site and the timing of ash interception by the traps. The data indicated sinking speeds of about 2.2 cm/s, or two orders of magnitude greater than predicted by Stokes’ Law for a particle corresponding in size to the median diameter of the ash collected by the traps (5.8f). To explore the underlying mechanism, settling experiments analogous to the fallout at the trap site were performed by Carey (1997). Particles 20–180 mm in diameter and a typical distal fallout mass flux rate of 0.17 g cm2 h1 (constrained by measurements from the 1980 eruption of Mount St. Helens) were used in the simulations. Three important observations were made: (1) subaerial multiparticle ash aggregates broke apart when falling onto the water surface; (2) because of the abrupt decrease in the Fig. 9 Current velocity vectors in the South China Sea at a the surface (derived from June mean ship drift data; Levitus 1982) and b 900 m water depth (re-gridded from data modeled for the southwest-monsoon period by Chao et al. 1996). Scales of velocity vectors are 0.2 and 0.004 m/s. Pinatubo tephra thickness contour intervals (in mm) are as in Fig. 1 settling of tephra from that in air to water, particle concentrations dramatically increased just below the surface, causing convective instabilities in the boundary layer; and (3) the instabilities initiated the descent of a series of ash-laden plumes or vertical density currents which settled at speeds identical to those recorded by the traps. The major difficulty in discussing convective transport-product relationships is the lack of experimental data on the textural and structural characteristics of ash beds produced by this process. The ash plumes intercepted by the traps were characterized by a coarse mode (at 3.5f) that graded toward a near-constant fine mode (at 6.5f) over the course of the fallout; both modes were composed of glass shards, hornblende and plagioglase (Wiesner et al. 1995). Convective settling must, therefore, have inhibited segregation of the fine particles released from the subaerial aggregates, but allowed sorting by size of the coarse particles. The cause for these contrasting trends may lie in differences in the reaction of particles to 238 turbulence. Convection plumes that grow out of the boundary layer produce large-scale turbulent motions causing the plumes to meander, swirl, and merge (e.g., Hoyal et al. 1999; Maxworthy 1999; Parsons et al. 2001). When these motions are faster than the Stokes settling of the particles entrained, the particles will simply follow the local velocity fluctuations and if the solid-liquid suspensions are well mixed by the turbulence, the particles should be randomly distributed (Eaton and Fessler 1994). The mean settling velocity for the fine-mode components of the ash in seawater is ~0.01 cm/s. Since this value is negligible compared to the average of the velocity fluctuations en route (i.e., to the speed of the vertically traveling plumes of ~2 cm/s), a deposit of unsorted ash is likely to be generated. The coarse-mode components clustering around 3.5f settle at ~0.7 cm/s and hence on the order of magnitude of the plume fall rate. Such particles will not have sufficient time to respond to the fluctuations and will largely follow the mean flow (e.g., McCool 2002). The coarser pyroclasts may thus have maintained their initial order of arrival at the sea surface up to the point of attaining the Stokes settling velocity class of the individual fine mode particles. Aggregation is another process which could have contributed to the vertical transport of the ash particles. Wiesner et al. (1995) assumed that in this case physical mechanisms of aggregation must have substantially dominated over biological processes because of the near-absence of organic matter in the descending plumes (<0.002 wt%). The efficiency of physically coagulated, multi-particle aggregates, however, is questioned by shear-flow and differential-settling controlled flocculation experiments performed by Lick et al. (1993). The authors used organic-free suspensions of river-borne particles in the range of very fine silt at concentrations of 0.001 to 0.2 g/L seawater. The results indicate that the time needed to generate flocs attaining settling velocities close to 2 cm/s is on the order of weeks. Furthermore, for these flocs to remain stable (at sizes on the order of millimeters), very low concentrations (0.001 g/L) are required. Irrespective of the problem that solids concentrations at the trap site cannot be quantified, the rate of aggregation is inconsistent with the timing of ash interception (<3 days; Wiesner et al. 1995). Moreover, the ash particles should flocculate at slower rates owing to their larger size. Increasing the particle concentration to 0.2 g/ L was found to reduce the time for the floc diameter to reach its maximal value (Lick et al. 1993). However, this would lead to an even greater discrepancy to the trap data because as the concentration increases both floc size and floc settling velocity significantly decrease (due to enhanced aggregate collision rates) (Lick et al. 1993; Teeter 2002). At concentrations of ~0.4 to 1 g/L, the role of flocculation as a means to accelerate the primary particles becomes insignificant; particle interactions begin to hinder settling and dense suspensions are generated which sink convectively even if flocs are still present (Parsons et al. 2001; Teeter 2002; McCool 2002). Information on the settling behavior of glass shards over this critical range of concentrations (and up to 6 g/L) has been presented by Wang (1999), Parsons et al. (2001), and McCool (2002). Settling and flocculation experiments were performed with shards in the size range of the fineash components of the Pinatubo tephra in both fresh- and seawater. In any of the experiments, the shards did not flocculate but settled convectively; high solids concentration, shard size, and the timing of convective plume formation (on the order of seconds) were proposed to have inhibited floc growth. Collectively, the experimental results and field observations imply that convective sedimentation was the major mode of ash transport at the trap site. The striking similarity in the grain size characteristics of the ash to unit II and the distal tephra layer then indicates that these deposits were produced by the same process. The almost perfect normal grading of the coarse particles in the near-coast deposits of unit I suggests that the majority of the pyroclasts settled through the water column individually. The small amounts of fine ash particles present throughout the unit (~7–8%; Fig. 3 and Table 1) may have been dragged down in the wakes of larger grains. Alternatively, in analogy to the formation of unit II, convective transport may have contributed to their co-deposition. In the lower unit, the median grain size of the coarse particle populations is 2.2f (Table 1). For the 2.2-f modal constituents (pumice, feldspar, and hornblende), the terminal settling velocities in seawater plot between about 1 and 2.5 cm/s. This range largely accords with typical fall rates of convective plumes (1–2 cm/s) measured experimentally over a wide range of particle concentrations (McCool 2002; see also Bradley 1965 and Carey 1997). Hence, if solids concentrations or turbulent mixing in the near-surface waters were sufficient to initiate vertical density currents (see Introduction), the fine ash could have co-settled with a large part of the coarse particles. Nonetheless, farther downwind, convective transport must have become predominant, generating the near-constant fine-mode in the lower unit as the coarse mode fined and finally merged with the one of unit II. During the southwest monsoon period the South China Sea is distinctly stratified, with a thermocline at ~25 m and haloclines at ~10,200, and 600 m water depths (Haupt et al. 1994). These may have provided levels of neutral buoyancy along which density currents are deflected laterally (Carey 1997). Based on the data obtained so far, it is not possible to assess the consequences of this stratification (or plume spreading on the seafloor) for the final depositional position of the particles. An estimate can be given for the current-induced modification of the initial sea surface position of a particle that becomes entrained into vertical density currents. The following conditions are considered: (1) average plume sinking rates of 2 cm/s; (2) maximum current velocities of 0.22 m/s at the surface, 0.1 m/s at 50 m, 0.007 m/s at 900 m, and 0.001 m/s at 2,000 m (see Chao et al. 1996); and (3) a linear velocity decrease between these levels. Then the maximum horizontal, unidirectional displacement of the 239 ash particles would only be about 3.3 km until settling out at the deepest core site (4,500 m water depth). This small distance strongly indicates that the fallout distribution and lobe axis inflection reflect the atmospheric conditions. Volume of the Pinatubo eruptive products Integration of the log thickness versus area1/2 plot to infinity yields a total volume of 5.5 km3 for the combined deposit of layer C and the submarine ash layer (Fig. 8). This estimate reduces to 5.2 km3 when the areas of the thinnest two isopachs (1 and 5 mm), closed by extrapolation, are included (Fig. 8). The ‘lost’ volume beyond the 10-mm contour line is about 18% of the total, providing confidence that the data measured to this isopach give a reasonably good estimate. PaladioMelosantos et al. (1996) estimated the volume of layer C at 1.1 km3, i.e., about 80% of the tephra volume fell out over the South China Sea. The average bulk ash density was calculated at 1.1 g/cm3 for both layer C (PaladioMelosantos et al. 1996) and the offshore deposits. Using a density of 2.4 g/cm3 appropriate to dacite magma, a prevesiculation volume of 2.5 km3 DRE is obtained. The total magma volume erupted then approximates 4.8– 6.0 km3 when the dense-rock volumes of layers A, B, and D (~0.21 km3; Paladio-Melosantos et al. 1996) and that of the June 15 pyroclastic flows (2.1–3.3 km3; Scott et al. 1996) are added. This is in good agreement with the estimate given by Holasek et al. (1996) (4.8–7.8 km3 DRE) and supports the reliability of volume calculations based on numerical models using remote sensing data. The total mass of the climactic tephra fall and pyroclastic flow deposits is 11–141012 kg, which translates to a value of around 6.1 for the eruption magnitude index (defined as log10[erupted mass] –7; e.g., Pyle 2000). Conclusions Tephra falls from the June 1991 climactic eruption of Mt. Pinatubo produced a discrete ash layer on Luzon Island and across the central South China Sea, covering an area of ~4105 km2. Near the coast of Luzon, the deposit consists of a normally graded unit, unimodal in grain size, which is covered by a finer-grained, internally structureless unit showing grain size bimodality. The basal ash bed correlates with the subaerial tephra fall deposits (layer C), whereas the upper unit does not appear to have an on-land counterpart. Based on recent studies (Rosi et al. 2001; Dartevelle et al. 2002), the two units may have been derived from co-ignimbrite-dominated ash plumes generated by two strong eruptive pulses during the climactic phase. With increasing distance from the volcano, the unit distinction fades as the coarse particle populations of the lower and upper ash bed merge and migrate towards a stationary fine particle population; the distal region is covered by a fine-mode dominated, virtually ungraded single ash layer. The westerly azimuths of the wind vectors at upper-tropospheric and stratospheric levels and easterly azimuths in the middle and lower troposphere indicate that both the coarse- and fine-mode components fell out from high-altitude eruption clouds. Trajectory estimates (Wiesner et al. 1995) suggest, however, that the high-altitude winds would not allow the fine ash particles to settle out individually over the South China Sea. The mechanism that accelerated the settling of fines is assumed to be particle aggregation, in analogy to conclusions drawn from other tephra layers displaying the same downwind grain size bimodality characteristics (e.g., Brazier et al. 1983). The boundary between the units can thus be explained by a change from fallout of predominantly discrete pyroclasts to simultaneous fallout of aggregated fines and freely falling, coarse-grained particles. The high-velocity upper-level winds almost completely removed the fine ash (aggregates and co-settling individual particles) from the proximal areas. At lower altitudes, the counterclockwise circulation of typhoon Yunya advected the ash southward and back toward the coast, producing both across-lobe sorting and a thickness maximum in the medial region (at about 160 km from source). The dispersal of the coarse ash forming the lower unit was not significantly affected by the typhoon’s flow system. The strong displacement of fines, possibly aided by wind turbulence, led to a significant break in bulk tephra thinning rates close to the coastline. In the distal region, outside the influence of the typhoon, southwest monsoonal winds created a distinct lobe axis inflection and thickness asymmetry. Within this region, at about 420 km from source, fallout of particle aggregates produced a second thickness maximum. Using the size of the co-deposited coarse particles as a proxy for aggregate settling behavior, it is suggested that the two maxima were formed by ash clusters grouping into the same settling velocity class. The second maximum then implies that a large fraction of the total mass of these aggregates was intruded at altitudes of the easterly (stratospheric) wind maximum. From a comparison of the field data with previous experimental observations and tephra flux records in the deep sea (Wiesner et al. 1995; Carey 1997; McCool 2002), it is concluded that the ash transport in the water column was largely determined by vertical density currents. With the onset of the fallout of aggregates and co-settling coarse pyroclasts onto the sea surface, massive amounts of slow settling individual particles were released into the boundary layer. The particles then became entrained into vertically traveling plumes that settled at rates several orders of magnitude higher than predicted by Stokes’ Law. Particles generating the lower unit near the coast largely settled discretely, but with the fining of the bulk populations farther downwind convective transport also became predominant. Re-aggregation of particles in the water column is unlikely to have played a role in enhancing the settling of the ash. Differences in the reaction of coarse and fine particles to turbulence in 240 the descending plumes probably inhibited the segregation of fines but allowed the coarser pyroclasts to maintain their initial order of arrival at the sea surface. For the rate of descent of convective plumes, modifications of the initial fallout position of the particles by the South China Sea current system are on the order of only a few kilometers. Convective sedimentation thus appears to ensure that both atmospheric particle transport directions and distances, and the modes of subaerial particle settling are preserved in the deep sea. The calculated volume of the climactic tephra fallout refines earlier total magma volume estimates for the eruptive products generated in June–September 1991 to 4.8–6.0 km3 DRE. This ranks the Pinatubo eruption the third largest of the twentieth century, following the eruptions of Novarupta in 1912 and Santa Maria in 1902 (~13€3 and >8.5 km3 DRE, respectively; Fierstein and Hildreth 1992; Williams and Self 1983). Acknowledgements The authors thank the officers and crew of R/ V Sonne for their assistance in coring operations; Fernando Siringan for providing core data obtained during the 1997 sampling campaigns on board R/V Explorer; Ronghua Chen for releasing unpublished core observations made on the 1998 cruises of R/V Xiangyanghong-14; Birgit Schwinge and Peter Berner for assistance in grain-size analyses; Stefan Hagemann for access to ECMWF data files; Hans-Rudolf Regg for assembling the microresistivity probe; Hajo Heye for the core photographs; Jeff Parsons, Wayne McCool, William Dade, and Nick McCave for insightful and stimulating discussions on convective sedimentation processes; and the German Federal Ministry of Education and Research for financial support (grant nos. 03G0132A and 03G0140A). A.Wetzel acknowledges grant no. 2100-052256 from the Swiss Science Foundation. Gerald Ernst and Steven Carey are thanked for their helpful reviews. 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