The archaeological site of Monte da Ramada 1, situated in the inland region of southern Portugal (Fig. 1), encompasses a diverse array of archaeological structures and contexts, exhibiting a range of different morphologies and chronologies. These span a considerable chronological range, from the Chalcolithic to the Islamic period (Baptista et al., 2018). Two hypogea (hypogeum 2 and hypogeum 4) have been identified among the remains. Each one is composed of a funerary chamber, closed by slabs, with an atrium and presents distinct inhumation sequences. They have been assigned to the southwestern LBA. In the context of hypogeum 4, the slabs were found to be wrapped in a greasy black clayey earth, which is likely to have had waterproof properties due to the presence of an organic component (a fatty material) that would have sealed the chamber (Ribeiro and Soares, 1991; Frade et al., 2012). Several individuals buried in these graves were radiocarbon-dated (Soares et al., 2020), providing an exceptional opportunity to study rituals and grave goods with a well-defined chronology (Valério et al., 2018; Soares et al., 2021). Actually, the funerary structures of Monte da Ramada 1 are the first LBA hypogea ever found in southwestern Iberia, substantiating the enduring prevalence of this funerary architecture, which had been in use from the Late Neolithic to the Middle Bronze Age (Alves et al., 2010; Valera et al., 2008).

The chamber floor of the hypogeum 4 revealed a primary burial of an individual, accompanied by an ossuary on its north side, that consisted of the bone remains of two individuals. The last individual buried in hypogeum 4 had a rich and uncommon set of personal ornaments, including three bronze bracelets and several beads (two of them of gold, six crafted from ostrich eggshell, one presumed to be glass and another made of ivory or bone). The skeleton was radiocarbon dated to the 10th century BC (Soares et al., 2020). The presence of such exotic materials and their early chronology point to the existence of pre-colonial contacts with the eastern Mediterranean (Soares et al., 2021; Valério et al., 2018).

Hypogeum 2 presented a very complex stratigraphic sequence, with a succession of osteo-archaeological deposits that corresponded to multiple phases of funerary usage. The recorded sequence of anatomical connections, isolated or mixed with disarticulated parts, indicates an intense reuse of the funerary structure within a relatively short period of time. In fact, the presence of these anatomical connections reveals that the oldest burials still had soft tissue when they were remobilized. The minimum number of individuals was calculated based on the conjunction of articulated skeletons and disarticulated bone remains, resulting in a total of 20 individuals (Baptista et al., 2018). This number is unique in peninsular Bronze Age funerary contexts. Grave goods include exotic ornaments, perhaps of foreign origin, specifically two tiny cylindrical beads, likely made of faience, and a ring, likely made of jet or amber. Six of the skeletons were radiocarbon dated. The results show that the hypogeum was in use during the 10th century BC and continued to be used during the 9th century BC (Soares et al., 2020).

In addition, grave goods include ceramics and bronze artefacts (most of them with an average content of c. 10 wt% Sn) that align with the typologies known from the southwestern LBA. However, some of the metal artefacts, such as the set of three bracelets from hypogeum 4, present an uncommon composition, i.e., one arsenical bronze (4.3 wt% Sn - 4.0 wt% As) and two bronze alloys (6.8 wt% Sn - 0.13 wt% Pb - 0.09 wt% Fe and 7.1 wt% Sn - 0.13 wt% Pb) all with a low tin content when compared with the rest of the collection (Valério et al., 2018). The unusual alloy composition and their association with exotic grave goods, either in hypogeum 4 or in the coeval hypogeum 2, suggest a foreign origin for those metal ornaments. It is most probable that they originate from the eastern Mediterranean, where a diversified metallurgical technology emerged during the early stages of the first millennium BC. For instance, a collection of fibulae and pins from Nimrud (Iraq) includes five binary bronzes of analogous composition (3.2–8.0 wt% Sn - 0.15–0.85 wt% As - 0.20–0.90 wt% Pb - 0.02–0.24 wt% Fe; Giumlia-Mair, 1992). The bracelets’ early chronology indicates that pre-colonial contacts occurred in some places on the Iberian coast at that time (Soares et al., 2021; Valério et al., 2018).

The Palhais necropolis is part of a distinctive type of EIA funerary structures specific to the Beja region. The funerary architecture and rituals of the EIA in the south and southwest of Portugal are the result of the Orientalising process that occurred in this region between the 7th and 5th centuries BC. Three sub-regions, corresponding to three distinct types of funerary architectural structures, can be identified. The coastal area is characterised by inhumations in stone cists, in accordance with the indigenous southwestern Bronze Age tradition. The inland area of Ourique displays stone tumuli, which appear to be associated with the ritual of incineration. The nucleus of Beja was only recently identified and characterised due to the archaeological works related to the Alqueva irrigation network. In this nucleus, the ritual of inhumation prevails, and the architectural structures are characterised by open (U-shaped) or closed orthogonal funerary enclosures that are limited by ditches. A central tomb, a pit with a rectangular shape, was placed within each enclosure, while other individual graves, also with a rectangular shape similar to that one of the central tomb, were located on the limits of these enclosures or in their immediate vicinity. The grave goods, which included ceramics, metal, and exotic raw materials, generally exhibited an Orientalising character (Arruda et al., 2016; Soares et al., 2016).

The fieldwork conducted at the Palhais necropolis was undertaken as a rescue excavation. The archaeological intervention did not exceed an area of 37 m² (Santos et al., 2009). Along with other EIA contemporary necropolises in the Beja region with similar architectural features and contexts, i.e., Monte do Marquês 7 (1300 m to the southwest from Palhais) and Vinha das Caliças 4 (2300 m to the northeast) (Arruda et al. 2016), Palhais stands out for being one of the first known Iron Age necropolises with this characteristic typology of the Beja region, and also for the richness and diversity of grave goods that have been recorded therein (Santos et al., 2016). In the excavated area, several structures were identified, namely two partially overlapping funerary enclosures. Inside enclosure 1, two negative structures were recorded: a severely damaged burial tomb (grave 4) and another structure, which may have been votive or related to a funerary cult, containing a number of ceramic vases (Santos et al. 2016, pp. 242-249). Among them, four vases à chardon with red paintings stand out, one of which is crowned by nine ornithomorphs. Furthermore, two additional graves were identified (graves 1 and 2), each featuring a rectangular shaped plant. Each grave held the remains of a single female individual accompanied by grave goods of a personal nature (Santos et al., 2016). In grave 1, a necklace with 438 tiny discoid beads and one fusiform bead (perhaps the central element of the necklace) was recovered, along with a small iron dagger with a falcata-shaped blade, a fibula, and a set of instruments for body grooming. These items were all made of copper-based metal (Santos et al., 2009, fig. 6; Santos et al., 2016, fig. 7). Analyses of these artefacts show that they were produced as functional tools using bronze alloys with low tin content (Valério et al., 2013). Grave 2 yielded a bronze belt-lock (type 4c, following Cuadrado and Brito, 1970), with an exceptional scroll decoration of palm leaves, a motif characteristic of the eastern Mediterranean region. A small iron falcata-shaped knife and a bronze toilet set, of a lesser quality than the one from grave 1, were also identified. Other grave goods include a silver acorn-shaped pendant and five hollow beads of the same metal (Valério et al., 2013). All of them would originally belong to a necklace, along with several beads of different shapes and apparently made from assorted materials, including glass beads, a decorated circular ceramic pendant and a scarab bearing an incised inscription of Amon-Ré (Santos et al., 2009, fig. 8; Santos et al., 2016, figs. 9, 10). The most distinctive feature of the copper-based grave goods from Palhais is the alloy composition - bronzes with a low tin content and a relatively high amount of iron impurities (2.0–8.3 wt% Sn - 0.34–0.92 wt% Fe). These compositions clearly fall within the parameters of Orientalising metallurgy (Valério et al., 2013). It should be noted that the composition of these metals agrees with the coeval metallurgy in the region, as evidenced by analyses of metal grave goods from other similar EIA funerary contexts in the Beja region (Valério et al., 2021). A different question is whether the items were manufactured abroad or locally. The presence of uncommon metallic typologies, such as the toilet sets, together with the association with clearly imported materials, such as the necklace beads and scarab made of exotic raw materials, suggest the potential trade with other Mediterranean regions. Furthermore, the iron content of the analysed bronze alloys is also of considerable significance. The importance of a low amount of iron (<0.05 wt%) in ancient bronze alloys was first acknowledged through a comparative analysis between LBA and Phoenician bronzes from Iberian sites. This observation was regarded as an indicator of smelting with a poor reducing atmosphere (Craddock and Meeks, 1987). In the Iberian Peninsula, the low iron contents of EIA bronzes are attributed to the continued use of smelting crucibles throughout the Iron Age, as opposed to the utilization of true furnaces (Rovira and Montero Ruiz, 2013; Valério et al., 2016). Additionally, in regard to the copper-based metallic artefacts unearthed in Morro de Mezquitilla (Málaga) and Tejada la Vieja (Escacena del Campo, Huelva), which date to the 7th-6th centuries BC and 6th-4th centuries BC, respectively, Giumlia-Mair states that “the relatively high iron content of the analysed items indicates the use of copper smelted in furnaces with facilities for tapping the slag and therefore close contact with the civilizations of the eastern Mediterranean” (Giumlia-Mair, 1992, p. 114). As far as we know, the earliest copper-based metallurgical workshop in EIA contexts of southwestern Iberian Peninsula is that of Cabeço Redondo (Moura), ascribed to the 5th century BC. This workshop used copper obtained in slag-tapping furnaces, which were likely imported from abroad (Valério et al., 2022). Therefore, the bronze artefacts recovered in the Palhais necropolis and other coeval necropolises in southern Portugal are most likely local copies of foreign models or imports, particularly those with a high iron content.

The site of Montinhos 6, located on the left bank of the Guadiana river (Fig. 1), was also surveyed in the framework of the irrigation network linked to the Alqueva dam. However, the area covered by the archaeological excavation was considerably larger than that of Palhais. Approximately 250 archaeological contexts were identified and recorded, of which around 200 were assigned to a prehistoric chronology. This consisted of hypogea and pits dated to the Chalcolithic and the Bronze Age. The remaining contexts are from the post-Roman period or of an undetermined chronology (Baptista et al., 2012). An unusual EIA grave was recorded. It contained the burial of an adult female individual, deposited in a long and narrow pit that seemed to have been in existence prior to the burial. It was radiocarbon dated to a period between the 8th and the first half of the 6th century BC (Soares et al., 2016, fig. 2, p. 133). With regard to grave goods, only a necklace made up of 39 whitish and/or bluish-green discoid beads, some with a vitreous appearance, as well as a drop-shaped glass pendant and two brownish tubular beads of the same material, were recovered. All of these items were located in the neck region of the deceased (Soares et al., 2016, fig. 3).

Two stone cists were excavated in the geological substrate (schist) at the necropolis of Corte Margarida. Their architecture is very similar to that of graves from the southwestern Bronze Age, i.e., a stone box with a rectangular shaped plant made up of four slabs placed vertically. The interior of grave 1 features a triangular compartment, situated within one of the cist’s corners, which contained a ceramic vase, potentially a funerary urn. However, no evidence of bones or ashes was found within this vessel or within the remaining space of the cist. The burial gifts consist of a ceramic cup, a necklace comprising approximately 20 beads, the majority of which are ring-eye black glass beads, and three small amber pendants. Similarly, grave 2 also lacks bone remains, but the grave goods are more varied. These include a necklace with 48 beads, some of which are ring-eye black glass beads and others of different shapes and raw materials; a scarab with an inscription on the base referring the name “Pedubaste”; a fragment of a silver ring; a probable shark tooth; and two bird-shaped clay figurines. An EIA chronology (6th century BC) has been attributed to this necropolis (Deus and Correia, 2005), which displays architectural features that are not affiliated with the typical EIA typology observed in Beja funerary necropolises, but rather with the funerary world of the coastal regions of Algarve and Alentejo (Arruda, 2009), although it is located not far from Beja (Fig. 1). It is important to note, however, that there seem to be a common symbology and mythology shared by these EIA communities, in which birds, bulls, and felines, among others, assume a central role. The ceramic ornithomorphs and bovids from funerary contexts in the Beja region, like those from Corte Margarida and Palhais necropolises, as well as the ceramic figurines representing felids and bovids from necropolises of the Ourique region, seem to translate a similar ideological discourse of Mediterranean inspiration, most likely with an Orientalising origin.

Archaeological excavations carried out in the estuarine settlement of Quinta do Almaraz have revealed a diverse material culture, in which Phoenician and/or Orientalising artefacts occupy an important place. However, the presence of materials with chronologies spanning a considerable length of time suggests that the occupation of the site began in the Late Neolithic. While an exhaustive study of the artefacts recovered during the various archaeological surveys has yet to be published, the radiocarbon dating of several samples indicates that the EIA occupation started at the end of the 9th, beginning of the 8th century BC (Barros and Soares, 2004; Soares and Arruda, 2018). Furthermore, the site, situated on the left bank of the Tagus River, has yielded a plethora of Orientalising archaeological finds, some of which are rare and even unique within the Portuguese territory. These include alabaster vases (Cardoso, 1995), a scarab dated between the 7th and 6th centuries BC (Almagro Gorbea and Torres Ortiz, 2009), Middle Corinthian pottery, a Greek import from the archaic period dated between 600 and 575 BC (Cardoso, 1995) which is very scarce in Portuguese sites (Arruda, 2007), some Phoenician red slip ware dishes with a flattened rim of small width (Barros et al., 1993) and a diversified copper-based metallurgy that diverges significantly from the indigenous metallurgy inherited from the LBA (Valério et al., 2012).

In fact, the metallurgy introduced by Orientalising populations is clearly discernible in the Phoenician settlement of Quinta do Almaraz (Almada). The metal collection from this coastal site, dating from the 9th to 7th century BC, comprises a considerable number of copper artefacts and some leaded bronzes. Nevertheless, binary bronzes remain the most common alloy, yet are much poorer in tin compared to those from LBA (5.4 ± 2.0 wt% Sn, n=15, Valério et al., 2012), exhibiting an average value that is approximately half of the LBA indigenous collections. The iron impurities are also much higher (0.15 to 1.3 wt% Fe) than the observed in the ‘indigenous’ collections (mostly <0.05 wt% Fe). A comparable diversification of metallurgy has been identified in other coeval areas of the southwestern Iberian Peninsula, suggesting strong links with the prevailing Mediterranean metallurgy of the period.

XRD was performed on all necklace beads and scarabs (Tab. 1), with the exception of beads #2 and #3 (Fig. 2 - 1 and 2) from hypogeum 4 of Monte da Ramada 1. They were only analysed by microPIXE, as it became evident through simple macroscopic analysis that their manufacture involved the use of raw materials of organic origin.

The diffractograms of the XRD analysis revealed that the majority of the specimens are faience (Tab. 2), with the exception of three beads. Bead #1 of hypogeum 4 of Monte da Ramada 1 (Fig. 2 - 5) and bead #5 of grave 2 of the Palhais necropolis (Fig. 2 - 14) were manufactured with an amorphous raw material. This result may initially be interpreted as corresponding to glass, although this requires confirmation or refutation by subsequent analysis by PIXE. Bead #16b (Fig. 2 - 12) of the same grave is made of calcite. The remaining specimens display a predominantly quartz composition, though they may also contain other minerals, such as coesite [SiO₂], lutecite or moganite [SiO₂], calcite [CaCO₃], gehlenite Ca₂Al [AlSiO₇] or genthelvite [Be₃Zn₄(SiO₄)₃S] (Tab. 2). Fig. 4 presents five XRD diffractograms, which demonstrate the diverse range of minerals or mineral mixtures identified through XRD analysis.

It should be noted that coesite and lutecite or moganite are polymorphs of quartz (SiO₂). These polymorphs are formed at pressures and temperatures different from those involved in the formation of quartz. This evidence indicates that the small crystalline particles that constitute the core of the artefact were obtained from quartz sand and not by the fragmentation of a quartz block or pebble. Genthelvite may be also indicative of the use of this type of sand, while gehlenite is the result of the decomposition of calcite at temperatures between 700-850 ºC, followed by a reaction with aluminosilicates present in faience. This process is similar to the one observed during the firing of clays for the manufacture of common ceramics (Trindade, 2007; Ringdalen, 2015). The presence of gehlenite may be indicative of the use of beach sand, as this kind of sand contains fragments of shells which are, as is known, made up of calcite (or aragonite).

For the PIXE results calculations presented here, all detected elements (those heavier than Na in the case of combining 1.0 MeV and 2 MeV proton beam spectra) were considered to be in their oxide form, with final concentrations normalised to 100 wt%.