Arthur Leck
email: arthur.leck@gmail.com

Ludovic Bellot-Gurlet

Guillaume Carazzo

Bernard Gratuze

Jessica Langlade

François-Xavier Le Bourdonnec

Céline Bressy-Leandri

Isaac Shearn

Christian Stouvenot

Alain Queffelec
email: alain.queffelec@u-bordeaux.fr

Céline Leandri

Obsidian in the Caribbean Islands? Mysterious Ceramic Age glass artefacts in the Lesser Antilles

Keywords: Obsidian, Andesite, Lesser Antilles, Ceramic Age, Impactites, Tektites, Sourcing

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Introduction

The archipelago of Caribbean islands was settled late in the history of the peopling of America, firstly by hunter-gatherers during what is called the Archaic Age, and from ca. 500 B.C onwards, by horti-ceramicists originating from the Lower Orinoco during what is called the Ceramic Age [START_REF] Keegan | The Oxford Handbook of Caribbean Archaeology[END_REF]Reid 2018). This migration of Amerindians during the Early Ceramic period, producing specific ceramics grouped in the Saladoid serie (Rouse 1992), has been very successful in colonising the archipelago up North to Puerto Rico, while remaining strongly homogeneous in their way of life as seen in their settlement patterns, food production and consumption, and production of goods such as ceramics and lapidary ornaments [START_REF] Bérard | The Saladoid[END_REF]Queffelec 2023). Their culture underwent a transformation from ca. 750 AD, evolving into more distinct regional groups marked by varying settlement patterns, shifts in material culture, and alterations in societal organisation [START_REF] Hofman | The Post-Saladoid in the Lesser Antilles (AD 600/800-1492)[END_REF]. Then, during the Recent Ceramic period, the remaining part of the Caribbean archipelago was settled until the arrival of Europeans in the late 15th century.

During the Ceramic Age, the non-perishable material culture is mainly formed of ceramics for diverse types of pots, shells for tools and adornments, and lithics for cutting, scraping and grinding tools, as well as personal adornments. The production of flaked stone tools, of particular interest for this work, is mainly driven by production of small unretouched flakes by bipolar percussion [START_REF] Walker | Analysis and replication of lithic artifacts from the Sugar Factory pier site, St. Kitts[END_REF][START_REF] Bérard | L'utilisation de la percussion sur enclume par les premières populations agro-céramistes des Antilles[END_REF]) to be used for different activities including the production of teeth for manioc graters [START_REF] Walker | Analysis and replication of lithic artifacts from the Sugar Factory pier site, St. Kitts[END_REF]). The principal raw materials for flaked industry are flint and jaspers, respectively coming mainly from Antigua and from local sources near the archaeological sites [START_REF] Knippenberg | Stone artefact production and exchange among the Lesser Antilles[END_REF]Queffelec et al. 2023). The provenance of the lithic raw materials used to produce tools, ornaments such as beads and pendants, or other symbolic artefacts like trigonoliths, have been one of the main proxy employed by archaeologists to study the regional mobility and networks in the Caribbean islands (e.g. [START_REF] Cody | Distribution of exotic stone artifacts through the Lesser Antilles : their implications for prehistoric interaction and exchange[END_REF][START_REF] Knippenberg | Stone artefact production and exchange among the Lesser Antilles[END_REF][START_REF] Garcia-Casco | Pre-Columbian jadeitite artifacts from the Golden Rock Site, St. Eustatius, Lesser Antilles, with special reference to jadeitite artifacts from Elliot's, Antigua: Implications for potential source regions and long-distance exchange networks in the Greater Caribbean[END_REF][START_REF] Knaf | Trace-elemental and multi-isotopic (Sr-Nd-Pb) discrimination of jade in the circum-Caribbean: Implications for pre-colonial inter-island exchange networks[END_REF]Queffelec 2022;Queffelec 2023).

When investigating the origins of lithic raw materials to gain a deeper understanding of the "litho-space" of ancient societies [START_REF] Delvigne | Quels territoires en Préhistoire? Une analyse par réseaux de lieux pour penser l'espace au Paléolithique supérieur[END_REF], one invaluable resource on a global scale is the natural glass known as obsidian. This vitreous silica-rich volcanic rock originates from the cooling of a very viscous magma, preventing its crystallisation [START_REF] Tuffen | Obsidian[END_REF]). It has a geochemical composition specific to the volcanoand even to the eruptionwhich produced the magma (Shackley 1998, p.5). Obsidian has served a dual purpose, having been widely utilised by past civilizations for its knapping capabilities and by archaeologists for its high potential in geochemical fingerprinting (e.g. [START_REF] Cann | The characterization of obsidian and its application to the Mediterranean region[END_REF]Poupeau et al. 2010). Despite the extensive use of obsidian in various regions across the Americas, proving highly effective in unveiling insights into the past networks and mobility of people [START_REF] Glascock | Obsidian provenance research in the Americas[END_REF][START_REF] Golitko | Complexities of collapse: The evidence of Maya obsidian as revealed by social network graphical analysis[END_REF]Mills et al. 2013), it was a prevailing consensus among archaeologists and geologists that the Caribbean islands are devoid of such raw material despite the volcanic origin of most islands in the Lesser Antilles. The volcanic arc of the Lesser Antilles originates from the subduction of the Atlantic plate beneath the Caribbean plate. This geological process predominantly produces andesitic magma, which differs from the silica-rich rhyolitic magma essential to the formation of obsidian sensu stricto. To the best of our knowledge, no andesitic volcanic glass suitable for flaking has been documented in archaeological or geological literature. Such andesitic glass is exceptionally rare and typically forms exclusively due to cosmic impacts, either as impactites or tektites. Impactites are terrestrial rocks formed by the high energy and pressure generated by a high velocity, massive asteroid or comet impact (Osinski and Pierazzo 2013). They primarily record the geochemistry of the impacted material and can thus exhibit considerable compositional variation. With large impacts, some material may be ejected into the atmosphere, where they rapidly cool and vitrify before falling back to Earth hundreds or even thousands of kilometres from the impact site -these are known as tektites (Osinski and Pierazzo 2013). Tektites, as micro-fragments in deep-sea deposits, have been identified in the southern Caribbean (Barbados), marking the southernmost extent of the North-East American tektite field [START_REF] Glass | North American tektites and microtektites from Barbados, West Indies[END_REF]. Certain rocks discovered in Haiti could also be linked to a meteorite impact, one that occurred around the Cretaceous-Tertiary transition and was responsible for the Chicxulub crater in the Yucatan. However, this interpretation remains contentious [START_REF] Jéhanno | The Cretaceous-Tertiary boundary at Beloc, Haiti: No evidence for an impact in the Caribbean area[END_REF][START_REF] Kring | Petrogenesis of an augite-bearing melt rock in the Chicxulub structure and its relationship to K/T impact spherules in Haiti[END_REF], and in any case, these rocks are way too small to be used for knapping. The recent discovery of a new field of tektites of andesitic composition in Belize, referred to as "belizites", shakes things up: the largest of these tektites can form nodules a few centimetres in diameter (Rochette et al., 2021 figure 2).

In this article, we present the first-ever identification of archaeological stone tools made of natural glass coming from several archaeological sites in Guadeloupe and Dominica. A thorough description of these artefacts is proposed, as well as geochemical and mineralogical characterization combining several analytical techniques.

Most of these artefacts being vitreous andesite, major questions have been raised about their geological and geographical origin. As one of the artefacts was made of obsidian, we collected a sample of rhyolitic glass that had been identified in the eastern part of Guadeloupe to determine whether it was the source material used. Based on the detailed characterization achieved, we are investigating the origin of this hitherto unknown raw material and its distribution in several archaeological sites from the Ceramic Age.

Material and methods

For the sake of reproducibility and transparency, note that we use throughout the text the MeRIT system as per Nakagawa et al. ( 2023): initials of authors, but also of acknowledged people, are used to precisely identify individual contributions.

Archaeological artefacts

Nineteen archaeological artefacts from eight Ceramic Age sites, made of natural glass, were identified in the literature (Table 1 and Figure 1). We were able to access and scrutinise sixteen of these (Figure 2). Most of them come from development-led archaeology and were initially identified thanks to the vigilant efforts of CS in monitoring grey literature sources.

Figure 1 Map indicating the locations of the archaeological sites from which the artefacts originate, and the locations of the geological deposits that have been sampled (Guadeloupe and Puerto Rico) or are scheduled for sampling but already used as comparative data (Martinique). SJB and MGCT02 are located on the same spot as the sites are only a few tens of metres apart.

108 1 List of archaeological and geological sites with volcanic glass artefacts or glassy geological samples (+: yet to be confirmed) and their location. Bis-05 and MGCT02-3 were inventoried but are now lost. PSF-1 was analysed in PIXE but is now lost. SJB-1 could only be analysed by pXRF during a preliminary study and could not be brought to the laboratory for logistical reasons. Out of the nineteen artefacts, seventeen originate from archaeological sites situated in Guadeloupe. Bisdary is "located at an elevation of 100 metres on the foothills of the Caribbean Mountains, 1 kilometre from the sea" (Romon 2004). This site underwent surveying in 2004 and subsequent excavation in 2006 revealing the remains of a Cedrosan Saladoid site dating back to approximately 500-800 cal. AD. In addition to its unique geographical location, quite far from the shore for this period, this site yielded five archaeological objects recorded as being made of "obsidian" (of which only four were found in the curated collection so far) (Fouéré 2006, p.34). The site of Tourlourous, located near the southwestern shore of Marie-Galante, is also attributed to the Cedrosan Saladoid [START_REF] Colas | Document final de Synthèse INRAP[END_REF]. Seven archaeological artefacts made of natural glass were identified during the excavation, and were analysed in 2007 in a preliminary project, but we only recovered six of them during our recent study. Excavated in the adjacent parcel of Tourlourous in 2014, the Stade José Bade is considered to be part of the [START_REF] Gagnepain | Première approche du site de Caille-à-Bélasse[END_REF].

Artefacts from archaeological sites

Two artefacts were discovered outside Guadeloupe. One was unearthed 20-30 cm below the surface by IS, in the site called Delices 3, on the southwest coast of Dominica (Shearn 2014, p.318). It is attributed to a Cedrosan Saladoid occupation. Additionally, there's a "small reduced core" designated as "obsidian" at the Mill Reef site (Antigua) (Murphy 1999, p.208) which could not be included in the present study. It is worth noting that there are mentions of other volcanic glass in the literature, but it seems that these are all misidentifications. A blade from the Maruca site in Puerto Rico was described as obsidian [START_REF] Febles | Informe de análisis tecnotipológico del material lítico, sitio arqueológico Maruca[END_REF]; Rodríguez Ramos 2013) despite being identified initially as black chalcedony (Rodriguez 2001) and subsequently confirmed as such (Rodriguez-Ramos, comm. pers.to AQ 2020). In Martinique, a report on the Early Saladoid site of Fond-Brûlé listed nine "volcanic glass" artefacts (Mattioni, 1982). However, upon a thorough examination of the complete archaeological collection, this identification can be discarded, since every artefact photographed in the report has been found in the curated collection, and there is not a single volcanic glass artefact (black jaspers and flints are present).

All the sixteen studied artefacts are small flakes and nuclei originating from bipolar percussion technique (Figure S1), as already noted by [START_REF] Fouéré | Étude du mobilier lithique, In Gourbeyre « Bisdary[END_REF] for those found in Bisdary site. They do not differ significantly from artefacts made of other raw materials in the respective sites. Technical drawings and surface views from the 3D models acquired by microtomography are presented in Supplementary Information (Figure S1 and S2) to support this interpretation.

Finally, it must be noted that AQ conducted a survey of the Caribbean archaeological community by email and during the IACA 2022 congress. None of the respondents (see Acknowledgements) never saw a single black vitreous artefact during their career in the Caribbean islands, and no participant of the conference came forward either to say so.

Geological volcanic glass

Volcanic glass worldwide is mostly of rhyolitic composition and is referred to as obsidian. Rhyolitic rocks are very scarce in the Lesser Antilles, with only three to four occurrences with no description of obsidian [START_REF] Smith | The Lesser Antilles-a discussion of the island arc magmatism[END_REF]Le Guen de Kerneizon et al. 1982). The only described obsidian, dated to 325 ka, is located in the Volcan du Tuf area (Basse-Terre, Guadeloupe) and consists of a brecciated dyke containing perlitic obsidian originating from maar eruptive activity [START_REF] Gadalia | La chaîne volcanique de Bouillante, Basse-Terre de Guadeloupe, (Petites Antilles) : Identité pétrographique, volcanologique et géodynamique[END_REF]. Our fieldwork enabled us to identify the location of this obsidian source in the commune of Vieux-Habitants (Basse-Terre, Guadeloupe), on the edge of the Volcan du Tuf maar (Table 1). Several samples were taken, all with very poor knapping qualities (Figure S3).

A lone obsidian block from Puerto Rico is known to exist, having been discovered by a local worker while clearing a drainage ditch beside the PR 191 road in the El Yunque national forest (Walker pers. com. to AQ 2022). Despite additional fieldwork conducted in the area, no other blocks matching this description were located (Knippenberg pers. com. to AQ 2022). Regrettably, the precise geological origin of this high-quality obsidian block, provided by JW and SK, therefore remains unknown. While there is documented evidence of a silicic suite in the northeastern Antilles, primarily dating back to the Albian age (113.0 ± 1.0 Ma to 100.5 ± 0.9 Ma), and found in Puerto Rico and the Virgin Islands [START_REF] Jolly | Bimodal volcanism in northeast Puerto Rico and the Virgin Islands (Greater Antilles Island Arc): Genetic links with Cretaceous subduction of the mid-Atlantic ridge Caribbean spur[END_REF], the composition of these rocks, predominantly rhyolites, does not align with that of our sample (ObsPR). Even though these Albian rocks have likely undergone significant devitrification due to their age, this observation underscores the capacity of the tectonic conditions in this particular region of the Antilles to generate high-silica rocks similar to the ObsPR sample analysed in this study.

In addition to our search for obsidian from the Volcan du Tuf, we carried out a prospecting campaign in the Guadeloupe archipelago to locate vitreous andesitic material. Based on data from the geological map and indications from local prospectors, we identified and collected three deposits of glassy andesitic rocks trapped in ash deposits in the Capesterre river and at the estuary of the Grand-Carbet river (Capesterre-Belle-Eau, Basse-Terre, Guadeloupe) and at Bois Joli (Terre-de-Haut, Saintes archipelago, Guadeloupe) (Table 1). Unfortunately, none of these deposits contained glassy rocks massive enough to be knapped and potentially matching the material of the studied artefacts.

Methods

All samples underwent macroscopic and binocular observations. The various methods of analysis applied to each sample are reported in Table 1. The artefact from Stade José Bade (SJB) could only be analysed by portable X-Ray Fluorescence (pXRF) because it remained in Guadeloupe. This pXRF analysis confirmed its andesitic composition.

AQ conducted binocular observations using a Leica Z16APO to observe the texture and the structure of samples, as well as the distribution of phenocrysts. Photographs were taken with a Leica Flexacam C1 camera and the LAS X 5.0 software.

LBG and CL performed non-destructive elemental analysis by Particle-Induced X-ray Emission (PIXE) on the AGLAE facility [START_REF] Calligaro | Ion beam analysis with external beams: Recent set-up improvements[END_REF] using the procedures presented in [START_REF] Bellot-Gurlet | A PIXE/fissiontrack dating approach to sourcing studies of obsidian artefacts in Colombia and Ecuador[END_REF].

AL and AQ observed and analysed the artefacts by Scanning Electron Microscope (SEM) coupled with Energy Dispersive Spectroscopy (EDS) in a JEOL IT500HR electron microscope (FEG source). The SEM images and EDS spectra were acquired without carbon coating, in a low-vacuum mode (here 40 Pa). The images were acquired with a backscattered electron detector, while the EDS analysis were performed with two Oxford Ultimax 100 detectors at 20 kV for 30 s, producing spectra with 4.0 -4.5 million counts.

AL conducted an analysis of the artefacts and geological samples using Energy Dispersive X-Ray Fluorescence (ED-XRF) on a Hitachi SEA 6000vx device. This device is equipped with a rhodium source (50kV/1mA) and a Vortex SDD detector, and a specialised protocol was developed specifically for the study of silica-rich archaeological artefacts (Leck et al. 2018;Leck 2022). The PCA was carried out using CoDaPack software [START_REF] Comas | CoDaPack 2.0: a stand-alone, multi-platform compositional software[END_REF]. The data were prior transformed by a centred log ratio transformation [START_REF] Aitchison | The Statistical Analysis of Compositional Data[END_REF].

Four micro-samples were prepared for Electron Microprobe Analyses (EPMA) and Laser Ablation -Inductively-Coupled Plasma -Mass Spectrometry (LA-ICP-MS) analyses by AQ. EPMA and LA-ICP-MS analyses were only conducted on a very limited selection of samples: three of them were cut with a wire saw (Well3500) and epoxy resin (Araldite 2020): two from two rather big archaeological artefacts for which the shape would not be altered by the sampling (BIS-03 and MGCT02-06), one from the natural glass from Puerto Rico. Several glass fragments from Volcan du Tuf were also impregnated in epoxy resin. All samples were abraded with silicon carbide discs and polished with diamond paste. We obtained the official authorization of cutting small sub-samples from both archaeological artefacts via the French Ministry of Culture.

EPMA and LA-ICP-MS were conducted to obtain accurate geochemical composition of both major, minor and trace elements. JL determined the major-element compositions of the glasses by EPMA analysis using a Cameca SX100 from the Microsonde Ouest platform using wavelength dispersive spectrometers at 15 KV accelerating voltage, 10-12 nA beam current, and a spot size ranging from 10 to 20 µm. Minerals (wollastonite

[Si, Ca], orthoclase [K], albite [Na], apatite [P]), oxide (MnTiO3 [Mn, Ti]), Al2O3 [Al], Fe2O3 [Fe], Cr2O3 [Cr], FeS2 [S], etc.
), and metal standards (Ni) were used for calibration. In order to avoid the heterogeneity effects induced by small crystals or inclusions, the compositions of the glasses given here are averages of 2 to 6 analyses depending on the sample. BG performed the LA-ICP-MS measurements using a Thermo Fisher Scientific ELEMENT XR mass spectrometer with a linear dynamic range of twelve orders of magnitude thanks to the combination of a Faraday detector and a dual-mode SEM detector. The laser was a Resonetics M50E excimer laser operating at a wavelength of 193 nm, 5mJ and a repetition rate of 10 Hz. The sampling cell is flushed with an argon/helium glass flow of 1 l/min Ar + 0.65 l/min He. The analytical protocols followed are those typically employed for the analysis of glass [START_REF] Gratuze | Glass Characterization Using Laser Ablation-Inductively Coupled Plasma-Mass Spectrometry Methods[END_REF], which include a pre-ablation time of 20 seconds and the acquisition of 9 mass scans for 58 elements. Trace elements data were normalised to N-MORB [START_REF] Gale | The mean composition of ocean ridge basalts[END_REF]) and normalised to chondrite [START_REF] Barrat | Geochemistry of CI chondrites: Major and trace elements, and Cu and Zn isotopes[END_REF].

AQ performed micro-Raman spectroscopy analysis on phenocrysts located inside the devitrifications centres in several samples with a Bruker SENTERRA Raman microspectrometer equipped with a 532 nm laser, and a 1200-line diffraction grating resulting in a resolution of 3 to 5 cm -1 , after cleaning the samples with hydrogen peroxide and ultrasonic bath. Spectra were interpreted using the RRUFF database [START_REF] Lafuente | The power of databases: the RRUFF project[END_REF].

Before micro-sampling for EPMA and LA-ICP-MS, 3D reconstruction of the surface and the inner structure of the samples was realised by NV via X-ray microtomography using a GE VTOMEX-S 240/180. Depending on the size of the artefacts and on the fact that they would suffer or not the microsampling for geochemical analysis, the microscan performed have variable resolutions between 6 and 21 µm 3 per voxel. AQ extracted isosurfaces from these 3D models using the Avizo software.

Results

The andesitic artefacts consist of a matrix that is entirely translucent, with a slight brownish-orange hue (see Figure 2). A perlitic structure is evident across all pieces, suggesting quenching, as this is the most likely way this material with this chemical composition formed naturally. A few phenocrysts of various morphologies can be observed on the surface: some are bi-pyramidal, showing fluidity and probably resulting from crystallisation in the magma chamber or chimney, others are definitely devitrification spherules (Figure 2, S4, and S5). Some pieces exhibit significant vesiculation, with vesicles accounting for approximately half the volume of certain pieces (Figure S4). Microtomography scanning reveals that these vesicles are of various types, sizes, shapes and orientations (Figure S6), signifying different degassing and solidification events. Lastly, the size of the artefacts and the occasional presence of cortical surfaces lead us to estimate that the original blocks were likely rounded and had a diameter of approximately five centimetres. It is also conceivable that these blocks were likely collected in a primary or sub-primary position, possibly within an ash layer, as the cortical surfaces show no signs of erosion caused by transport.

The rhyolitic artefact, in contrast, features a dark grey vitreous matrix with a banded texture highlighted by submillimetric phenocrysts of feldspar (Figure S4). The perlitic structure is remarkably prominent, to the extent that it probably hindered the development of a useful conchoidal fracture for knapping.

Non-invasive techniquesto ensure the conservation of these rare artefactswere used on most samples to assess the homogeneity of the collection. SEM-EDS and PIXE data showed a very homogeneous glass composition and revealed the andesitic composition of most samples (Figure 3, Table S1 &S2). ED-XRF analysis confirmed the overall high homogeneity among trace elements for the archaeological andesitic artefacts and the close proximity of the rhyolitic artefact with the Volcan du Tuf source, as PIXE already did in the initial study (Figure 4 and Table S1, S3 & S4). Andesites containing vitreous phases sampled in Guadeloupe do not match the archaeological artefacts' composition. SEM-EDS analysis detected plagioclase feldspar and rare Fe-Ti oxides.

It revealed the fibrous structure of plagioclase feldspars within voids (Figure S7), likely formed due to matrix devitrification. These spherulites displayed bow-tie and spherical shapes. Their alignment is probably due to the original alignment of crystallisation nuclei in fluidal planes (Figure S4). Raman spectroscopy (Figures S5) confirmed the identification of most crystals as labradorite, indicating their formation in fluidal planes likely occurred within the magma chamber prior to the eruption, rather than through devitrification, due to the low calcium concentration of the obsidian. It also identified the presence of augite, cristobalite, and quartz in the clusters or lines of minerals. Based on these non-invasive results and in order to obtain high accuracy measurements from these surprising artefacts and potential sources, we conducted EPMA and LA-ICP-MS analysis (Table 2). The homogeneity and the andesitic nature of the archaeological was confirmed, as well as the rhyolitic composition of both nonarchaeological glass (Figure 3). The homogeneity of the two archaeological artefacts is incredibly high, for all the major and trace elements that we were able to measure (51 in total), clearly indicating that these two artefacts, unearthed from two different archaeological sites, originate from the same volcanic event, probably from the andesitic volcanism of the central Lesser Antilles subduction context (Figure 5). On the other hand, the trace elements and REE spectra suggest an origin from an andesitic volcanism that could be related directly to central Lesser Antilles context like the andesites from the northwestern part of Martinique, where the Mont Conil and the Montagne Pelée have been sampled (Figure 5). Other andesitic rocks from the region have been sampled and analysed previously [START_REF] Labanieh | Géochimie de l'île de la Martinique aux Petites Antilles[END_REF][START_REF] Germa | The K-Ar Cassignol-Gillot technique applied to western Martinique lavas: a record of Lesser Antilles arc activity from 2 Ma to Mount Pelée volcanism[END_REF][START_REF] Howe | Evolution of young andesitic-dacitic magmatic systems beneath Dominica, Lesser Antilles[END_REF][START_REF] Fedele | Petrological insights on the last 1000 years of explosive activity at La Soufrière volcano, St. Vincent (Lesser Antilles)[END_REF]) and if the general shape of the diagram is similar, the absolute values do not match the results from the archaeological artefacts (Figure S8). There is apparently a large enough variability in trace elements and REE in the Lesser Antilles context, between islands, and between periods of volcanic activity, to propose a potential provenance of the archaeological material from Martinique. The samples of rhyolites (ObsPR and VolcanTuf) exhibit typical compositions of differentiated volcanic rocks, such as a negative anomaly in Eu. However, it can be observed that these two rocks are not derived from the same type of magma. The Puerto Rico obsidian is low in alkaline earth elements and does not display anomalies in Nb and Ta, which may indicate a significant contribution from the oceanic crust in the formation of the magma during subduction [START_REF] Briqueu | Quantification of Nb, Ta, Ti and V anomalies in magmas associated with subduction zones: petrogenetic implications[END_REF][START_REF] Jolly | Bimodal volcanism in northeast Puerto Rico and the Virgin Islands (Greater Antilles Island Arc): Genetic links with Cretaceous subduction of the mid-Atlantic ridge Caribbean spur[END_REF]. The composition of the obsidian from the Volcan du Tuf corresponds, in turn, to the ultimate term of a tholeiitic arc series, as previously suggested by [START_REF] Gadalia | La chaîne volcanique de Bouillante, Basse-Terre de Guadeloupe, (Petites Antilles) : Identité pétrographique, volcanologique et géodynamique[END_REF].

Discussion

The results presented here introduce, for the first time, fragments of glassy material found in several archaeological sites from the Ceramic Age in the Caribbean islands. These eighteen elements were discovered within an area of only a 50 km radius. Our extensive review of the literature and survey of the Caribbean archaeologist community has confirmed that these are the only artefacts of this kind currently known. The thorough analysis of these objects, from both an archaeological and geological perspective, aims to document them and bring them to the attention of the community. It also sought to determine their origin, as this type of material is traditionally used in archaeology to study the mobility of materials, people, and exchange networks. Two different materials have been identified in this archaeological corpus: obsidian sensu stricto and vitreous andesite, a material hitherto unknown.

A single obsidian artefact

Obsidian sensu stricto is a vitreous volcanic rock, oversaturated with silica and typically of rhyolitic composition [START_REF] Tuffen | Obsidian[END_REF]. While all the archaeological samples from this study were initially recognized as such on the field, their geochemical analysis using PIXE yielded unexpected results by unveiling the presence of a single rhyolitic sample within the corpus. These findings were subsequently confirmed through the application of other analytical techniques. The RRC-01 sample sets itself apart from other glassy artefacts in our study due to its distinct geochemical composition and its dark grey coloration (Figure 3 and4). The combination of its chemical profile and macroscopic features strongly suggests it originates from the Volcan du Tuf, the sole known rhyolitic volcano in Guadeloupe, situated at a mere distance of less than 2 kilometres from the archaeological site where it was unearthed.

Despite its uniqueness in the archaeological record, this artefact provides valuable insights. It attests the choice of experimenting with local materials, when the knappable lithic raw materials in Guadeloupe are scarce. The low knapping quality of this obsidian underscores the Early Ceramic Age inhabitants' ability to work with relatively poor-quality raw materials. Although most of the lithic tools produced in the Lesser Antilles are based on good quality flint from Antigua, jasper from several islands and radiolarite from La Désirade (van Gijn 1993; [START_REF] Knippenberg | Stone artefact production and exchange among the Lesser Antilles[END_REF][START_REF] De Waal | On the reconstruction of prehistoric social territories: The La Désirade lithic workshops and the distribution of La Désirade chert (French West Indies)[END_REF]Queffelec et al. 2023). Interestingly, they decided to produce some flaking products with a poor quality material, while they could have used this shiny and unique material to produce other kind of artefacts such as the diverse beads or pendants they used to produce, including some rare black ones [START_REF] Brock | Dark materials: Pre-Columbian black lithic carvings from St Vincent and the wider Caribbean[END_REF]Queffelec et al., 2020). We think that this novelty could be related to the exploration of yet uncharted areas of the islands, as Early Ceramic occupations are predominantly coastal, at least as evidenced by the archaeological record [START_REF] Stouvenot | Recherche des occupations précolombiennes dans les hauteurs de Capesterre-Belle-Eau (Guadeloupe) : résultats préliminaires[END_REF].

While it is possible that this particular raw material may never be encountered again in any other archaeological site, our work has established a geochemical reference for both a plausible source of volcanic glass in the Caribbean islands and for the artefact. Furthermore, the search for the source of this artefact has allowed us to discover the existence of a likely obsidian deposit in Puerto Rico, analyse a sample from it, and thereby provide a reference for the composition of this obsidian. This may prove highly valuable for future provenance studies if similar materials are uncovered in the Caribbean again.

Andesitic glass artefacts

The confirmed andesitic glass artefacts were recovered in a 50 km radius area, where the southern site is located on the southeast coast of Dominica and the northernmost site is located in the southern half of the island of Basse-Terre (Guadeloupe). If the artefact from Mill Reef (Antigua) were to be confirmed, it would significantly modify the geographical extent even if keeping it constrained to the central Lesser Antilles. Apart from two exceptions, they were all recovered in Early Ceramic context. Two samples originate from an archaeology dig at the Caille à Bélasse site, on the Ilet de Petite Terre, which regrettably remains incomplete due to the passing of the excavator. This site, despite remaining unpublished, is considered to be Late Ceramic in age [START_REF] Gagnepain | Première approche du site de Caille-à-Bélasse[END_REF].

The technological analysis conducted on the artefacts connects them all to a chaîne opératoire using bipolar percussion techniques. They do not differ in this way from the artefacts made from other raw materials in the sites where they were unearthed and in many sites from this period [START_REF] Walker | Analysis and replication of lithic artifacts from the Sugar Factory pier site, St. Kitts[END_REF]Rodriguez Ramos 2001;[START_REF] Bérard | L'utilisation de la percussion sur enclume par les premières populations agro-céramistes des Antilles[END_REF]. It is therefore interesting to note that despite being a very unusual material, probably seen for the first time by the crafter, the method employed was exactly the same as with the jasper or the flint they usually knapped.

Given the poor quality of the material and the simplicity of the products, it seems unlikely that these rocks were part of an exchange network. They would therefore suggest that the same group was highly mobile within different islands of the Guadeloupe archipelago, Dominica and perhaps Antigua.

Despite intensive literature research and discussion with volcanologists, including glass specialists, and archaeologists specialised in obsidian, no such andesitic glass has been ever identified, neither in the Caribbean nor anywhere else in the world. This vitreous andesite, and its origin in particular, is thus of tremendous interest, both for archaeologists and geologists. There are two concurrent hypothesis: it was produced by volcanoes but never identified or studied by geologists, or it originates from an impact, and would therefore add to the list of meteoritic material used by people in the past, beside meteoritic iron in Arctic, Egypt or Europe [START_REF] Buchwald | On the use of iron by the Eskimos in Greenland[END_REF]Rehren et al. 2013;[START_REF] Comelli | The meteoritic origin of Tutankhamun's iron dagger blade[END_REF][START_REF] Hofmann | An arrowhead made of meteoritic iron from the late bronze age settlement of mörigen, Switzerland and its possible source[END_REF], and impactites, especially Libyan glass (e.g. Lull García 2014). Surprisingly, despite tektites being found in many archaeological sites, including some where obsidian was used as raw material for knapping, no mention of modified tektites has been found [START_REF] Hildebrand | Tektites found in the ruins of the Maya city of Tikal, Guatemala[END_REF][START_REF] Cornec | A layered tektite from the Central American strewn field[END_REF]Marwick et al. 2021).

The only mentions of naturally occurring andesitic composition glass we could locate all pertained impactites and tektites. Several rocks of this type exhibit significant similarities with our vitreous andesites: automorphic feldspars, originating from the pre-existing target rock of the meteorite impact, embedded within the perlitestructured impact glass (French, 1998, p.90), as well as closely related elemental compositions [START_REF] Izett | Tektites in Cretaceous-Tertiary boundary rocks on Haiti and their bearing on the Alvarez Impact Extinction Hypothesis[END_REF]: the chemical composition of the rock mainly copy the chemical composition of the impacted rock, it can therefore be glass of a very diverse range of compositions. Recently, a new field of tektites has been identified in Belize, of which unmodified elements have been found in some Mayan archaeological sites (Rochette et al. 2021). These rocks display elemental compositions quite similar to the andesites we are studying and are notably located in the Caribbean region. Several lithic materials found in the Caribbean islands already pointed to Central America, such as part of the jadeite jade celts [START_REF] Garcia-Casco | Pre-Columbian jadeitite artifacts from the Golden Rock Site, St. Eustatius, Lesser Antilles, with special reference to jadeitite artifacts from Elliot's, Antigua: Implications for potential source regions and long-distance exchange networks in the Greater Caribbean[END_REF][START_REF] Knaf | Trace-elemental and multi-isotopic (Sr-Nd-Pb) discrimination of jade in the circum-Caribbean: Implications for pre-colonial inter-island exchange networks[END_REF]) but also, as a working hypothesis, the green lapidary material sudoite, which could come hypothetically from Costa Rica [START_REF] Delvigne | Quels territoires en Préhistoire? Une analyse par réseaux de lieux pour penser l'espace au Paléolithique supérieur[END_REF]Queffelec et al. 2023).

We focused our efforts on investigating various indicators that could help us identify an extraterrestrial origin for these artefacts or, conversely, confirm a volcanic origin whose exact source might potentially be traced. Firstly, as mentioned earlier, the raw nodules were likely generally spherical, akin to many tektites. However, their dimensions would have approached approximately five centimetres in diameter, which is an exceptionally large size for tektites especially if they were far from the impact (Montanari and Koeberl 2000, p.58). Furthermore, the chemical composition of the artefacts, even though they could be derived from several blocks, is highly uniform. Moreover, no variation in the chemical composition of the glass is observed at the microscopic scale with the SEM-EDS (Table S2). This characteristic is more commonly shared by volcanic rocks than by impact glasses, whether tektites or impactites, which can exhibit significant heterogeneity [START_REF] French | Traces of catastrophe: A handbook of shock-metamorphic effects in terrestrial meteorite impact structures[END_REF]. Although some tektites can be relatively homogeneous (Rochette et al. 2021), their level of homogeneity is not comparable with what we observe here (Table S5).

No positive anomalies in chromium, cobalt, or nickel were observed, which are typically indicators of contamination by meteoritic material, frequently found in impactites [START_REF] Koeberl | The Geochemistry and Cosmochemistry of Impacts[END_REF]. The profiles of trace elements and rare earth elements are, in turn, consistent with arc volcanism, specifically aligning with recent volcanic activity in the central part of the Lesser Antilles (Figure 5) where the artefacts were recovered.

A volcanic origin therefore appears to be the most likely scenario. However, as of now, we have not been able to trace the exact source of this material. The distribution of artefacts suggests a probable origin in the southern part of the Guadeloupean archipelago. Yet, this may be influenced by the robust state of archaeology in Guadeloupe due to standard and development-led archaeology, compared to neighbouring islands. In 2021, we conducted a survey in this region, guided by a thorough review of geological literature, geological maps, and their descriptions. However, we did not find any vitreous andesite blocks; only porphyritic andesites were discovered, with a matrix that is largely vitrified but unsuitable for toolmaking. These rocks were analysed and their compositions do not fit with the same volcanic event (Table 1, Figure 4). Comparisons with rocks from Guadeloupe or Dominica revealed pattern similarities in the general, qualitative shape of trace and REE spectra, pointing to the possibility of finding such patterns in andesites originating from subduction in the region. It is only with rocks from northern Martinique that qualitative and quantitative very good fits were observed (Figures 1 and5). This region is particularly challenging to access, mostly uninhabited, and no surveys have been possible thus far. However, we plan to conduct explorations in the coming years to search for a source of vitreous andesite.

Another hypothesis that can be considered is that the original deposit has now vanished or is inaccessible. Indeed, erosion is quite pronounced in this tropical climate, where raining events can be important and even catastrophic in case of hurricanes. The deposit of these highly distinctive vitreous andesites is, or was, almost certainly very limited and may have been eroded. Additionally, the region experiences very active volcanic activity, and large portions of the land available to Early Ceramic inhabitants have been covered by recent eruption products. The fact that almost all artefacts were unearthed in sites dated to the Early Ceramic period may indicate that the source disappeared around 500 CE. Recent volcanic eruptions on the islands of Guadeloupe, Dominica and Martinique are well known and may have covered the potential source, as for example the well-known P2 Plinian eruption, dated to 280 AD, which entirely covered archaeological sites in Martinique, like the site of Vivé, under a few cm of dilute pyroclastic flow deposits overlain by 10 to 50 cm of pumice fallout deposits [START_REF] Carazzo | Marginally stable recent Plinian eruptions of Mt. Pelée volcano (Lesser Antilles): the P2 AD 280 eruption[END_REF].

Conclusion

We present here the first identification of natural glass artefacts in the Ceramic Age context in the Caribbean Islands. One among these samples is identified as obsidian sensu stricto, for which the origin is the Volcan du Tuf, located near the archaeological site, on the Western part of Basse-Terre island in Guadeloupe. This raw material, despite its bad quality for knapping, seems to have been attractive for inhabitants of Guadeloupe during the Early Saladoid, with which they produced at least a small flake by bipolar percussion, as they usually do with other raw materials. Looking for the obsidian sources in the Caribbean islands led us to identify an obsidian deposit in Puerto Rico, which does not appear to have been utilised by any population because of its current absence in the archaeological series. The deposit is only known through secondary sources but provides a massive and impurity-free material of very good quality for crafting. We provide here a geochemical reference framework that will make it possible to properly identify this material if it is ever found in an archaeological site. We present a geochemical reference framework here that will enable the proper identification of this material if it is ever found at an archaeological site.

The other artefacts have been identified as vitreous andesites, which are highly atypical rocks whose origin is a real challenge to identify. While a formation related to a meteorite impact has been extensively considered, our observations and analysis lead us to favour the hypothesis of a volcanic origin. Geochemical similarities with volcanic deposits from Martinique demonstrate that the volcanism from the central part of the Lesser Antilles could produce andesitic lava of such a composition. However, despite geologists' work conducted in Guadeloupe and Martinique for decades, and despite some field surveys in Guadeloupe, we have not been able to locate the original deposit or even find a few secondary vitreous andesites. Therefore, we seriously consider the possibility that the source, if it was located in Guadeloupe or Martinique, could now be lost, perhaps covered by more recent volcanic deposits. Additional field surveys on the Northwestern coast of Martinique might be interesting to organise in the future. The thorough mineralogical and geochemical description of the artefacts will allow to easily connect any new discovery of artefacts or raw material to these samples.

Surveying the literature and the community of archaeologists in the Antilles, we confirmed that the use of volcanic glass is extremely rare and that, outside the Guadeloupean artefacts, currently only one artefact is confirmed in Dominica and one still needs to be confirmed in Antigua. This constrained geographical distribution allows us to make the hypothesis that the source material would be located in Guadeloupe or a neighbouring island. While we have not yet identified the original source of these vitreous andesites, this study allows us to include this material in the limited list of materials discovered in Antillean archaeological sites for which provenance can be traced. The list is currently rather short and is composed of the Antiguan flint, the St. Martin calci-rudite and cherto-tuffite, and the numerous lapidary raw materials. By adding two new geochemically fingerprinted raw materials to this list, this study may facilitate future endeavours to determine the provenance of similar artefacts and help reconstruct the litho-spaces of different sites [START_REF] Delvigne | Quels territoires en Préhistoire? Une analyse par réseaux de lieux pour penser l'espace au Paléolithique supérieur[END_REF]. It is only by conducting and combining the analysis of the techno-economical pattern of different litho-spaces of sub-contemporaneous sites that one can approach a dynamic vision of the structure and relations that existed during the Early Ceramic inhabitants of the Caribbean islands. 1).

Figure 2

 2 Figure 2 Macrophotographs of the sixteen glassy artefacts recovered from six archaeological sites.

Figure 3

 3 Figure 3 Total Alkali Silica (TAS) diagram (Le Maitre et al. 2005) illustrates the elemental composition measured using PIXE and EPMA on glassy archaeological and geological samples. All the artefacts, with the exception of one, consist of an unusual andesitic glass, while the geological samples are composed of obsidian, a more typical rhyolitic glass.

Figure 5

 5 Figure 5 Comparison of both archaeological artefacts, the two obsidian samples analysed by LA-ICP-MS, with Belizites (from Rochette et al. 2021, Pb is below detection limit in this analysis) and some andesites from northwest Martinique (from Labanieh, 2009, Tm are lacking in these analysis). A. N-MORB-normalised trace elements patterns. B. Chondrite-normalised REE patterns.

Figure

  Figure S2 Developed view of the surface of artefacts extracted from the 3D models from microtomography acquisitions prior to the microsampling of two samples. Acquisition by NV, Surface extraction and infographic by AQ

Figure

  Figure S4 Microphotographs of archaeological samples, showing perlitic texture in BIS-03 (A), the high quantify of crystals in RRC-02 (B), the quasi-absence of crystals in RRC-01 (C), and the planar distribution of crystals in CB051 (D), BIS-02 (E) and BIS-01 (F). Pictures and infographic by AQ

Figure S5- 2

 2 Figure S5-2 Raman spectra acquired on two different grains (colours of circle in picture is equivalent to colours of spectra) in the DEL-3-1 flake. Despite the measured spot size of a few microns, both spectra exhibit a mix of labradorite and augite.

Figure S5- 3

 3 Figure S5-3 Raman spectra acquired in clusters of grains on the BIS-04 and BIS-04 artefacts, showing the presence of quartz and cristobalite, as well as labradorite.

Figure S5- 4

 4 Figure S5-4 Raman spectrum acquired on a white nodule on the CB-050a artefact, showing the presence of both quartz and cristobalite in the same analysed spot.

Figure S5- 6

 6 Figure S5-6 Raman spectra acquired on several grains on the RRC-01 and RRC-02 artefacts, labradorite on the former, and of quartz and cristobalite in the later

Figure

  Figure S7 Plagioclase phenocrysts and fibrous feldspar spherules in the RRC-1, RRC-2, BIS-04 and CB050a samples (after H2O2 + ultrasound cleaning)

Samples from geological formations Sample Code Site City Island Longitude Latitude Type of rock SEM-EDS PIXE EPMA LA-ICP-MS ED-XRF

	MGCT02-1 DEL-3-1		Tourlourous Delices 3	Capesterre-de-Marie-Galante Marie-Galante Saint Patrick Parish Dominique	-61.224 -61.256	15.889 Early Ceramic 15.275 Early Ceramic Shearn, 2014 Colas, 2002		1.394 0.373	Flake Flake		X	X	X X	X	X X
	Sample Code MGCT02-2 SJB-1 MGCT02-3 PSF-1		Site Tourlourous Stade José Bade Tourlourous Place Saint François	City Capesterre-de-Marie-Galante Marie-Galante Island Capesterre-de-Marie-Galante Marie-Galante Capesterre-de-Marie-Galante Marie-Galante Basse-Terre Basse-Terre	Longitude Latitude -61.224 15.889 Early Ceramic Period -61.224 15.889 Early Ceramic Serrand, 2016 Bibliography Colas, 2002 -61.224 15.889 Early Ceramic Colas, 2002 -61.73 15.995 Early Ceramic Sellier-Ségard, 2001	Mass (g) 4.063 N.A.	Type Flake Flake Lost Flake (Lost)		X SEM-EDS	X PIXE EPMA X	LA-ICP-MS	X pXRF ED-XRF	X Raman	X Microtomo graphy
	Bis-01 Not MGCT02-4 Included Yet	Bisdary Tourlourous Mill Reef+	Gourbeyre Capesterre-de-Marie-Galante Marie-Galante Basse-Terre Saint Philip Antigua	-61.709 -61.224 -61.679	15.988 Early Ceramic Middle/Late 15.889 Early Ceramic 17.057 Ceramic	Romon et al., 2006 Colas, 2002 Murphy, 1999		1.312 2.792	Flake Nucleus Nucleus			X X	X X	X X
	Bis-02 MGCT02-5		Bisdary Tourlourous	Gourbeyre Capesterre-de-Marie-Galante Marie-Galante Basse-Terre	-61.709 -61.224	15.988 Early Ceramic 15.889 Early Ceramic	Romon et al., 2006 Colas, 2002		2.21 0.156	Flake Flake		X X	X X	X X	X X
	Bis-03 MGCT02-6		Bisdary Tourlourous	Gourbeyre Capesterre-de-Marie-Galante Marie-Galante Basse-Terre	-61.709 -61.224	15.988 Early Ceramic 15.889 Early Ceramic	Romon et al., 2006 Colas, 2002		4.318 16.896	Nucleus Flake			X X	X X	X X	X X	X	X X
	Bis-04 MGCT02-7 Volc.Tuf Bisdary Tourlourous	Gourbeyre Capesterre-de-Marie-Galante Marie-Galante Basse-Terre Volcan du Tuf	-61.709 -61.224 Vieux-Habitants 15.988 Early Ceramic 15.889 Early Ceramic Basse-Terre -61.734 Romon et al., 2006 Colas, 2002	2.367 2.682 16.051 Rhyolite Flake Flake	X	X X	X X X	X	X X	x	X	X	X X
	RRC-01 CB-050a Riv.Capesterre Rivière de Capesterre Ruelle Roches Caraïbes Baillif Caille à Bélasse Terre de Bas Est.Carbet Embouchure du Grand-Carbet Capesterre-Belle-Eau Basse-Terre -61.736 16.038 Early Ceramic Capesterre-Belle-Eau Basse-Terre Ilets de Petite Terre -61.11 16.17 Late Ceramic Gagnepain, 2007 Bonnissent & Chancerel, 2001 -61.609 16.072 Basse-Terre -61.574 16.021	2.733 Andesite Flake 0.901 Flake Andesite		X	X X	X X	X X	X X	X X
	BoisJoli	Bois Joli	Terre-de-Haut	Les Saintes	-61.609	16.072	Andesite			x
	RRC-02 CB-051a ObsPR Ruelle Roches Caraïbes Caille à Bélasse Yunque National Forest Baillif Basse-Terre Terre de Bas Ilets de Petite Terre	-61.736 -61.11	16.038 Early Ceramic 16.17 Late Ceramic Gagnepain, 2007 Bonnissent & Chancerel, 2001 Puerto Rico -65.777 18.299	5.504 Undetermined 0.299 Flake Rhyolite X	X X	X X	x	X X	X	X	X	X X
	Table
															6

  same site (Sellier-Segard and Casagrande 2016). One flake made of a similar glassy material has been found on the site, regrettably, it comes from levels containing a mixture of Cedrosan Saladoid and Troumassan Troumassoid artefacts. Place Saint François was excavated in 2001, just in front of the cathedral of Basse-Terre, and is interpreted as a Cedrosan Saladoid occupation(Sellier-Ségard 2001). Similarly, the Ruelle des Roches Caraïbes site, excavated in 2001, a few kilometres south of Volcan du Tuf, yielded two glassy artefacts from the Cedrosan Saladoid levels[START_REF] Bonnissent | Commune de Baillif. Rapport d'opération archéologique d'urgence AFAN[END_REF]. The Caille à Bélasse site is the only Late Ceramic site having yielded glassy artefacts. It is interpreted as a Troumassan Troumassoid settlement and located on the Ilets de Petite Terre in the southwestern part of the Guadeloupean archipelago

Table 2 .

 2 Major and minor elements composition measured by EPMA and trace elements abundances measured by LA-ICP-MS.For the andesitic archaeological artefacts, no enrichment in Cr, Ni, or Co are visible in the archaeological artefacts, indicating that no extra-terrestrial contamination can be suspected from this data[START_REF] Koeberl | Identification of meteoritic components in impactites[END_REF][START_REF] Koeberl | The Geochemistry and Cosmochemistry of Impacts[END_REF] Rochette et al. 2021).

	277
	EPMA	ObsPR VolcanTuf MGCT02-	BIS-03
	(%)			6
	SiO2	76,36	78,02	61,74	62,00
	TiO2	0,22	0,15	0,57	0,57
	Al2O3	11,54	12,58	16,94	16,99
	FeO	2,16	1,80	5,49	5,40
	MnO	0,12	0,06	0,13	0,12
	MgO	0,07	0,14	2,66	2,65
	CaO	0,11	1,51	6,87	6,72
	Na2O	4,92	4,22	3,35	3,48
	K2O	4,83	2,22	1,29	1,29
	P2O5	0,02	0,04	0,23	0,23
	SO2	0,03	0,02	0,01	0,00
	F	0,14	0,01	0,01	0,00
	Cl	0,20	0,24	0,06	0,06
	Total	100,72	101,01	99,35	99,51
	LA-ICP-MS	ObsPR VolcanTuf MGCT02-	BIS-03
	(µg/g)			6
	V	3.98	0.24	124	124
	Cr	0.31	0.48	8.54	8.57
	Co	0.02	0.88	12.9	13.8
	Ni	<LOD	0.33	4.51	4.59
	Cu	0.04	13.9	142	147

Table S4

 S4 Trace elements measured by ED-XRF on archaeological artefacts. 762 Table S5 Major element concentrations and compositional variability of vitreous rocks analysed in this study and tektites from different strewn fields, particularly belizites. According to Rochette et al. (2021, Table

	759 761
		CB-050a BIS-02 BIS-04 3.5 2.7 1 CB-050a 3.7 2.8 MGCT02-MGCT02-MGCT02-RRC-01 4.5 0.1 Volc.Tuf 882 21571 CB-051a 1802 68212 MGCT02-04 1629 61497	61.46 17.01 17.4 62.7 17.9 63.2 12.8 77.6 35 11 68 16 37 45 70 15 34	5.38 1.2 1.1 1.9 246 114 0.12 6.3 5.8 1.3 22 223 20	5.64 0.6 0.5 0.1 42 91 81	3.07 163	1.07 20 19 0.1 0.1 0.1 17	0.49 5.4 4.7 1.4	57	17	81	202	91
		polished 02 06 polished	Na2O 3.0 2.6 MgO 3.4 2.7 3.5 2.7 3.2 2.6 MnO Fe2O3 MnO Fe2O3	Al2O3 17.2 17.3 17.5 17.2 Zn Zn	SiO2 62.5 62.6 62.8 62.4 Ga Ga	Rb Rb	1.2 1.2 1.1 1.2	CaO 6.7 6.3 6.2 6.6 Sr Sr	Y Y	TiO2 0.6 0.5 0.5 0.6 Zr Zr	MnO 0.1 0.1 0.1 0.1 Nb Nb	Fe2O3 6.0 5.6 5.3 5.9 Pb Pb
	756	Table S1 Compositions measured in 2007 by PIXE on archaeological artefacts and a geological sample from the Volcan du Tuf. (%) (%) (%) K2O (%) (%) (%) (%) (%) 3.6 2.7 (%) 17.5 63.1 1.1 6.1 0.5 0.1 5.0 3.4 2.7 17.5 62.6 1.2 6.2 0.5 0.1 5.4 4.3 0.1 12.9 76.8 1.9 1.6 0.1 0.1 1.8 (µg/g) (µg/g) (µg/g) (µg/g) (µg/g) (µg/g) (µg/g) (µg/g) (µg/g) (µg/g) 1003 23981 38 12 50 131 48 194 23 (µg/g) Sample BIS-02 BIS-04 DEL-03-1 MGCT02-MGCT02-MGCT02-RRC-01 Sample Volc.Tuf Sample (µg/g) (µg/g) (µg/g) (µg/g) (µg/g) (µg/g) (µg/g) (µg/g) (µg/g) DEL-03 1697 64528 70 16 35 227 22 84 19 MGCT02-04 1613 61317 64 13 33 219 19 81 17
		BIS-01 polished 02 06 polished BIS-04 DEL-03-1 RRC-01 BoisJoli1 Volc.Tuf BIS-01 DEL-03 MGCT02-05 1521 553 16498 3.5 2.7 3.4 2.8 3.5 2.7 3.5 2.7 3.1 2.7 3.5 2.7 3.4 2.7 4.8 0.1 798 19817 1514 57634 1604 60521 58075	17.4 17.5 17.4 17.5 17.4 17.3 17.6 12.8 45 32 52 63 52	12 13 13	62.6 62.8 62.4 62.8 62.7 63.2 62.5 76.3 21 12	19 42 30 33 31	1.1 1.2 1.2 1.1 1.2 1.1 1.2 2.0	6.3 6.3 6.4 6.2 6.5 6.2 6.3 1.5 305 130 203 19 212 20 204 19	18 40	0.5 0.6 0.6 0.5 0.5 0.5 0.5 0.1 76 79 77	100 149	0.1 0.1 0.1 0.1 0.1 0.1 0.2 0.1 17 18 17	19 20	5.3 5.6 5.3 5.7 5.5 5.0 5.5 1.9
		BIS-01 BIS-03 BIS-04 DEL-03-1 MGCT02-02 MGCT02-06 MGCT02-polished RRC-01 BoisJoli1 Volc.Tuf BIS-01 DEL-03 MGCT02-06 1572 892 23696 3.5 2.7 3.5 2.7 3.4 2.2 3.4 2.7 3.8 2.8 3.6 2.7 2.7 2.5 4.6 0.1 1173 28389 1516 58066 1639 62521 59431	17.6 17.5 15.2 17.5 17.7 17.5 16.9 12.7 64 37 51 65 60	12 15 14	62.7 62.9 64.4 62.4 63.4 62.9 62.4 76.9 20 11	23 43 31 33 32	1.2 1.1 1.2 1.2 1.1 1.1 1.2 2.0	6.3 6.2 5.6 6.3 5.8 6.1 7.0 1.4 253 106 204 19 220 21 210 19	20 43	0.5 0.5 0.9 0.5 0.5 0.5 0.6 0.1 76 82 77	110 179	0.1 0.1 0.2 0.1 0.1 0.1 0.1 0.1 16 18 16	20 20	5.3 5.3 6.6 5.6 4.7 5.2 6.5 1.7
	760	BIS-01 BIS-03 BIS-04 DEL-03-1 MGCT02-MGCT02-MGCT02-RRC-01 BoisJoli1 BIS-02 DEL-03 MGCT02-06 1615 1543 34378 3.5 2.7 3.6 2.7 3.4 2.7 3.4 2.7 3.4 0.2 Table S3 Trace elements measured by ED-XRF on geological samples. 17.6 62.7 1.1 6.2 0.5 17.4 62.7 1.1 6.2 0.5 17.5 62.6 1.2 6.4 0.5 17.7 61.8 1.2 6.3 0.5 13.0 77.3 1.9 1.5 0.3 72 19 27 252 25 127 1658 62582 65 13 34 220 20 82 1575 60149 57 13 32 211 19 78 61752 64 16 34 224 20 82	0.1 0.1 0.1 0.1 0.1 17 17 17	20	5.3 5.3 5.4 5.7 2.0
		02 06 07	3.7 2.8 3.6 2.7 3.5 2.7	17.6 17.4 17.4		63.2 62.5 62.6		1.1 1.1 1.1	5.9 6.3 6.3			0.5 0.5 0.5			0.1 0.1 0.1	4.9 5.4 5.5
		BIS-01 BIS-03 BIS-04 DEL-03-1 RRC-01 BoisJoli1 BIS-02 RRC-01 MGCT02-06 1522 525 18725 3.5 2.7 3.8 2.8 3.4 2.7 3.4 2.7 4.2 0.1 1732 65767 886 22406 57965	17.5 17.4 17.5 17.6 12.8 61 69 37 53	16 13 13	62.8 62.5 62.7 62.4 77.5 17	19 36 48 31	1.1 1.1 1.2 1.2 2.0	6.2 6.3 6.3 6.2 1.4 250 237 21 142 45 205 19	17	0.5 0.5 0.5 0.5 0.1 87 179 111 75	0.1 0.1 0.1 0.1 0.1 18 21 16	18	5.3 5.3 5.4 5.6 1.6
		MGCT02-MGCT02-MGCT02-
		BIS-02 BIS-03 BIS-04 MGCT02-02 polished 07 RRC-01 BoisJoli2 BIS-02 RRC-01 MGCT02-06 1572 575 19565 3.6 2.7 3.6 2.7 3.6 2.7 3.5 2.7 3.5 2.7 3.4 2.7 3.2 0.2 1644 63785 915 23305 59902	17.6 17.4 17.6 17.3 17.5 17.3 13.2 34 63 37 56	14 13 13	62.8 62.7 62.9 62.7 62.9 62.6 77.3 19	31 36 47 32	1.1 1.1 1.1 1.2 1.1 1.2 1.8	6.2 6.2 6.1 6.2 6.2 6.4 1.7 325 239 22 122 46 213 20	31	0.5 0.5 0.5 0.5 0.5 0.6 0.2 88 220 100 79	0.1 0.2 0.1 0.2 0.1 0.1 0.1 19 21 17	18	5.0 5.3 5.1 5.4 5.3 5.6 2.1
		01	3.5 2.7	17.6		62.9		1.1	6.1			0.5			0.1	5.2
		BIS-02 BIS-03 BIS-04 MGCT02-02 MGCT02-polished MGCT02-07 RRC-02 BoisJoli2 BIS-02 RRC-02 MGCT02-07 1691 2982 66435 3.2 2.7 3.5 2.7 3.6 2.7 3.5 2.7 3.4 2.6 3.5 2.7 3.3 2.7 1278 58544 1580 63696 64238	17.9 17.3 17.7 17.3 17.2 17.4 17.5 76 60 71 67	14 14 14	62.7 62.7 63.0 62.5 62.5 62.6 62.4 15	30 34 34 35	1.2 1.2 1.1 1.2 1.2 1.2 1.2	6.1 6.3 6.1 6.3 6.5 6.3 6.3 220 207 19 229 21 227 21	30	0.5 0.6 0.5 0.5 0.6 0.5 0.6 82 85 84		98	0.1 0.1 0.1 0.1 0.2 0.1 0.1 8 18 18	18	5.5 5.5 5.0 5.6 5.8 5.4 5.6
		MGCT02-
		BIS-02 BIS-03 BIS-04 01 MGCT02-MGCT02-MGCT02-RRC-02 BoisJoli2 BIS-03 RRC-02 MGCT02-07 1509 993 28943 2.9 2.6 3.7 2.8 3.6 2.7 3.6 2.7 3.3 2.6 1520 59139 1625 65392 56944	17.9 17.6 17.4 17.5 17.7 38 63 73 58	13 15 13	62.9 63.1 62.6 62.9 62.5 17	33 31 35 31	1.1 1.1 1.1 1.1 1.2	6.0 6.0 6.3 6.1 6.3 310 206 19 236 21 200 19	30	0.5 0.5 0.5 0.5 0.6 77 88 76	106	0.1 0.1 0.1 0.1 0.1 16 19 16	19	5.6 4.9 5.4 5.2 5.5
		02 polished 07	3.8 2.8 2.9 2.6 3.4 2.7	17.8 17.2 17.4		63.5 62.8 62.6		1.1 1.2 1.2	5.7 6.6 6.3			0.5 0.6 0.5			0.1 0.1 0.1	4.5 5.8 5.4
		BIS-02 polished MGCT02-MGCT02-RRC-01 BIS-04 CB-051a MGCT02-01 RRC-02 Est.Carbet1 BIS-03 RRC-02	3.5 2.7 4.6 0.1 3.5 2.7 3.6 2.7 3.5 2.7 3.2 2.6 1159 47658 1538 62115 1556 62200	17.3 12.7 17.5 17.4 17.6 17.6 31 73 70	14 15	62.7 77.4 63.1 62.8 62.5 62.0 13	17 33 33	1.1 2.0 1.1 1.1 1.2 1.3	6.4 1.4 6.2 6.2 6.2 6.5 252 217 20 223 20	22	0.5 0.1 0.5 0.5 0.6 0.6 82 83		74	0.1 0.1 0.1 0.1 0.1 0.2 17 18	15	1.5 5.5 5.1 5.3 5.5 6.0
		BIS-04 CB-051a MGCT02-02 polished RRC-02 Est.Carbet1 BIS-03 MGCT02-01 1502 982 42236 3.5 2.7 3.6 2.8 3.5 2.7 3.1 2.4 3.4 2.7 1508 60754 57323 BIS-02 polished 3.5 2.7 01 2.8 2.3 RRC-01 4.5 0.1 BIS-04 3.4 2.7 CB-051a 3.6 2.8 MGCT02-05 3.6 2.7 MGCT02-polished 3.0 2.6 RRC-02 3.4 2.6 Est.Carbet1 1322 56028 BIS-04 1580 60276 MGCT02-01 1531 58557	17.4 17.5 17.4 16.7 17.5 28 73 51 17.3 16.4 12.6 17.4 17.4 17.6 17.1 17.3 32 63 51	13 12 13 13	63.0 63.1 62.7 63.6 62.7 15 62.4 55.8 77.0 62.6 62.8 62.3 62.7 61.8 14	14 33 31 15 32 32	1.1 1.1 1.2 1.3 1.2 1.2 1.1 2.0 1.2 1.2 1.1 1.2 1.3	6.2 6.1 6.3 6.3 6.3 266 220 20 204 19 6.5 5.6 1.4 6.4 6.1 6.4 6.6 6.6 251 213 19 210 19	18 20	0.5 0.5 0.5 0.5 0.5 82 76 0.5 0.5 0.2 0.5 0.5 0.5 0.6 0.6 78 77		62 72	0.1 0.1 0.1 0.1 0.1 17 17 0.1 0.2 0.1 0.2 0.2 0.1 0.1 0.2 16 17	15 15	5.1 5.1 5.5 5.8 5.5 5.6 1.9 5.7 5.5 5.3 5.3 6.0 6.2
		BIS-02 polished BIS-04 CB-051a MGCT02-01 MGCT02-MGCT02-RRC-01 RRC-02 Riv.Capesterre 1 BIS-04 MGCT02-02 1663 2125 67503 3.3 2.6 3.5 2.7 3.5 2.7 3.6 2.7 4.3 0.1 3.5 2.0 1560 59883 62659	17.3 17.4 17.4 17.6 12.6 18.4 66 56 64	13 15	62.5 62.7 62.6 63.1 77.2 60.6 15	20 33 35	1.2 1.2 1.1 1.1 2.1 1.0	6.6 6.3 6.3 6.1 1.4 7.1 188 217 20 228 21	46	0.6 0.5 0.5 0.5 0.1 0.6 80 83	107	0.2 0.1 0.1 0.1 0.1 0.1 17 17	18	5.7 5.5 5.4 5.1 1.7 6.4
		BIS-04 MGCT02-05 polished RRC-01 CB-050a MGCT02-02 1536 1556 BIS-02 polished BIS-04 CB-050a 02 MGCT02-06 MGCT02-polished RRC-01 RRC-02 Riv.Capesterre 1745 66798 3.5 2.7 3.7 2.8 3.1 2.7 4.5 0.1 58582 58059 3.5 2.7 3.4 2.7 3.5 2.7 3.5 2.7 3.5 2.7 2.9 2.6 4.7 0.2 2.8 2.6 1 CB-050a 1544 58444 MGCT02-02 1514 57639	17.4 17.8 17.6 13.2 58 59 17.4 17.6 17.6 17.4 17.5 17.2 14.2 17.5 65 51 52	13 13 13 13	62.7 63.0 63.2 76.4 62.8 62.8 62.8 62.6 62.9 62.9 73.7 62.5 13	31 31 20 31 31	1.2 1.1 1.1 2.0 1.1 1.2 1.1 1.1 1.1 1.2 2.0 1.3	6.3 6.0 6.2 1.7 20 18 6.3 6.2 6.2 6.3 6.2 6.6 2.7 6.4 180 204 205 206 19 203 18	45	0.5 0.5 0.5 0.1 75 76 0.5 0.5 0.5 0.5 0.6 0.6 0.1 0.6 75 75	107	0.1 0.1 0.1 0.1 17 16 0.1 0.1 0.1 0.1 0.1 0.2 0.1 0.1 16 16	17	5.4 4.7 5.3 1.8 5.5 5.3 5.2 5.5 5.3 5.9 1.9 5.9
		CB-050a MGCT02-RRC-02 BIS-02 polished BIS-04 02 MGCT02-MGCT02-RRC-01 Riv.Capesterre 1 CB-051a MGCT02-04 1618 1736 66898 4.0 2.8 3.4 2.1 3.2 2.7 3.8 2.8 3.5 2.7 4.5 0.1 1489 56283 61878	17.3 18.7 17.4 17.8 17.4 12.8 65 50 75	11 15	61.9 60.9 62.7 63.5 62.7 77.4 14	20 30 34	1.2 1.0 1.2 1.1 1.1 2.0	6.3 6.7 6.4 5.8 6.3 1.4 182 200 18 222 21	46	0.5 0.6 0.6 0.5 0.5 0.1 74 82	107	0.1 0.1 0.1 0.1 0.1 0.1 16 18	18	5.1 6.3 5.6 4.5 5.4 1.4
		CB-050a 06 polished RRC-02	3.6 2.7 3.1 2.7 3.2 2.7 2.8 2.6	17.6 17.5 17.5 17.5		62.8 63.0 63.1 62.4		1.1 1.1 1.1 1.3	6.2 6.3 6.3 6.5			0.5 0.6 0.6 0.6			0.1 0.2 0.1 0.1	5.2 5.4 5.4 6.0
															50 51

Acknowledgments

We would like to thank Nicolas Vanderesse for the microtomography acquisitions, Yannick Lefrais for his help with the SEM-EDS analyses and Jean-Alix Barrat who kindly proposed to make the EPMA analysis. We thank Jeff Walker for providing us with the sample of obsidian from Puerto Rico via Sebastiaan Knippenberg. We also want to thank Erwan Bourdon (BRGM) for providing help during the prospecting campaign, and Charles Le Losq and Pierre Rochette for discussion on volcanic glasses and tektites. Finally, we want to thank all the respondents to our survey about the presence of such material in the Caribbean archaeological record and the discussion about it, beyond those already mentioned: Benoît Bérard, Andrzej T. Antczak, Dominique Bonnissent, Arie Boomert, John Crock, Antonio Curet, Scott M. Fitzpatrick, Pierrick Fouéré, Jonathan A. Hanna, Jay Haviser, Queta Kaye, Reniel Rodriguez-Ramos, Nathalie Sellier-Segard, Nathalie Serrand, Peter E. Siegel, Martijn Van den Bel.

This work was conducted in the framework of the Projet Collectif de Recherche MAPLA (MAtières Premières Lithiques dans les Antilles), funded by the French Ministry of Culture (SRA Guadeloupe) and the Regional Council of Guadeloupe. This study also received financial support from the French government in the framework of the University of Bordeaux's IdEx "Investments for the Future" program / GPR "Human Past".

For the purpose of Open Access, a CC-BY public copyright licence has been applied by the authors to the present document and will be applied to all subsequent versions up to the Author Accepted Manuscript arising from this submission.

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