Shining Like Gold and New: The Emergence of Brass North of the Alps Around the Turn of the Era.

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Daniel Bursák, Alžběta Danielisová, Tomáš Magna, Petr Pajdla, and 4 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-715158/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted 8 You are reading this latest preprint version Abstract Ancient brass ( aurichalcum ) was a valued commodity in the Antiquity, notably because of its gold-like appearance. After mastering brass fabrication using the cementation procedure in the 1 st century BC in the Mediterranean, this material became widely used by the Romans for coins, jewellery and other objects. Because of its visual qualities, it is believed that since this period, brass played an important role in diplomatic and economic contacts with indigenous communities, notably Celtic and Germanic tribes north of Danube and west of Rhine. To test this hypothesis, we performed for the first time the archaeometric and advanced statistical multivariate analysis of a suite of late Iron Age and Early Roman period (1 st century BC – 1 st century AD) brass and other copper-alloy objects from the territory of Bohemia to constrain their provenance. The new results for brass objects from this early phase of the massive occurrence of Roman aurichalcum in the Barbarian territories point to the ore deposits in the western Mediterranean or the Massif Central area in Gaul, consistent with historical events. These new findings underscore the great economic and political importance of the new and rich mineral resources in the Transalpine Gaul acquired due to Caesar's military campaigns Archaeology Geochemistry Shining gold Ancient brass (aurichalcum) commodity Antiquity notably brass fabrication material western Mediterranean Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Figure 8 Figure 9 1. Introduction Brass is undoubtedly one of the most valued materials in Antiquity. Its high appreciation is underscored by the written sources, particularly in Pliny the Elder's and Cicero's works [1, 2]. Since the discovery of Zn-rich alloys in the material culture of the Early Roman period, several studies have summarised its origins, the technological process of its fabrication by the Romans and its importance during that time [3, 4, 5, 6, 7]. It appears that the widespread distribution of brass is connected with the period of the reign of Augustus and his coinage reform in 23 BC. The earliest brass objects in Bohemia are represented by a brass fourrée (counterfeit) stater from the oppidum of Stradonice [8], brass Almgren 65 brooch from the oppidum of Závist, and several imported brass rings from the other oppida (Fig. 1, Table 2-4), all dated around the middle of the 1 st century BC and, except for the coin, supposedly the products of Roman workshops imported to the North as exclusive jewellery pieces [9]. However, there is still limited knowledge on the nature of trade with brass between the Romans and the indigenous populations (i.e . Celtic and Germanic tribes) beyond the Roman territories. The only known indication from this region is a hoard retrieved from the Rhine river, containing over 50 bars, with some of them made of brass [10]. The massive emergence of brass objects north of the Alps and in Bohemia in particular, almost unknown during the preceding La Tène period, corresponds well with a significant influx of Roman imports to the Barbarian territories in the Early Roman period, i.e. between the second half of the 1 st century BC and the first half of the 1 st century AD [11, 12, 13, 14, 15]. The original brass produced by Roman workshops in the first half of the 1 st century BC with very distinctive composition and material properties has been referred to as the aurichalcum [1, 4, 7]. Thanks to modern analytical tools, there has been some progress in identifying brass manufacture (possibly from the Roman imports) in the broader area of Europe among the objects dated already to the early 60s BC; however, their geological provenance remained mostly undetected [16, 17, 2, 18, 9]. More recently, studies systematically dealing with the Pb isotope compositions of selected materials, such as copper [19, 20, 21, 22], lead [24, 25], and brass [2], have become available. It has been noted that the provenance analyses of ancient Cu from the Iron Age and later periods might be challenging due to the complexity of the interpretations imposed by numerous and often unknown resources, widespread material mixing, recycling, depletion, and other reasons. However, even if the determination of the exact origin of the objects in question proves to be difficult, the provenance studies remain to be a great source of information for the understanding of contemporary socio-economic networks that are often key to understanding the historical events [e.g., 25, 26, 27, 28]. The historical framework of this study could be briefly outlined as a period starting with the decline of the late La Tène civilisation (conventionally linked with the Celts), around the middle of the 1 st century BC, followed by a massive migration wave(s) of the early Germanic tribes (Marcomanni, Quadi, and others) sometime between the second half of the 1 st century BC to the 2 nd century AD [29, 9]. Beginning and the course of the Julio-Claudian dynasty with a distinct intensification of the Romano–'Barbarian' contacts is the primary time frame for the majority of samples presented in this study [30, 31, 32, 33]. In this period, jewellery from the Germanic graves in Bohemia was identified to be made of high-quality brass, approaching the chemical composition of the original aurichalcum [15, 13, 4]. A possible Roman origin of the brass coming to indigenous territories was naturally assumed when these objects were first analysed [15]. Especially in the case of early Germanic brooches of the so-called 'eye type' with ca. 20% Zn, it was proposed that recycled Roman imports, primarily brass coins, were used for their fabrication [13, 10]. All this makes Bohemia an exceptionally well-suited territory for studying brass production and circulation patterns compared to other 'Barbarian' territories north of the Alps and east of the Rhine (Fig. 1). The striking richness and material diversity of copper-alloy objects in the Bohemian territory have frequently been related to the existence of the so-called Empire of Marobudus, a power structure that kept friendly relations with the expanding Roman Empire after the critical defeat of three legions in the Battle of the Teutoburg Forest in AD 9 [12, 34]. In that period, the Central European territory was at the intersection of the territorial interests of the expanding Roman Empire, new migration waves of the Germanic tribes from the North and the West, and the remainder of the late Celtic population. As such, this territory interconnected many cultural traditions manifested in the material culture. Those were especially the costume parts (brooches, belts, pins and other personal objects), imported luxury items such as bronze drinking vessels, tableware, and other objects. In this study, we present new compositional and Pb isotopic data for the early Roman brass artefacts from the territory of Bohemia to initiate the discussion on the currently scarce archaeometric research on the early brass in Europe. The character of the Early Roman period bronze and brass is compared with the previous late Iron Age [27, 35, 28]. 2. Material 2.1. Studied samples In total, 50 Late Iron Age and Early Roman period objects from the territory of Bohemia were sampled for geochemical analyses (Fig. 1). Most items come from metal detector prospections, so the information about their original context is scarce. Nonetheless, all samples can be characterised by localisation, typological determination, cultural provenance and dating (Table 1, 2). The selection of samples for further investigations was driven by identifying those objects among the cultural groups most likely fabricated from brass. 2.2. Categorisation of samples Rich typological diversity of the finds led to a robust scholarly tradition in the past, which was aimed towards a thorough typo-chronological evaluation with much effort put into the detailed mapping, sequencing and cataloguing of the finds [36, 37, 38, 39, 40, 41, 42, 43, 44, 45, 46]. A vital research premise was to establish the general typo-chronological groups of personal jewellery and other objects, usually described as the 'Western tradition' (i.e. Gallic and Rhenish), the 'Danube tradition' (or Norico-Pannonian, Rhaetian), or in a more general sense the 'Roman-provincial tradition'. Such categorisation represents a valuable methodological tool for working with archaeometric data because it can be used as independent evidence. The following cultural and chronological groups of brass objects were defined for the correlation with the geochemical analysis: La Tène ('LT - Brass'): objects made in the late La Tène tradition of metallurgical production, usually carried out at the oppida or other major agglomerations (mainly in the Middle Danube area). Their chronological assessment and interpretation are based on a recent study of the late Iron Age in Bohemia [9]. This group contains four brass objects: a late Almgren 65 type brooch and three imported brass rings of the Roman provenance (Fig. 9, Table 2). Local (' L' ): objects generally supposed to be fabricated in the early 'Barbarian' metallurgical tradition. This material culture commonly is associated with the Germanic tribes appearing in the Bohemian territory from the second half of the 1 st century BC. This group contains mostly personal objects, especially eye brooches of the Almgren 45-49 type [37, 47, 48]. Import ('I'): finds not of the 'Barbarian' provenance; they usually are considered to be the diplomatic gifts brought to the Bohemian territory by trade, exchange or as booty from the territories controlled by the Romans [12, 49, 50, 51]. Because several different typological groups are included in this broad category, further subdivisions were needed, such as 'Noric' and 'Western'. Also, more ambivalent types in terms of the place of origin were included, such as Almgren 18 brooches, which are sometimes interpreted as being produced locally. Bohemian finds appear to be exogenous and ultimately connected with the populations that occupied the territory from the second half of the 1 st century BC [52]. Noric ('N'): objects made in the cultural tradition of the territories around the Middle Danube zone and the Eastern Alps, including the parts of the so-called 'Norico-Pannonian costume' and finds mainly occurring in the territory of ancient Rhaetia (roughly the Alpine zone of today's Austria). Brooches and other jewellery are thought to represent continuity from the preceding late La Tène costume tradition [36, 53, 40, 43]. Western ('W'): this category has been used as a label for Alesia, Almgren 19 (including its subvariants), Almgren 15, and the so-called Gallic brooches of the types Feugère 13b, 19b and 19d. These objects mainly occurred around the Middle Rhine area or in eastern Gaul. To avoid ambiguity in cultural determination, some types, such as the Aucissa and Almgren 18, were categorised simply as Import ('I'), indicating their non-Germanic provenance. La Tène period Early Roman period 130/120–70s BC LT LT D1a - 70s–50/40s BC LT D1b - from 60s/40s–20s/0 BC LT D2 / R A 10/5 BC–AD 20/30 - R B R B1 R B1a AD 20/30–40/50 - R B1b AD 50/70–150/160 - R B2 Table 1: Summary of the chronological system employed in the sample categorisation. The generally accepted chronological framework for the late La Tène [15] and the Early Roman period, respectively [54, 45, 29] were followed 3. Results 3.1. Chemical composition For comparison with data published elsewhere, all compositional data used in this work are presented in the form of the analytical totals normalised to 100 wt.%. Most analysed samples are represented by alloys with Zn contents > 15 wt.% (Suppl. 2). In terms of main alloying components, Pb, Zn and Sn (Fig. 2 ), variations, most likely compatible with their different chronology, are apparent. Zinc content in late Iron Age brass rings from the oppida were always ca. 20 wt.%. In the Almgren 65 brooch, the alloy also contains around 20 wt.% Zn. Very high Zn contents (median at 17 wt.%) on the one hand and very low Sn and Pb concentrations on the other are typical for the phase R B1 (10 BC-AD 50). There is a slight tendency towards more consistent and also higher Zn contents among samples towards the end of this phase (ca. AD 30–50). Brass with significantly lower Zn contents (2–9 wt. %) was detected in categories of imports ('I') from the beginning of the Early Roman period (second half of the 1st century BC). These objects also have comparable contents of Zn and Sn. The second category with a similar position in the composition plot (Fig. 2 ; Suppl. 1) is partly represented by samples of the local ('L') origin that are usually dated around the middle of the 1st century AD (phase R B2). There are also two leaded Cu alloys: (i) a drinking horn fitting and (ii) a fragment of a handle of the Roman imported vessel (bronze decoration with a human mask). Four samples were detected to be made of Sn bronze without the addition of Zn. All belong to the 'L' category. A single case of a brooch (sample RIM008) with an exceptionally high amount of Ag at 20.8 wt. % is also reported. Principal component analysis (PCA) was performed for a more detailed evaluation of the chemical composition. The choice of minor/trace elements (Pb, Co, Sb, Ag) has been made considering their symptomatic value for provenance studies [56, 57]. The resulting factor scores are plotted in Fig. 3 . They clearly distinguish between the imported items ('I') and the rest of the samples, mainly due to the variability of the Zn content. The most extensive dispersion is observed in the category of local items ('L'), reflecting significant variations in the general composition of the used alloys (Fig. 2 ). Most samples in the 'N' category tend to have higher Ag contents (0.26–1.2 wt. %) which may show consistency with their supposed Alpine origin (see below). A slightly negative correlation between Co and Ag was observed; however, there does not seem to be a clear correlation with the typo-chronological categorisation of samples (Fig. 3 ). 3.2. Lead isotope systematics Lead isotope analysis shows similar results as the PCA (Fig. 4 ; Suppl. 3). The most significant variability is observed in the category of local items ('L'), followed by a slightly more homogeneous Norican ('N') group and the imports ('I').Samples in the 'Western' category ('W') form the tightest cluster, which is also coherent chronologically (phase R B1; Fig. 4 a). Their linear trend and its spatial overlap are most similar with the cloud of the ores from the Massif Central (Fig. 7 ). Almost all samples from the 'LT-brass' category are mutually close and show a significant consistency with the ore deposits in the western Mediterranean (i.e. Iberia) and the Massif Central in France. Sample TRS 003 is offset from the rest of the suite but still plots in the Pb isotope space of the Spanish or French deposits. All brass objects in the 'I' category (imports) are from the phase R A, and all of these samples show a tendency towards more radiogenic 206 Pb/ 204 Pb ratios. A tendency towards less radiogenic 207 Pb/ 204 Pb and 206 Pb/ 204 Pb ratios is observed for items from the chronologically youngest period (R B2). A costume pin sample RIM 001 made of brass with high Zn content (> 15 wt.%) represents an 'outlier' with the lowest 207 Pb/ 204 Pb. A clear tendency of samples with low Zn content (< 5 wt.%), dated either in the earliest or in the latest phase (R A or R B2), owards less radiogenic 207 Pb/ 204 Pb values is apparent (Fig. 4 b). The samples from the phase R B1 with high Zn contents appear to be dispersed around 206 Pb/ 204 Pb ratio of 15.68 and are relatively homogeneous. Lead-rich (~ 5 wt.%) imported vessel has the same Pb isotope systematics as the high-Zn low-Pb items from the phase R B1. A drinking horn fitting with the highest Pb content of 9.5 wt. % plots separately with 207 Pb/ 204 Pb and 206 Pb/ 204 Pb ratios of 18.55 and 15.65, respectively. 4. Discussion The original aurichalcum, i.e. the brass produced in Rome, must have contained at least 22–28 wt.% Zn [4]. In fact, the content of Zn in aurichalcum started to decrease already in the 1 st century AD and later produced aurichalcum further continued to lose its original qualities [58]. In parallel to such compositional evolution on the Roman side, lower Zn contents in Barbarian objects measured here can be attributed to local mixing and recycling of the imported objects. It was shown that alloy with the Zn content between 10 and 15 wt.%, that could be produced by a simple dilution process of equal quantities of bronze and the aurichalcum, already got its typical golden colour that was in demand among the indigenous communities [1, 59, 4]. This characteristic feature was favoured for producing the costume parts such as brooches, rings, pins and belts made both in Roman and Barbarian cultural environments. However, geochemical data for metal finds from the Barbaricum are still sparse, particularly those of the local (i.e. Germanic) provenance. In order to reveal further details about the manufacturing of brass in the indigenous territories, the assemblage analysed in this study was compared with chronologically and typologically compatible data from published reports. 4.1. Comparison with contemporary assemblages The comparative dataset of chemical compositions included early Roman finds from Bohemia (NAA method, [15]) and Cambodunum (AAS method, [60]), both analysed in the 1990s, brass brooches from the territory of Slovenia (PIXE method, [16, 17]) and brass staters from Gaul (FNAA, [61]). Due to the currently followed hypothesis about the Roman brass used for the fabricating costume parts in the Barbaricum, chemical data from the brass coinage [62] were used for a more detailed comparison. The latest data for the Roman brass coinage were obtained by PIXE and, unfortunately, do not provide sufficiently accurate results for the comparison. When comparing the earliest brass objects from the 1 st century BC, the main alloying components (Zn, Sn, Pb) reveal a cluster of late Iron Age brass staters of VERCA and Vercingetorix CAS series because of their lower mean Zn content (ca. 12.2 wt.%; Fig. 5). The difference between coins and other brass objects is probably due to chronology because the 'pure' brass, with high Zn content (>15 wt.%), and low contents of Sn and Pb (sum below 0.5 wt.%) appeared no earlier than around the 0 BC/AD. Simultaneously, there is evidence of Zn-rich brass in the second half of the 1 st century BC (phase R A). A second PCA with only selected trace elements (Co, Ni, Sb, Ag) was carried out with the comparative datasets. To avoid inconsistency, the dataset was reduced to brooches only. This step further enhanced the chronological compatibility among the typological groups of objects. Also, in the archaeological categorisation of groups, several trends were revealed (Suppl. 5a). Similarly to 'N' samples from Bohemia, also Norican brooches tend to contain more Ag, which is paralleled by higher contents of Sb, thus indicating fahlore copper used for their fabrication. The most significant trace element composition variability was observed for the local items ('L'). Chronologically speaking, a notable heterogeneity in the chemical composition may be observed in the phase R B1a compared to the following phase R B1b (Suppl. 5b). A specific group of objects of the Norican tradition from the phase R B2 forms a tight cluster in both plots. These findings indicate rather heterogeneous supply patterns of brass in the beginnings of the trade contacts between the early Empire and the Germanic communities, compared to the late Republic and Celtic agglomerations on the one hand and later part of the 1 st century AD on the other. When these results are compared with the Roman copper AES coinage, a slight correlation between the part of the Bohemian samples from the phase R B1a and the AES coinage group pattern III (EPG III), characterised by increased levels of Sb and Ag, is apparent [19]. Similar Sb- and Ag-rich copper coinage is also specific for the Lyon altar series I (LAS I) AES coinage [63]. These groups are also compatible with the dating of Ag-rich Norican samples in this study. However, the Sb levels of samples from Bohemia do not exceed 0.2 wt. %, which is the lowest level of AES coinage EPG III. There might have been an issue with partial volatilisation of Sb if the material had been repeatedly remelted to produce brass alloy and then possibly remelted again to fabricate the final artefact [68]. Nevertheless, in this case, high levels of Zn and only marginally lower Sb appear to exclude multiple re-processing of brass. Therefore, raw materials for AES coinage [19, 63] and brass objects from this study are less likely to come from the same source. The comparison of brass artefacts with > 5 wt.% Zn from Bohemia and Cambodunum [60] with the Roman brass coinage [62] is based on the Sb versus Ag bi-plot (Fig. 6). It clearly shows incompatibility between the local brass artefacts and the Roman sestertii . Due to analytical differences, the data must, however, be treated with caution. Also, a significant variability of the Roman metal supply for the coin production [cf. 20] must be taken into account. Therefore, for successful future provenance studies, a targeted archaeometric analysis of the Roman coins is vital. A brooch with unusually high Ag content (20,8 wt. %) is, generally speaking, uncommon - even in the context of the broad spectrum of Early Roman finds from Central Europe [13, 60]. Still, there are artefacts made of pure silver known from the contemporary cemeteries, and particularly this type of brooch (Almgren 24) is the one most frequently fabricated objects from precious metals [48, 64]. Considering the technologically advanced metallurgy – both Roman and Barbarian – unintentional contamination caused by the accidental use of silver-rich ore is highly improbable. An explanation of local manufacture with deliberate alloying with silver is thus plausible 4.2. Provenance analysis – mineral exploitation and raw resources in the Early Roman period Lead isotope analysis has become a prevalent method for tracing the archaeological artefacts containing lead to their possible geological origins, i.e. the ores they were fabricated from [65, 66]. The provenance analysis testing the consistency between the samples and the known ore deposits was carried out using a combination of the conventional biplots and the Euclidean (ED) and Mahalanobis (MD) distance algorithms [28]. The same approach was then applied to compare the contemporary bronze and brass assemblages of various cultural backgrounds. ED has initially been suggested by Stos [67] as a simple metric to compare how far the point distributions are from one another in a multivariate space defined by individual isotopic signals. While ED is currently widely used, it is advised to be complemented with MD in which the effects of the shape, scale and trend of the distribution of the data are accounted for [68]. Therefore, the metric is capable of measuring the distance from a data point to distribution in the multivariate space and can account for the distance of points as well as for the linear trends in the data and distributions of the data clouds. Derived plots (Fig. 8; Suppl. 6) are used to predict the allocation of analysed brass objects from Bohemia into the comparative datasets. Because of considerable overlaps in the data distributions of different ore deposits, it should be kept in mind that the predictive value of ED + MD can vary from one source to another. The best level of consistency for most of our samples is observed with polymetallic deposits from the Massif Central (Fig. 7; Suppl. 6, 7). These results were verified by both the ED and MD; however, the outliers in the Massif Central ore dataset provided a less pronounced consistency than the standard biplot. There is also a possibility of mixing the sources from various deposits, namely the Mediterranean (Iberia, Sardinia, Macedonia, or Attica) or the Alpine (namely the south-eastern Alps and the Inn Valley; Suppl. 6; Suppl. 7). The Alpine signal is the strongest in the 'N' category. British ores did not come into consideration until AD 43 when Britain came under Roman control, so these data were omitted for historical reasons. Because of their analytical match with the Massif Central, the geochemical data from early Roman imperial Pb objects were included in the comparative analysis: the Augustan Pb water pipes from Pompeii [code 'Pb pipes'; 69] and Pb ingots from the shipwreck of Sainte Maries de la Mer [code 'Pb ingots'; 70]. A similar analytical match and subsequent historical interpretation favouring the Massif Central deposits were suggested for brass ingots from the Aléria shipwreck [code 'Cu-Zn Ingot'; 2]. Because no Pb isotope data for the artefacts of the 'Barbarian' provenance are available, only the early Roman Imperial datasets could be included in the comparative analysis. Regarding the provenance of Cu, there is an extensive corpus of comparative data from the Roman AES coinage [20, 63] and Cu ingots of the Sud-Lavezzi 2 Bonifacio wreck from the beginning of the 1 st century AD [21]. Finally, since one of our aims was to detect possible consistency between the Germanic finds and the preceding late Iron Age artefacts, to detect potential looting of the abandoned Celtic oppida by the newly incoming Germanic populations, bronze objects mainly from the 1 st century BC ('Oppida' set) were also included in the comparative dataset [27, 28, 35]. The results show that the Pb isotope compositions of most of the Early Roman samples in this study are generally inconsistent with late Iron Age finds (cf. results of ED and MD, Fig. 8; Suppl 8). A part of samples, consisting mostly of samples dated to the La Tène period or late 1 st and/or 2 nd century AD with less radiogenic 207 Pb/ 204 Pb and 206 Pb/ 204 Pb ratios are closer to deposits in Germany, and are consistent with Roman Cu coins, Cu-Zn, Pb ingots and part of the copper AES coinage from the LAS I. There is no analytical match with the Cu bars from Sud-Lavezzi 2 Bonifacio wreck, although the Cu bars might be a very convenient and contemporary source of copper. The group of samples with low Zn contents (Fig. 2) from the R A and R B2 phases and their tendency towards less radiogenic 207 Pb/ 204 Pb ratios (Fig. 4b) are still within the range of the ores from the Massif Central. However, three out of four samples from the early phase (R A) show some proximity towards the south-eastern Iberian zone, most compatible with the late La Tène samples [27]. Sample RIM017 with a lower 206 Pb/ 204 Pb ratio contradicting this chronological explanation could be dated into the phase R B1 as well (Table 2, 3). The LAS I is consistent with part of the Bohemian samples in their Pb isotope ratios and the Ag content [63]. A tendency towards less radiogenic 207 Pb/ 204 Pb and 206 Pb/ 204 Pb ratios may result from the influence of the Iberian Massif (Suppl. 8). The southern Spanish mines are thought to be the most important in the organisation of the Roman Cu supply [20], which is also evidenced by the most chronologically compatible dataset - the imperial AES copper coinage. Data from the AES coinage are partly inconsistent with Cu ingots, but the variability of Cu sources corresponds well with the suggested complexity of the Cu industry of the Roman Empire [21]. In the case of samples from the phase R B2, i.e. after 43 AD, Pb-Zn deposits from Great Britain may also come into consideration [cf. 2]. Since the amount of data from this late phase is low, further historical analysis, such as the trend comparisons with discussed ore deposits, cannot be performed. To sum up, there are three most distinctive analytical matches in terms of possible ore resources. All these scenarios are generally historically plausible and can be thus discussed further: (i) The mixing of Mediterranean sources has been thoroughly discussed for the Pb pipes from Pompeii, which had Pb isotopic signature close to the samples from this study (Fig. 8) [69]. The authors interpreted lead from Pompeii as a mixture of Sardinian, Iberian and Laurion ores; however, as recently pointed out [71], the possibility of the involvement of the Massif Central ores was initially omitted from the discussion. Considering the original 'mixing scenario', a more satisfying explanation for Pb in the Pompeiian pipes would favour the Cartago Nova deposits with a minor influence from Sardinian ores [71]. (ii) The Alpine origin of brass is unsupported because of the lack of clear historical evidence of Roman copper or lead mining in this region. There is a partial Pb isotope overlap with the deposits from the Central Alps (Valais) that may be associated with the 'Sallustian' copper, mentioned by Pliny the Elder, and linked to the Haute Savoie (Suppl. 6, 7), which was discussed in the context of the chemical composition of Lyon alter series AES coinage. This explanation, however, was abandoned because of the inconsistency of the LAS coinage with the Pb isotope ratios of given deposits [63]. A slight correlation of the chemical composition and Pb isotope compositions of the 'N' category of samples can be considered for geographical reasons, but this consistency is far from being solid. (iii) According to Leblanc's [72] map, the Pb-Zn mineralisation in the Massif Central is spread from Les Malines to Lyon, where the production of brass is dated from the middle of the 1 st century AD to the beginning of the 2 nd century AD [73, 74]. The south-eastern part of the Massif Central is rich in various Cu-bearing ore bodies with specific combinations of the trace elements, for example, ophiolites (Ni, Co, Ag), pyrite ores (Ag, Au), Permo-Triassic (As, Pb, Ag), and Hercynian veins (Sb-Ag-Pb) with the Salsigne type mineralisation (As, Bi, Au) [72]. The connection of the polymetallic deposits in the Massif Central [72, 75] with the Roman lead metallurgy has been suggested earlier [70]. To support this argumentation, six samples in this study that are made of Sn-bronze, Pb-bronze or Ag-rich bronze, i.e. without any cementation process possibly taking place, still have their Pb isotope compositions consistent with the Massif Central ores, and we may thus assume that even Cu was extracted in the same region. A specific mining site, consistent with the Pb isotopic data from this study, cannot be assigned because the available data cover the entire Pb isotope diversity of the Massive Central ore deposits [71]. At present, this dataset appears to bear similarity with Pb isotope I values from the Les Malines Pb-Zn deposit [75]. Whether the deposits in the Cevénnes area also served as a Cu source remains unclear [2]. 4. 3. Consideration of possible contamination A particular methodological risk should be considered when comparing brass objects with possible Cu ores because Zn ores, as an essential constituent of the produced brass, may also contain trace amounts of Pb [6, 2, 76, 77]. The inclusion of such Pb may then disturb or obscure the Pb isotope signature of the intrinsic Cu source during the cementation process [78]. There is also the uncertainty on how exactly and how much the cementation medium had impacted the trace element composition, which is crucial for the correct interpretation of the chemical composition of the analysed brass objects. So far, it is known that at least Fe and As can enter Cu metal during the cementation process [78]. In Roman Imperial workshops, where a very pure Cu was manufactured due to the advanced refining [19], the risk of contamination could be exceptionally high. Therefore, it must be acknowledged that the Pb isotope signal from the samples may point to the Pb-Zn source ore instead of the Cu ore [cf. 2]. Furthermore, the hypothetical contamination during the cementation process could strongly influence the comparison of Roman Cu coins and brass artefacts based on trace elements such as Sb and Ag. These notions, however, require carefully controlled metallurgical experiments. We assume that the cementation process was carried out using Zn in Pb-Zn ore rather than Zn in the form of ZnO, typically developed in furnaces during the pyrotechnological process [cf. 6]. The Pb contents in brass samples from this study are significantly higher than those in the LAS I coinage [63], representing at present the purest available copper from the Massif Central. 4.4. Roman brass production in the Massif Central Archaeological evidence for copper mining in the southern Massif Central during the Roman period is still rare; however, two sites in the Cavénes area served as Cu mines during the late 1 st century BC and early Imperial period [79]. One deposit around Carcassone, exploited during the later Roman Republic (2 nd and 1 st century BC), has also been documented [80, 63]. In general, there always is a possibility of missing archaeological evidence of past extraction activities due to medieval and later mining that may have obscured or eradicated the traces of earlier exploitation. Therefore, clear evidence of the Gallic metal supplies is still missing [24]. The best evidence for the early Roman (i.e. Augustan period) mining in the Massif Central is the Pb isotope analysis of the AES coinage of the so-called Lyon altar series I [63], supposedly originating in the Cévennes part of the Massif Central. Despite the fact that a part of the Roman brass coin production took place in the Lugdunum (Lyon) mint [63], similarly to Pb ingots of Santa Maria and partially also to Pb pipes from Pompeii, an Iberian origin was initially expected. However, as the chemical analysis of further Lyon altar series coins (the LAS II collection of the AES coinage) indicates, the Gallic production alone might not have been sufficient for the great demand for Cu during the reign of Augustus, and another Cu source (possibly of the Iberian origin) was thus used for this other series of ases [63]. From the historical perspective, there has been a suggestion that copper used for coins of the LAS I may have been the 'Livian' Gallic copper, mentioned by Pliny the Elder, as one that was quickly depleted [63]. It should be noted that also other Pb objects have been assumed to originate in the Massif Central, including the artefacts found in Germania [23]. Recently, another assemblage of Roman and Byzantine Cu and Cu-alloy coins nummi minimi from the 4 th – 8 th century AD was found to be consistent with the deposits in the Massif Central, suggesting a long-term mining tradition of local mineral resources [81]. On the other hand, critical notes have also cast some doubt on the Lyon crucibles, pointing out their lack of technical properties [6]. Nevertheless, based on the reasons presented above, we are confident that our data, in fact, indicate the early Roman cementation in the south-eastern part of the Massif Central, and the increasing evidence for the Imperial exploitation of Cu, Zn and Pb in general [63, 70] supports the original interpretation of the Lyon crucibles [73, 74]. The origin of most of the brass found in Bohemia in the Massif Central, and possibly their fabrication directly in Lyon, is not entirely impossible, as it is in accordance with the recent research, regularly pointing out the Gallic production [70, 23, 63, 2]. Consistency of these deposits with the data from an entirely different cultural tradition may appear surprising at first; however, they only point out the complexity of the socio-economic networks and the organisation of the metal supplies taking place already in the Early Roman period. Given the presence of the mint in Lugdunum (Lyon), a hypothetical origin of brass for the imperial coinage in the Massif Central seems to be very likely and should be verified by further analyses. The proximity of numerous rich ore deposits to Lugdunum was undoubtedly crucial for its economic importance. These indices could have been underestimated before the publication of geochemical data from this area that supported the ancient exploitation of local resources. Furthermore, the consistency of the Pb isotope compositions with samples from the late Iron Age may indicate a long-distance distribution of these mineral resources as soon as around the middle of the 1 st century BC, i.e. the time directly around Caesar's military campaigns in Gaul. 5. Conclusions The majority of samples from this study were made of high-quality brass, arguably of a Roman origin. The Pb isotope data show a clear consistency with ore deposits in the Massif Central, especially with Pb-Zn deposits near Les Malines. In addition, a high degree of homogeneity of the analysed samples in terms of their Pb isotope ratios probably excludes recycling using significantly different resources. Whether the Massif Central connection is provided by the Pb contained in the Cu source (metallic or geological), or is a result of the cementation process, cannot be unambiguously distinguished. Given the high purity of the Roman Cu – known from the Cu ingots and Cu-based coinage – with low Pb levels compared to slightly Pb-enriched brass samples, a lead isotope signal linked to the Pb-Zn ores is more likely. Nevertheless, as indicated by non-brass samples from our assemblage and local provenance of the AES coins of the first altar series from Lyon [63], even the copper could come from the same territory. The archaeological cultural groups used to categorise samples appear to have only a moderate significance in the pattern of trace element composition; even the Pb-isotope ratios were not influenced so significantly compared to categorisation of the samples according to dating. If we accept the possibility that the Pb isotope values refer to lead originating in the cementation medium, the variation in trace element patterns may point to various copper sources, or it may be a result of some further admixtures. Such fact does not contradict a possible different origin of a given artefact suggested by its typological classifications and refers solely to the material used for its fabrication. An important message provided by the geochemical analysis is the inconsistency of brass objects with contemporary brass coinage, the Roman sestertii . However, this finding requires verification by further analysis of a more varied selection of brass coins using state-of-the-art analytical methods. The best level of consistency is found among samples with high Zn content from the phase R B1, i.e. a period around the turn of the Era and the following five decades of the 1st century AD. Already the objects from the late Iron Age do not fall outside the range of Pb isotope ratios of the Massif Central deposits. Therefore, it can be assumed that the brass production might have started in the Massif Central as early as around the middle of the 1st century BC. The existence of Gallic brass coins from the time of Caesar's military campaigns in Gaul supports this hypothesis [61]. Also, there is evidence of large-scale exploitation of gold in the Massif Central that took place already before the Roman conquest [82, 83, 84]. It is generally accepted that the Romans benefited from the developed tradition of local Gallic mining [79]. The importance of natural resources in the Massif Central for the expanding Roman Empire is underlined by the intensive iron production around the Montagne Noire area that became significant in the 1st century AD. According to archaeometric analyses, local iron was distributed widely via long-distance trade and served as a vital source of material for the Roman army [85, 86]. The influx of brass to the territories north of the Alps occurred as early as in southern Europe and the Gaul, thus indicating the instant popularity of the new and attractive material. The earliest evidence of brass used in diplomatic contacts with the indigenous populations can be already seen in the late Iron Age. The nature of its distribution mechanisms is hard to evaluate, but in that period, brass was still a rare commodity. Massive-scale and, perhaps more importantly, a regular occurrence is dated no earlier than the Augustan and Tiberian Era. Brass became a ubiquitous yet still highly valued commodity in Germanic society. Its special social status was derived from its distinctive visual qualities and, initially, its exclusive Roman provenance. The level of dependency of the Barbarian society on an external material supply from the Romans seems to be very high. Based on the current scientific evidence, the importance of brass in political relations between the Romans and Barbarians, possibly similar to the role of the silver coins in northern Britain [87] can be assumed. This material with the connotations of prestige and luxury could serve as an effective medium in determining the quality of relations among different Barbarian groups. The 'value: cost-effectiveness ratio' for the material such as brass seems to have played in the Roman favour. The archaeological evidence from other regions beyond Bohemia suggests that a similar strategy of diplomatic contacts may also apply to other territories where early Roman brass objects occur (i.e. Slovakia, Poland, Germany) [88]. Given the sufficient influx of the Roman brass into the Barbarian territories, the recycling has not affected the geochemical properties attributed to the original Roman aurichalcum as much as is observed for materials from the 2nd century AD [60, 89]. Only the samples from the earliest phase of the Early Roman period (R A) may have had their Pb isotope ratios influenced by Iberian Cu sources. A specificity of data from the latest phase (R B2) could be explained at this point by exploitation of different deposits in the Massif Central than in the early stages of brass production. Such a hypothesis is also supported by the 2nd century AD brass ingots from the shipwreck of Aléria that share the Pb isotope signature with our samples and is also thought to be produced in the Massif Central. The volume of material entering the Germania Magna in the Early Roman period is hard to estimate and represents a research topic on its own. There have been some rough estimations in the work of Becker [90] for the Barbarian territory of the late Roman Germania, which led to an estimated 2.5 tons of material just for brooches. Given the larger dimensions of the Early Roman brooches compared to Late Roman types, plus the overall abundance of the metallic goods in the Early Roman graves, the quantity of consumed material must have been probably higher than that estimated. 6. Methods Selected objects were drilled to the metal core to avoid the corrosion layers and collect the minimum sufficient amount of material for the chemical and Pb isotope analyses. Due to the small sizes of the objects and the high corrosion stage of some, the sample weight varied between 0.01 and 0.05 g. Because of the sample preparation methodology, As contents were not determined. Samples of drilled-out bronze/brass materials were carefully weighed into pre-cleaned Savillex beakers, dissolved in a mixture of 6M HCl–7M HNO 3 (3:1 v/v) with several drops of 23M HF and placed on a hotplate for 24 hours at 50°C. For the measurements of element abundances, freshly prepared solutions were dried down and re-dissolved in 2% HNO 3 . The abundances of selected elements were determined using an Agilent 7900x inductively coupled plasma mass spectrometer (ICP-MS), housed at the Czech Geological Survey. The chemical procedures for Pb isolation and purification employed two chromatographic columns. The first step was modified from Pin et al. [91] and used pre-cleaned and pre-conditioned Sr.Spec resin (50–100 mesh; Triskem, France) packed in 0.2 mL columns. Samples were dried down and re-dissolved in 2M HCl. Lead was eluted with 6M HCl. The second step employed anion-exchange resin BioRad AG 1x8 (100–200 mesh) combined with HCl and HBr as elution media, following the methodology outlined in Romer et al. [92]. The eluted Pb fraction was then dried down and repeatedly re-dissolved with 50 µl 14M HNO 3 to remove any residual organic material. Prior to Pb isotope measurements, the dried Pb fractions were re-dissolved in 1 mL 2% HNO 3 and doped with Tl solution (NIST SRM 997; 205 Tl/ 203 Tl = 2.3871). Lead isotope compositions were determined using an Aridus 2 desolvating unit (Cetac) coupled to a Neptune multi-collector ICPMS (ThermoFisher), housed at the Czech Geological Survey, in static mode. Sample analysis followed a conventional standard–sample–standard bracketing protocol in which the SRM-981 reference material solution was run after every unknown sample. Potential 204 Hg isobaric interference on 204 Pb was monitored at mass 202 Hg and corrected by assuming natural Hg isotope ratios ( 202 Hg/ 204 Hg = 4.35). Correction of the measured Pb isotope ratios for mass discrimination utilised a generalised power law and natural isotope composition of Tl [93]. The results were then normalised off-line to the certified values for SRM 981, and the combined statistics for three measurements of each unknown sample were calculated. Data represent the uncertainty-weighted mean of three replicate measurements. Repeat measurements of NBS 981 yielded mean 206 Pb/ 204 Pb, 207 Pb/ 204 Pb and 208 Pb/ 204 Pb ratios of 16.942 ± 0.003, 15.4998 ± 0.0030 and 36.725 ± 0.007 (2SEM, n = 66), respectively. Samples dated into the La Tène period and comparative Iron Age samples were processed with a slightly different methodology detailed elsewhere [28]. For consistency in the data evaluation, the ore deposits data were prepared for the comparative analysis by removing multivariate outliers detected using the Mahalanobis distance [68]. This step is a prerequisite to fitting linear models to the data or using any other method to visualise the trends. By outliers, we understand data points with extreme values regarding the shape of the whole data distribution in a multidimensional setting defined by lead isotopic ratios ( 206 Pb/ 204 Pb, 207 Pb/ 204 Pb, 208 Pb/ 204 Pb, 207 Pb/ 206 Pb and 208 Pb/ 206 Pb, respectively). Declarations Acknowledgements This work was supported by the Czech Science Foundation project 18-20096S [Mobility of materials and life cycles of artefacts: archaeometry of metals and glass of the La Tène and Early Roman period]. TM, JM and ZR contributed through the Strategic Research Plan of the Czech Geological Survey (DKRVO/ČGS 2018–2022). Authors' contributions AD and DB designed the research project (Grant 18-20096 S). DB, AD and TM performed statistical analyses, were responsible for the interpretation of the data, designed the manuscript and the figures. PP performed provenance and comparative analyses. TM, JM and ZR performed the analyses of Roman period samples. TM supervised the data quality. JT and LS contributed with the measurements of La Tène period samples. References [1] Craddock, P. T. The composition of the copper alloys used by the Greek, Etruscan and Roman civilizations. Journal of Archaeological Science 5 , 1–16 (1978). [2] Hanel, N., Bode, M. 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Rapid, simultaneous separation of Sr, Pb, and Nd by extraction chromatography prior to isotope ratios determination by TIMS and MC-ICP-MS. Journal of Analytical and Atomic Spectrometry 29 , 1858–1870 (2014). [92] Romer R. L. et al. Elemental dispersion and stable isotope fractionation during reactive fluid-flow and fluid immiscibility in the Bufa del Diente aureole, NE-Mexico: evidence from radiographies and Li, B, Sr, Nd, and Pb isotope systematics. Contributions to Mineralogy and Petrology 140 , 400–429 (2005). [93] Košler J., Forst L. & Sláma J. Lamdate and lamtool: spreadsheet-baserd data reduction for laser ablation ICP-MS. In Sylvester, P. (ed.) Laser ablation ICP-MS in the Earth Sciences: current practices and outstanding issues. Short Course Series 40 , 315–317 (Mineralogical Association of Canada, 2008). [94] Almgren, O. Studien über Nordeuropäische Fibelformen der ersten nachchristlichen Jahrhunderte mit Berücksichtigung der provinzial-römischen und südrussischen Formen. (Kabitzsch / Leipzig, 1923). Tables Due to technical limitations, table 2-4 is only available as a download in the Supplemental Files section. Additional Declarations No competing interests reported. Supplementary Files SupplementaryinformationBrassmanuscript.docx Supplementary information Table2.pdf Table 2 Table3.pdf Table 3 Table4.pdf Table 4 Cite Share Download PDF Status: Under Review Version 1 posted Editorial decision: Major revision 13 Sep, 2021 Reviews received at journal 29 Jul, 2021 Reviewers agreed at journal 22 Jul, 2021 Reviewers invited by journal 22 Jul, 2021 Editor assigned by journal 22 Jul, 2021 Editor invited by journal 21 Jul, 2021 Submission checks completed at journal 21 Jul, 2021 First submitted to journal 14 Jul, 2021 You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-715158","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":40962632,"identity":"1305b693-04df-4b89-8226-8d6e36a4a30d","order_by":0,"name":"Daniel Bursák","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAxElEQVRIiWNgGAWjYBACAzB5wIZ0LWmkazlMghZzidzHH36cOS9vPiP3AMOPmjoG/v4D+LVYzkg3k+y5cdtwzo28BMaeY4cZJA4Q0GJwI42NgefDbcYZEjkGzAxsBxgMGBsIamH++OfDOXuIln91DECSoBYGaZ4bBxLBWhjbmBkM2Ahosex5xiYtcyY5eQbPu4SDvX2HeSTOENBizg502JtjdrYz2HMPPvjxrU6OYIghAR6GA2CSBECS4lEwCkbBKBhJAAAgC0Dr6pF/zwAAAABJRU5ErkJggg==","orcid":"","institution":"Institute of Archaeology CAS","correspondingAuthor":true,"submittingAuthor":false,"prefix":"","firstName":"Daniel","middleName":"","lastName":"Bursák","suffix":""},{"id":40962633,"identity":"d0ed053d-ff7a-4e9c-ad5e-94a17c30bd74","order_by":1,"name":"Alžběta Danielisová","email":"","orcid":"","institution":"Institute of Archaeology CAS","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Alžběta","middleName":"","lastName":"Danielisová","suffix":""},{"id":40962634,"identity":"84309887-2a72-40a3-ac11-98ff1a04ccd7","order_by":2,"name":"Tomáš Magna","email":"","orcid":"","institution":"Czech Geological Survey","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Tomáš","middleName":"","lastName":"Magna","suffix":""},{"id":40962635,"identity":"613c81be-dfbc-43c4-a143-c79e6a50facc","order_by":3,"name":"Petr Pajdla","email":"","orcid":"","institution":"Masaryk University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Petr","middleName":"","lastName":"Pajdla","suffix":""},{"id":40962636,"identity":"1d190adc-351c-4bc5-b70d-26f107e55ed9","order_by":4,"name":"Jitka Míková","email":"","orcid":"","institution":"Czech Geological Survey","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Jitka","middleName":"","lastName":"Míková","suffix":""},{"id":40962637,"identity":"00057c9a-e9e2-419c-a977-b573376ea3ca","order_by":5,"name":"Zuzana Rodovská","email":"","orcid":"","institution":"Czech Geological Survey","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Zuzana","middleName":"","lastName":"Rodovská","suffix":""},{"id":40962638,"identity":"a0363851-6938-43be-bc08-630d5f402837","order_by":6,"name":"Ladislav Strnad","email":"","orcid":"","institution":"Charles University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Ladislav","middleName":"","lastName":"Strnad","suffix":""},{"id":40962639,"identity":"04f5952e-ba46-4f3e-a606-9fdeac3ec121","order_by":7,"name":"Jakub Trubač","email":"","orcid":"","institution":"Charles University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Jakub","middleName":"","lastName":"Trubač","suffix":""}],"badges":[],"createdAt":"2021-07-14 09:14:10","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-715158/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-715158/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":11749249,"identity":"5709cf66-f4a1-4a69-9c60-a544b2b0565b","added_by":"auto","created_at":"2021-07-23 17:20:03","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":666579,"visible":true,"origin":"","legend":"A: Geographical overview of Central Europe with main territorial units of the later Roman provinces (hatched areas) at the beginning of the 1st cent. AD; B: detail of the area of interest in Bohemia with sites providing samples for the analyses.","description":"","filename":"Fig1.png","url":"https://assets-eu.researchsquare.com/files/rs-715158/v1/aa7a7afb39aa0c0cc0065bc9.png"},{"id":11749244,"identity":"13f10205-9ea6-4f04-ae2f-713dd1d744a1","added_by":"auto","created_at":"2021-07-23 17:20:03","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":48700,"visible":true,"origin":"","legend":"Ternary diagram of the Zn, Sn and Pb contents of the Bohemian brass samples from this study categorised according to their dating. Zinc content is divided by a factor of 10, Pb content is multiplied by a factor 10. For categorisation according to the cultural groups see Suppl. 1.","description":"","filename":"Fig2.png","url":"https://assets-eu.researchsquare.com/files/rs-715158/v1/f31138db4bdc00faaf28799b.png"},{"id":11749320,"identity":"4a44b1f9-b403-44d9-a5dd-39fba071fb65","added_by":"auto","created_at":"2021-07-23 17:23:03","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":87158,"visible":true,"origin":"","legend":"Bi-plot of PCA results of the Bohemian brass objects from this study. Factor 1 versus Factor 2 is categorised according to A: the cultural groups B: dating.","description":"","filename":"Fig3.png","url":"https://assets-eu.researchsquare.com/files/rs-715158/v1/5b867099c117430da2e14b12.png"},{"id":11749248,"identity":"d6b37b4f-9db7-4e3d-8260-e67197a48a22","added_by":"auto","created_at":"2021-07-23 17:20:03","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":107985,"visible":true,"origin":"","legend":"Overview of lead isotope systematics of the Bohemian brass objects from this study categorised according to the A: dating B: groups defined by Zn content. For categorisation according to the cultural groups see Suppl. 3.","description":"","filename":"Fig4.png","url":"https://assets-eu.researchsquare.com/files/rs-715158/v1/92e6a03f33cedfccaa07bf8f.png"},{"id":11749242,"identity":"aec7e9ff-15b6-47b9-b184-fa922c50a7b6","added_by":"auto","created_at":"2021-07-23 17:20:03","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":96272,"visible":true,"origin":"","legend":"Bi-plot of Zn verus Sn + Pb content of the earliest brass objects from the 1st Century BC. For categorisation according to dating see Suppl. 4. Sources: [16, 17, 60] + this study.","description":"","filename":"Fig5.png","url":"https://assets-eu.researchsquare.com/files/rs-715158/v1/8e7dbd67a166efac5db4fe79.png"},{"id":11749321,"identity":"9bf74272-9c96-4214-8408-bc81e012a1d7","added_by":"auto","created_at":"2021-07-23 17:23:03","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":123184,"visible":true,"origin":"","legend":"Bi-plot of Ag verus Sb content of brass artefacts with \u003e 5 wt.% Zn from Bohemia and Cambodunum with the Roman brass coinage categorised according to the cultural and chronological groups. Sources: [60, 62], this study.","description":"","filename":"Fig6.png","url":"https://assets-eu.researchsquare.com/files/rs-715158/v1/a2599882d4371b24ef872240.png"},{"id":11749251,"identity":"36fd7309-3ea9-4696-9764-64bed959ac93","added_by":"auto","created_at":"2021-07-23 17:20:03","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":122485,"visible":true,"origin":"","legend":"Overview of lead isotope systematics of ore sources from the northwest Mediterranean zone and the Bohemian brass objects categorised according to the cultural groups. Sources: see [2, 22, 27, 28, 35, 70, 76, 71].","description":"","filename":"Fig7.png","url":"https://assets-eu.researchsquare.com/files/rs-715158/v1/b6da1405b6230d4bd5d5a245.png"},{"id":11749254,"identity":"f6590d7a-6b18-437b-a9cc-a10a62840b0b","added_by":"auto","created_at":"2021-07-23 17:20:03","extension":"png","order_by":8,"title":"Figure 8","display":"","copyAsset":false,"role":"figure","size":381802,"visible":true,"origin":"","legend":"Euclidean (ED) and Mahalanobis (MD) distances between lead isotope ratios of various sets of artefacts from the Early Roman period and the Bohemian brass objects. Sources: see description in text + this study.","description":"","filename":"Fig8.png","url":"https://assets-eu.researchsquare.com/files/rs-715158/v1/4c460725090954d878333ab6.png"},{"id":11749323,"identity":"3c0c2422-653a-4c8c-8b2c-8aade251b76a","added_by":"auto","created_at":"2021-07-23 17:23:03","extension":"png","order_by":9,"title":"Figure 9","display":"","copyAsset":false,"role":"figure","size":212525,"visible":true,"origin":"","legend":"Analysed samples with captions corresponding to the sample description in the table 2-4.","description":"","filename":"Fig9.png","url":"https://assets-eu.researchsquare.com/files/rs-715158/v1/31d7c9028e7b11d818c85830.png"},{"id":13705342,"identity":"db153143-fcde-473a-abbf-75e4b3c4067d","added_by":"auto","created_at":"2021-09-17 13:51:24","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2025308,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-715158/v1/96804671-ed6e-4053-b613-55de3c6a0d33.pdf"},{"id":11749246,"identity":"2f93ac73-f4ec-4051-b5d4-ce47240fc3f6","added_by":"auto","created_at":"2021-07-23 17:20:03","extension":"docx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":2918481,"visible":true,"origin":"","legend":"Supplementary information","description":"","filename":"SupplementaryinformationBrassmanuscript.docx","url":"https://assets-eu.researchsquare.com/files/rs-715158/v1/26172c578d8ecc3bfd5c552f.docx"},{"id":11749245,"identity":"9708cba7-c1f4-4893-95a5-fde96b2b3943","added_by":"auto","created_at":"2021-07-23 17:20:03","extension":"pdf","order_by":2,"title":"","display":"","copyAsset":false,"role":"supplement","size":217445,"visible":true,"origin":"","legend":"Table 2","description":"","filename":"Table2.pdf","url":"https://assets-eu.researchsquare.com/files/rs-715158/v1/a69e1d7788355910dbd5f74c.pdf"},{"id":11749319,"identity":"ad32afc6-b4e4-4129-8f80-861ea5f4e482","added_by":"auto","created_at":"2021-07-23 17:23:03","extension":"pdf","order_by":3,"title":"","display":"","copyAsset":false,"role":"supplement","size":188393,"visible":true,"origin":"","legend":"Table 3","description":"","filename":"Table3.pdf","url":"https://assets-eu.researchsquare.com/files/rs-715158/v1/c463186cd8c8323a1ed88c08.pdf"},{"id":11749322,"identity":"42fa8d2f-6798-4c1d-82d5-82fafb3d3221","added_by":"auto","created_at":"2021-07-23 17:23:03","extension":"pdf","order_by":4,"title":"","display":"","copyAsset":false,"role":"supplement","size":175896,"visible":true,"origin":"","legend":"Table 4","description":"","filename":"Table4.pdf","url":"https://assets-eu.researchsquare.com/files/rs-715158/v1/63c358db045ea31a9b79c31b.pdf"}],"financialInterests":"No competing interests reported.","formattedTitle":"\u003cp\u003eShining Like Gold and New: The Emergence of Brass North of the Alps Around the Turn of the Era.\u003c/p\u003e","fulltext":[{"header":"1. Introduction","content":"\u003cp\u003eBrass is undoubtedly one of the most valued materials in Antiquity. Its high appreciation is underscored by the written sources, particularly in Pliny the Elder\u0026apos;s and Cicero\u0026apos;s works [1, 2]. Since the discovery of Zn-rich alloys in the material culture of the Early Roman period, several studies have summarised its origins, the technological process of its fabrication by the Romans and its importance during that time [3, 4, 5, 6, 7]. It appears that the widespread distribution of brass is connected with the period of the reign of Augustus and his coinage reform in 23 BC.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eThe earliest brass objects in Bohemia are represented by a brass \u003cem\u003efourr\u0026eacute;e\u003c/em\u003e (counterfeit) stater from the oppidum of Stradonice [8], brass Almgren 65 brooch from the oppidum of Z\u0026aacute;vist, and several imported brass rings from the other oppida (Fig. 1, Table 2-4), all dated around the middle of the 1\u003csup\u003est\u003c/sup\u003e century BC and, except for the coin, supposedly the products of Roman workshops imported to the North as exclusive jewellery pieces [9]. However, there is still limited knowledge on the nature of trade with brass between the Romans and the indigenous populations (i.e . Celtic and Germanic tribes) beyond the Roman territories. The only known indication from this region is a hoard retrieved from the Rhine river, containing over 50 bars, with some of them made of brass [10]. The massive emergence of brass objects north of the Alps and in Bohemia in particular, almost unknown during the preceding La T\u0026egrave;ne period, corresponds well with a significant influx of Roman imports to the Barbarian territories in the Early Roman period, i.e. between the second half of the 1\u003csup\u003est\u003c/sup\u003e century BC and the first half of the 1\u003csup\u003est\u003c/sup\u003e century AD [11, 12, 13, 14, 15].\u003c/p\u003e\n\u003cp\u003eThe original brass produced by Roman workshops in the first half of the 1\u003csup\u003est\u003c/sup\u003e century BC with very distinctive composition and material properties has been referred to as \u003cem\u003ethe aurichalcum\u003c/em\u003e [1, 4, 7]. Thanks to modern analytical tools, there has been some progress in identifying brass manufacture (possibly from the Roman imports) in the broader area of Europe among the objects dated already to the early 60s BC; however, their geological provenance remained mostly undetected [16, 17, 2, 18, 9]. More recently, studies systematically dealing with the Pb isotope compositions of selected materials, such as copper [19, 20, 21, 22], lead [24, 25], and brass [2], have become available. It has been noted that the provenance analyses of ancient Cu from the Iron Age and later periods might be challenging due to the complexity of the interpretations imposed by numerous and often unknown resources, widespread material mixing, recycling, depletion, and other reasons. However, even if the determination of the exact origin of the objects in question proves to be difficult, the provenance studies remain to be a great source of information for the understanding of contemporary socio-economic networks that are often key to understanding the historical events [e.g., 25, 26, 27, 28].\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eThe historical framework of this study could be briefly outlined as a period starting with the decline of the late La T\u0026egrave;ne civilisation (conventionally linked with the Celts), around the middle of the 1\u003csup\u003est\u003c/sup\u003e century BC, followed by a massive migration wave(s) of the early Germanic tribes (Marcomanni, Quadi, and others) sometime between the second half of the 1\u003csup\u003est\u003c/sup\u003e century BC to the 2\u003csup\u003end\u003c/sup\u003e century AD [29, 9]. Beginning and the course of the Julio-Claudian dynasty with a distinct intensification of the Romano\u0026ndash;\u0026apos;Barbarian\u0026apos; contacts is the primary time frame for the majority of samples presented in this study [30, 31, 32, 33]. In this period, jewellery from the Germanic graves in Bohemia was identified to be made of high-quality brass, approaching the chemical composition of the original \u003cem\u003eaurichalcum\u0026nbsp;\u003c/em\u003e[15, 13, 4]. A possible Roman origin of the brass coming to indigenous territories was naturally assumed when these objects were first analysed [15]. Especially in the case of early Germanic brooches of the so-called \u0026apos;eye type\u0026apos; with ca. 20% Zn, it was proposed that recycled Roman imports, primarily brass coins, were used for their fabrication [13, 10]. All this makes Bohemia an exceptionally well-suited territory for studying brass production and circulation patterns compared to other \u0026apos;Barbarian\u0026apos; territories north of the Alps and east of the Rhine (Fig. 1). The striking richness and material diversity of copper-alloy objects in the Bohemian territory have frequently been related to the existence of the so-called Empire of Marobudus, a power structure that kept friendly relations with the expanding Roman Empire after the critical defeat of three legions in the Battle of the Teutoburg Forest in AD 9 [12, 34]. In that period, the Central European territory was at the intersection of the territorial interests of the expanding Roman Empire, new migration waves of the Germanic tribes from the North and the West, and the remainder of the late Celtic population. As such, this territory interconnected many cultural traditions manifested in the material culture. Those were especially the costume parts (brooches, belts, pins and other personal objects), imported luxury items such as bronze drinking vessels, tableware, and other objects.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eIn this study, we present new compositional and Pb isotopic data for the early Roman brass artefacts from the territory of Bohemia to initiate the discussion on the currently scarce archaeometric research on the early brass in Europe. The character of the Early Roman period bronze and brass is compared with the previous late Iron Age [27, 35, 28].\u0026nbsp;\u003c/p\u003e"},{"header":"2. Material","content":"\u003cp\u003e\u003cstrong\u003e2.1. Studied samples\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eIn total, 50 Late Iron Age and Early Roman period objects from the territory of Bohemia were sampled for geochemical analyses (Fig. 1). Most items come from metal detector prospections, so the information about their original context is scarce. Nonetheless, all samples can be characterised by localisation, typological determination, cultural provenance and dating (Table 1, 2). The selection of samples for further investigations was driven by identifying those objects among the cultural groups most likely fabricated from brass.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e2.2. Categorisation of samples\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eRich typological diversity of the finds led to a robust scholarly tradition in the past, which was aimed towards a thorough typo-chronological evaluation with much effort put into the detailed mapping, sequencing and cataloguing of the finds [36, 37, 38, 39, 40, 41, 42, 43, 44, 45, 46]. A vital research premise was to establish the general typo-chronological groups of personal jewellery and other objects, usually described as the \u0026apos;Western tradition\u0026apos; (i.e. Gallic and Rhenish), the \u0026apos;Danube tradition\u0026apos; (or Norico-Pannonian, Rhaetian), or in a more general sense the \u0026apos;Roman-provincial tradition\u0026apos;. Such categorisation represents a valuable methodological tool for working with archaeometric data because it can be used as independent evidence.\u003c/p\u003e\n\u003cp\u003eThe following cultural and chronological groups of brass objects were defined for the correlation with the geochemical analysis:\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e\u003cem\u003eLa T\u0026egrave;ne\u0026nbsp;\u003c/em\u003e\u003c/strong\u003e\u003cstrong\u003e(\u0026apos;LT\u003c/strong\u003e-\u003cstrong\u003eBrass\u0026apos;):\u0026nbsp;\u003c/strong\u003eobjects made in the late La T\u0026egrave;ne tradition of metallurgical production, usually carried out at the oppida or other major agglomerations (mainly in the Middle Danube area). Their chronological assessment and interpretation are based on a recent study of the late Iron Age in Bohemia [9]. This group\u003cstrong\u003e\u0026nbsp;\u003c/strong\u003econtains four brass objects: a late Almgren 65 type brooch and three imported brass rings of the Roman provenance (Fig. 9, Table 2).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e\u003cem\u003eLocal\u0026nbsp;\u003c/em\u003e\u003c/strong\u003e(\u0026apos;\u003cstrong\u003eL\u0026apos;\u003c/strong\u003e): objects generally supposed to be fabricated in the early \u0026apos;Barbarian\u0026apos; metallurgical tradition. This material culture commonly is associated with the Germanic tribes appearing in the Bohemian territory from the second half of the 1\u003csup\u003est\u003c/sup\u003e century BC. This group contains mostly personal objects, especially eye brooches of the Almgren 45-49 type [37, 47, 48].\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e\u003cem\u003eImport\u0026nbsp;\u003c/em\u003e\u003c/strong\u003e\u003cstrong\u003e(\u0026apos;I\u0026apos;):\u0026nbsp;\u003c/strong\u003efinds not of the \u0026apos;Barbarian\u0026apos; provenance; they usually are considered to be the diplomatic gifts brought to the Bohemian territory by trade, exchange or as booty from the territories controlled by the Romans [12, 49, 50, 51]. Because several different typological groups are included in this broad category, further subdivisions were needed, such as \u0026apos;Noric\u0026apos; and \u0026apos;Western\u0026apos;. Also, more ambivalent types in terms of the place of origin were included, such as Almgren 18 brooches, which are sometimes interpreted as being produced locally. Bohemian finds appear to be exogenous and ultimately connected with the populations that occupied the territory from the second half of the 1\u003csup\u003est\u003c/sup\u003e century BC [52].\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e\u003cem\u003eNoric\u003c/em\u003e\u003c/strong\u003e (\u0026apos;N\u0026apos;): objects made in the cultural tradition of the territories around the Middle Danube zone and the Eastern Alps, including the parts of the so-called \u0026apos;Norico-Pannonian costume\u0026apos; and finds mainly occurring in the territory of ancient Rhaetia (roughly the Alpine zone of today\u0026apos;s Austria). Brooches and other jewellery are thought to represent continuity from the preceding late La T\u0026egrave;ne costume tradition [36, 53, 40, 43].\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e\u003cem\u003eWestern\u003c/em\u003e\u003c/strong\u003e (\u0026apos;W\u0026apos;): this category has been used as a label for Alesia, Almgren 19 (including its subvariants), Almgren 15, and the so-called Gallic brooches of the types Feug\u0026egrave;re 13b, 19b and 19d. These objects mainly occurred around the Middle Rhine area or in eastern Gaul. To avoid ambiguity in cultural determination, some types, such as the Aucissa and Almgren 18, were categorised simply as \u003cstrong\u003e\u003cem\u003eImport\u003c/em\u003e\u003c/strong\u003e (\u0026apos;I\u0026apos;), indicating their non-Germanic provenance.\u0026nbsp;\u003c/p\u003e\n\u003cdiv align=\"center\"\u003e\n \u003ctable border=\"0\" cellpadding=\"0\" cellspacing=\"0\" width=\"0\"\u003e\n \u003ctbody\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" width=\"34.36293436293436%\"\u003e\u003cbr\u003e\u003c/td\u003e\n \u003ctd colspan=\"2\" width=\"27.99227799227799%\"\u003e\n \u003cp\u003eLa T\u0026egrave;ne period\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd colspan=\"3\" width=\"37.64478764478765%\"\u003e\n \u003cp\u003eEarly Roman period\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" width=\"34.36293436293436%\"\u003e\n \u003cp\u003e130/120\u0026ndash;70s BC\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd rowspan=\"2\" width=\"6.94980694980695%\"\u003e\n \u003cp\u003eLT\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" width=\"21.042471042471043%\"\u003e\n \u003cp\u003eLT D1a\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd colspan=\"3\" valign=\"top\" width=\"37.64478764478765%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" width=\"36.92946058091286%\"\u003e\n \u003cp\u003e70s\u0026ndash;50/40s BC\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" width=\"22.61410788381743%\"\u003e\n \u003cp\u003eLT D1b\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd colspan=\"3\" valign=\"top\" width=\"40.45643153526971%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" width=\"34.36293436293436%\"\u003e\n \u003cp\u003efrom 60s/40s\u0026ndash;20s/0 BC\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd colspan=\"5\" valign=\"top\" width=\"65.63706563706563%\"\u003e\n \u003cp\u003eLT D2 / R A\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" width=\"34.36293436293436%\"\u003e\n \u003cp\u003e10/5 BC\u0026ndash;AD 20/30\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd colspan=\"2\" valign=\"top\" width=\"27.99227799227799%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd rowspan=\"3\" width=\"11.583011583011583%\"\u003e\n \u003cp\u003eR B\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd rowspan=\"2\" width=\"7.915057915057915%\"\u003e\n \u003cp\u003eR B1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" width=\"18.146718146718147%\"\u003e\n \u003cp\u003eR B1a\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" width=\"42.68585131894484%\"\u003e\n \u003cp\u003eAD 20/30\u0026ndash;40/50\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd colspan=\"2\" valign=\"top\" width=\"34.77218225419664%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" width=\"22.54196642685851%\"\u003e\n \u003cp\u003eR B1b\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" width=\"38.8646288209607%\"\u003e\n \u003cp\u003eAD 50/70\u0026ndash;150/160\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd colspan=\"2\" valign=\"top\" width=\"31.65938864628821%\"\u003e\n \u003cp\u003e-\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd colspan=\"2\" valign=\"top\" width=\"29.475982532751093%\"\u003e\n \u003cp\u003eR B2\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003c/tbody\u003e\n \u003c/table\u003e\n\u003c/div\u003e\n\u003cp\u003eTable 1: Summary of the chronological system employed in the sample categorisation. The generally accepted chronological framework for the late La T\u0026egrave;ne [15] and the Early Roman period, respectively [54, 45, 29] were followed\u003c/p\u003e"},{"header":"3. Results","content":"\u003cdiv id=\"Sec6\" class=\"Section2\"\u003e \u003ch2\u003e3.1. Chemical composition\u003c/h2\u003e \u003cp\u003eFor comparison with data published elsewhere, all compositional data used in this work are presented in the form of the analytical totals normalised to 100 wt.%.\u003c/p\u003e \u003cp\u003eMost analysed samples are represented by alloys with Zn contents\u0026thinsp;\u0026gt;\u0026thinsp;15 wt.% (Suppl. 2). In terms of main alloying components, Pb, Zn and Sn (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e), variations, most likely compatible with their different chronology, are apparent. Zinc content in late Iron Age brass rings from the oppida were always ca. 20 wt.%. In the Almgren 65 brooch, the alloy also contains around 20 wt.% Zn. Very high Zn contents (median at 17 wt.%) on the one hand and very low Sn and Pb concentrations on the other are typical for the phase R B1 (10 BC-AD 50). There is a slight tendency towards more consistent and also higher Zn contents among samples towards the end of this phase (ca. AD 30\u0026ndash;50).\u003c/p\u003e \u003cp\u003eBrass with significantly lower Zn contents (2\u0026ndash;9 wt. %) was detected in categories of imports ('I') from the beginning of the Early Roman period (second half of the 1st century BC). These objects also have comparable contents of Zn and Sn. The second category with a similar position in the composition plot (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e; Suppl. 1) is partly represented by samples of the local ('L') origin that are usually dated around the middle of the 1st century AD (phase R B2). There are also two leaded Cu alloys: (i) a drinking horn fitting and (ii) a fragment of a handle of the Roman imported vessel (bronze decoration with a human mask). Four samples were detected to be made of Sn bronze without the addition of Zn. All belong to the 'L' category. A single case of a brooch (sample RIM008) with an exceptionally high amount of Ag at 20.8 wt. % is also reported.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003ePrincipal component analysis (PCA) was performed for a more detailed evaluation of the chemical composition. The choice of minor/trace elements (Pb, Co, Sb, Ag) has been made considering their symptomatic value for provenance studies [56, 57]. The resulting factor scores are plotted in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e. They clearly distinguish between the imported items ('I') and the rest of the samples, mainly due to the variability of the Zn content. The most extensive dispersion is observed in the category of local items ('L'), reflecting significant variations in the general composition of the used alloys (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e). Most samples in the 'N' category tend to have higher Ag contents (0.26\u0026ndash;1.2 wt. %) which may show consistency with their supposed Alpine origin (see below). A slightly negative correlation between Co and Ag was observed; however, there does not seem to be a clear correlation with the typo-chronological categorisation of samples (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec7\" class=\"Section2\"\u003e \u003ch2\u003e3.2. Lead isotope systematics\u003c/h2\u003e \u003cp\u003eLead isotope analysis shows similar results as the PCA (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e; Suppl. 3). The most significant variability is observed in the category of local items ('L'), followed by a slightly more homogeneous Norican ('N') group and the imports ('I').Samples in the 'Western' category ('W') form the tightest cluster, which is also coherent chronologically (phase R B1; Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea). Their linear trend and its spatial overlap are most similar with the cloud of the ores from the Massif Central (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003e). Almost all samples from the 'LT-brass' category are mutually close and show a significant consistency with the ore deposits in the western Mediterranean (i.e. Iberia) and the Massif Central in France. Sample TRS 003 is offset from the rest of the suite but still plots in the Pb isotope space of the Spanish or French deposits.\u003c/p\u003e \u003cp\u003eAll brass objects in the 'I' category (imports) are from the phase R A, and all of these samples show a tendency towards more radiogenic \u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb ratios. A tendency towards less radiogenic \u003csup\u003e207\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb and \u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb ratios is observed for items from the chronologically youngest period (R B2). A costume pin sample RIM 001 made of brass with high Zn content (\u0026gt;\u0026thinsp;15 wt.%) represents an 'outlier' with the lowest \u003csup\u003e207\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb. A clear tendency of samples with low Zn content (\u0026lt;\u0026thinsp;5 wt.%), dated either in the earliest or in the latest phase (R A or R B2), owards less radiogenic \u003csup\u003e207\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb values is apparent (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb). The samples from the phase R B1 with high Zn contents appear to be dispersed around \u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb ratio of 15.68 and are relatively homogeneous. Lead-rich (~\u0026thinsp;5 wt.%) imported vessel has the same Pb isotope systematics as the high-Zn low-Pb items from the phase R B1. A drinking horn fitting with the highest Pb content of 9.5 wt. % plots separately with \u003csup\u003e207\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb and \u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb ratios of 18.55 and 15.65, respectively.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e"},{"header":"4. Discussion","content":"\u003cp\u003eThe original \u003cem\u003eaurichalcum,\u003c/em\u003e i.e. the brass produced in Rome, must have contained at least 22\u0026ndash;28 wt.% Zn [4]. In fact, the content of Zn in aurichalcum started to decrease already in the 1\u003csup\u003est\u003c/sup\u003e century AD and later produced aurichalcum further continued to lose its original qualities [58]. In parallel to such compositional evolution on the Roman side, lower Zn contents in Barbarian objects measured here can be attributed to local mixing and recycling of the imported objects. It was shown that alloy with the Zn content between 10 and 15 wt.%, that could be produced by a simple dilution process of equal quantities of bronze and the \u003cem\u003eaurichalcum,\u003c/em\u003e already got its typical golden colour that was in demand among the indigenous communities [1, 59, 4]. This characteristic feature was favoured for producing the costume parts such as brooches, rings, pins and belts made both in Roman and Barbarian cultural environments. However, geochemical data for metal finds from the Barbaricum are still sparse, particularly those of the local (i.e. Germanic) provenance. In order to reveal further details about the manufacturing of brass in the indigenous territories, the assemblage analysed in this study was compared with chronologically and typologically compatible data from published reports.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e4.1. Comparison with contemporary assemblages\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe comparative dataset of chemical compositions included early Roman finds from Bohemia (NAA method, [15]) and Cambodunum (AAS method, [60]), both analysed in the 1990s, brass brooches from the territory of Slovenia (PIXE method, [16, 17]) and\u0026nbsp;brass staters from Gaul (FNAA, [61]).\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eDue to the currently followed hypothesis about the Roman brass used for the fabricating costume parts in the Barbaricum, chemical data from the brass coinage [62] were used for a more detailed comparison. The latest data for the Roman brass coinage were obtained by PIXE and,\u0026nbsp;unfortunately, do not provide sufficiently accurate results for the comparison.\u003c/p\u003e\n\u003cp\u003eWhen comparing the earliest brass objects from the 1\u003csup\u003est\u003c/sup\u003e century BC, the main alloying components (Zn, Sn, Pb) reveal a cluster of late Iron Age brass staters of VERCA and Vercingetorix CAS series because of their lower mean Zn content (ca. 12.2 wt.%; Fig. 5). The difference between coins and other brass objects is probably due to chronology because the \u0026apos;pure\u0026apos; brass, with high Zn content (\u0026gt;15 wt.%), and low contents of Sn and Pb (sum below 0.5 wt.%) appeared no earlier than around the 0 BC/AD. Simultaneously, there is evidence of Zn-rich brass in the second half of the 1\u003csup\u003est\u003c/sup\u003e century BC (phase R A).\u003c/p\u003e\n\u003cp\u003eA second PCA with only selected trace elements (Co, Ni, Sb, Ag) was carried out with the comparative datasets. To avoid inconsistency, the dataset was reduced to brooches only. This step further enhanced the chronological compatibility among the typological groups of objects. Also, in the archaeological categorisation of groups, several trends were revealed (Suppl. 5a). Similarly to \u0026apos;N\u0026apos; samples from Bohemia, also Norican brooches tend to contain more Ag, which is paralleled by higher contents of Sb, thus indicating fahlore copper used for their fabrication. The most significant trace element composition variability was observed for the local items (\u0026apos;L\u0026apos;). Chronologically speaking, a notable heterogeneity in the chemical composition may be observed in the phase R B1a compared to the following phase R B1b (Suppl. 5b). A specific group of objects of the Norican tradition from the phase R B2 forms a tight cluster in both plots. These findings indicate rather heterogeneous supply patterns of brass in the beginnings of the trade contacts between the early Empire and the Germanic communities, compared to the late Republic and Celtic agglomerations on the one hand and later part of the 1\u003csup\u003est\u003c/sup\u003e century AD on the other.\u003c/p\u003e\n\u003cp\u003eWhen these results are compared with the Roman copper AES coinage, a slight correlation between the part of the Bohemian samples from the phase R B1a and the AES coinage group pattern III (EPG III), characterised by increased levels of Sb and Ag, is apparent [19]. Similar Sb- and Ag-rich copper coinage is also specific for the Lyon altar series I (LAS I) AES coinage [63]. These groups are also compatible with the dating of Ag-rich Norican samples in this study. However, the Sb levels of samples from Bohemia do not exceed 0.2 wt. %, which is the lowest level of AES coinage EPG III. There might have been an issue with partial volatilisation of Sb if the material had been repeatedly remelted to produce brass alloy and then possibly remelted again to fabricate the final artefact [68]. Nevertheless, in this case, high levels of Zn and only marginally lower Sb appear to exclude multiple re-processing of brass. Therefore, raw materials for AES coinage [19, 63] and brass objects from this study are less likely to come from the same source.\u003c/p\u003e\n\u003cp\u003eThe comparison of brass artefacts with \u0026gt; 5 wt.% Zn from Bohemia and Cambodunum [60] with the Roman brass coinage [62] is based on the Sb versus Ag bi-plot (Fig. 6). It clearly shows incompatibility between the local brass artefacts and the Roman \u003cem\u003esestertii\u003c/em\u003e. Due to analytical differences, the data must, however, be treated with caution. Also, a significant variability of the Roman metal supply for the coin production [cf. 20] must be taken into account. Therefore, for successful future provenance studies, a targeted archaeometric analysis of the Roman coins is vital.\u003c/p\u003e\n\u003cp\u003eA brooch with unusually high Ag content (20,8 wt. %) is, generally speaking, uncommon - even in the context of the broad spectrum of Early Roman finds from Central Europe [13, 60]. Still, there are artefacts made of pure silver known from the contemporary cemeteries, and particularly this type of brooch (Almgren 24) is the one most frequently fabricated objects from precious metals [48, 64]. Considering the technologically advanced metallurgy \u0026ndash; both Roman and Barbarian \u0026ndash; unintentional contamination caused by the accidental use of silver-rich ore is highly improbable. An explanation of local manufacture with deliberate alloying with silver is thus plausible\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e4.2.\u0026nbsp;\u003c/strong\u003e\u003cstrong\u003eProvenance analysis\u0026nbsp;\u003c/strong\u003e\u003cstrong\u003e\u0026ndash; mineral exploitation and raw resources in the Early Roman period\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eLead isotope analysis has become a prevalent method for tracing the archaeological artefacts containing lead to their possible geological origins, i.e. the ores they were fabricated from [65, 66].\u0026nbsp;The provenance analysis testing the consistency between the samples and the known ore deposits was carried out using a combination of the conventional biplots and the Euclidean (ED) and Mahalanobis (MD) distance algorithms [28]. The same approach was then applied to compare the contemporary bronze and brass assemblages of various cultural backgrounds.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eED has initially been suggested by Stos [67] as a simple metric to compare how far the point distributions are from one another in a multivariate space defined by individual isotopic signals. While ED is currently widely used, it is advised to be complemented with MD in which the effects of the shape, scale and trend of the distribution of the data are accounted for [68]. Therefore, the metric is capable of measuring the distance from a data point to distribution in the multivariate space and can account for the distance of points as well as for the linear trends in the data and distributions of the data clouds. Derived plots\u0026nbsp;(Fig. 8; Suppl. 6) are\u0026nbsp;used to predict the allocation of analysed brass objects from Bohemia into the comparative datasets. Because of considerable overlaps in the data distributions of different ore deposits, it should be kept in mind that the predictive value of ED + MD can vary from one source to another.\u003c/p\u003e\n\u003cp\u003eThe best level of consistency for most of our samples is observed with polymetallic deposits from the Massif Central (Fig. 7;\u0026nbsp;Suppl. 6, 7). These results were verified by both the ED and MD; however, the outliers in the Massif Central ore dataset provided a less pronounced consistency than the standard biplot. There is also a possibility of mixing the sources from various deposits, namely the Mediterranean (Iberia, Sardinia, Macedonia, or Attica) or the Alpine (namely the south-eastern Alps and the Inn Valley; Suppl. 6; Suppl. 7). The Alpine signal is the strongest in the \u0026apos;N\u0026apos; category. British ores did not come into consideration until AD 43 when Britain came under Roman control, so these data were omitted for historical reasons.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eBecause of their analytical match with the Massif Central, the geochemical data from early Roman imperial Pb objects were included in the comparative analysis: the Augustan Pb water pipes from Pompeii [code \u0026apos;Pb pipes\u0026apos;; 69] and Pb ingots from the shipwreck of Sainte Maries de la Mer [code \u0026apos;Pb ingots\u0026apos;; 70]. A similar analytical match and subsequent historical interpretation favouring the Massif Central deposits were suggested for brass ingots from the Al\u0026eacute;ria shipwreck [code \u0026apos;Cu-Zn Ingot\u0026apos;; 2].\u003c/p\u003e\n\u003cp\u003eBecause no Pb isotope data for the artefacts of the \u0026apos;Barbarian\u0026apos; provenance are available, only the early Roman Imperial datasets could be included in the comparative analysis. Regarding the provenance of Cu, there is an extensive corpus of comparative data from the Roman AES coinage [20, 63] and Cu ingots of the Sud-Lavezzi 2 Bonifacio wreck from the beginning of the 1\u003csup\u003est\u003c/sup\u003e century AD [21]. Finally, since one of our aims was to detect possible consistency between the Germanic finds and the preceding late Iron Age artefacts, to detect potential looting of the abandoned Celtic oppida by the newly incoming Germanic populations, bronze objects mainly from the 1\u003csup\u003est\u003c/sup\u003e century BC (\u0026apos;Oppida\u0026apos; set) were also included in the comparative dataset [27, 28, 35].\u003c/p\u003e\n\u003cp\u003eThe results show that the Pb isotope compositions of most of the Early Roman samples in this study are generally inconsistent with late Iron Age finds (cf. results of ED and MD, Fig. 8; Suppl 8). A part of samples, consisting mostly of samples dated to the La T\u0026egrave;ne period or late 1\u003csup\u003est\u003c/sup\u003e and/or 2\u003csup\u003end\u003c/sup\u003e century AD with less radiogenic \u003csup\u003e207\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb and \u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb ratios are closer to deposits in Germany, and are consistent with Roman Cu coins, Cu-Zn, Pb ingots and part of the copper AES coinage from the LAS I. There is no analytical match with the Cu bars from Sud-Lavezzi 2 Bonifacio wreck, although the Cu bars might be a very convenient and contemporary source of copper. The group of samples with low Zn contents (Fig. 2) from the R A and R B2 phases and their tendency towards less radiogenic \u003csup\u003e207\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb ratios (Fig. 4b) are still within the range of the ores from the Massif Central. However, three out of four samples from the early phase (R A) show some proximity towards the south-eastern Iberian zone, most compatible with the late La T\u0026egrave;ne samples [27]. Sample RIM017 with a lower \u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb ratio contradicting this chronological explanation could be dated into the phase R B1 as well (Table 2, 3). The LAS I is consistent with part of the Bohemian samples in their Pb isotope ratios and the Ag content [63]. A tendency towards less radiogenic \u003csup\u003e207\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb and \u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb ratios may result from the influence of the Iberian Massif (Suppl. 8). The southern Spanish mines are thought to be the most important in the organisation of the Roman Cu supply [20], which is also\u0026nbsp;evidenced\u0026nbsp;by the most chronologically compatible dataset - the imperial AES copper coinage. Data from the AES coinage are partly inconsistent with Cu ingots, but the variability of Cu sources corresponds well with the suggested complexity of the Cu industry of the Roman Empire [21]. In the case of samples from the phase R B2, i.e. after 43 AD, Pb-Zn deposits from Great Britain may also come into consideration [cf. 2]. Since the amount of data from this late phase is low, further historical analysis, such as the trend comparisons with discussed ore deposits, cannot be performed.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eTo sum up, there are three most distinctive analytical matches in terms of possible ore resources. All these scenarios are generally historically plausible and can be thus discussed further:\u003c/p\u003e\n\u003cp\u003e(i) The mixing of Mediterranean sources has been thoroughly discussed for the Pb pipes from Pompeii, which had Pb isotopic signature close to the samples from this study (Fig. 8) [69]. The authors interpreted lead from Pompeii as a mixture of Sardinian, Iberian and Laurion ores; however, as recently pointed out [71], the possibility of the involvement of the Massif Central ores was initially omitted from the discussion. Considering the original \u0026apos;mixing scenario\u0026apos;, a more satisfying explanation for Pb in the Pompeiian pipes would favour the Cartago Nova deposits with a minor influence from Sardinian ores [71].\u003c/p\u003e\n\u003cp\u003e(ii) The Alpine origin of brass is unsupported because of the lack of clear historical evidence of Roman copper or lead mining in this region. There is a partial Pb isotope overlap with the deposits from the Central Alps (Valais) that may be associated with the \u0026apos;Sallustian\u0026apos; copper, mentioned by Pliny the Elder, and linked to the Haute Savoie (Suppl. 6, 7), which was discussed in the context of the chemical composition of Lyon alter series AES coinage. This explanation, however, was abandoned because of the inconsistency of the LAS coinage with the Pb isotope ratios of given deposits [63]. A slight correlation of the chemical composition and Pb isotope compositions of the \u0026apos;N\u0026apos; category of samples can be considered for geographical reasons, but this consistency is far from being solid.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003e(iii) According to Leblanc\u0026apos;s [72] map, the Pb-Zn mineralisation in the Massif Central is spread from Les Malines to Lyon, where the production of brass is dated from the middle of the 1\u003csup\u003est\u003c/sup\u003e century AD to the beginning of the 2\u003csup\u003end\u003c/sup\u003e century AD [73, 74]. The south-eastern part of the Massif Central is rich in various Cu-bearing ore bodies with specific combinations of the trace elements, for example, ophiolites (Ni, Co, Ag), pyrite ores (Ag, Au), Permo-Triassic (As, Pb, Ag), and Hercynian veins (Sb-Ag-Pb) with the Salsigne type mineralisation (As, Bi, Au) [72].\u0026nbsp;The connection of the polymetallic deposits in the Massif Central [72, 75] with the Roman lead metallurgy has been suggested earlier [70]. To support this argumentation, six samples in this study that are made of Sn-bronze, Pb-bronze or Ag-rich bronze, i.e. without any cementation process possibly taking place, still have their Pb isotope compositions consistent with the Massif Central ores, and we may thus assume that even Cu was extracted in the same region. A specific mining site, consistent with the Pb isotopic data from this study, cannot be assigned because the available data cover the entire Pb isotope diversity of the Massive Central ore deposits [71]. At present, this dataset appears to bear similarity with Pb isotope I values from the\u0026nbsp;Les Malines Pb-Zn deposit [75].\u0026nbsp;Whether the deposits in the Cev\u0026eacute;nnes area also served as a Cu source remains unclear [2].\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e4. 3. Consideration of possible contamination\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eA particular methodological risk should be considered when comparing brass objects with possible Cu ores because Zn ores, as an essential constituent of the produced brass, may also contain trace amounts of Pb [6, 2, 76, 77]. The inclusion of such Pb may then disturb or obscure the Pb isotope signature of the intrinsic Cu source during the cementation process [78]. There is also the uncertainty on how exactly and how much the cementation medium had impacted the trace element composition, which is crucial for the correct interpretation of the chemical composition of the analysed brass objects. So far, it is known that at least Fe and As can enter Cu metal during the cementation process [78]. In Roman Imperial workshops, where a very pure Cu was manufactured due to the advanced refining [19], the risk of contamination could be exceptionally high. Therefore, it must be acknowledged that the Pb isotope signal from the samples may point to the Pb-Zn source ore instead of the Cu ore [cf. 2]. Furthermore, the hypothetical contamination during the cementation process could strongly influence the comparison of Roman Cu coins and brass artefacts based on trace elements such as Sb and Ag. These notions, however, require carefully controlled metallurgical experiments. We assume that the cementation process was carried out using Zn in Pb-Zn ore rather than Zn in the form of ZnO, typically developed in furnaces during the pyrotechnological process [cf. 6]. The Pb contents in brass samples from this study are significantly higher than those in the LAS I coinage [63], representing at present the purest available copper from the Massif Central.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e4.4. Roman brass production in the Massif Central\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eArchaeological evidence for copper mining in the southern Massif Central during the Roman period is still rare; however, two sites in the Cav\u0026eacute;nes area served as Cu mines during the late 1\u003csup\u003est\u003c/sup\u003e century BC and early Imperial period [79]. One deposit around Carcassone, exploited during the later Roman Republic (2\u003csup\u003end\u003c/sup\u003e and 1\u003csup\u003est\u003c/sup\u003e century BC), has also been documented [80, 63]. In general, there always is a possibility of missing archaeological evidence of past extraction activities due to medieval and later mining that may have obscured or eradicated the traces of earlier exploitation. Therefore, clear evidence of the Gallic metal supplies is still missing [24].\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eThe best evidence for the early Roman (i.e. Augustan period) mining in the Massif Central is the Pb isotope analysis of the AES coinage of the so-called Lyon altar series I [63], supposedly originating in the\u0026nbsp;C\u0026eacute;vennes\u003cstrong\u003e\u0026nbsp;\u003c/strong\u003epart of the Massif Central. Despite the fact that a part of the Roman brass coin production took place in the Lugdunum (Lyon) mint [63], similarly to Pb ingots of Santa Maria and partially also to Pb pipes from Pompeii, an Iberian origin was initially expected. However, as the chemical analysis of further Lyon altar series coins (the LAS II collection of the AES coinage) indicates, the Gallic production alone might not have been sufficient for the great demand for Cu during the reign of Augustus, and another Cu source (possibly of the Iberian origin) was thus used for this other series of ases [63]. From the historical perspective, there has been a suggestion that copper used for coins of the LAS I may have been the \u0026apos;Livian\u0026apos;\u003cem\u003e\u0026nbsp;\u003c/em\u003eGallic copper, mentioned by Pliny the Elder, as one that was quickly depleted [63].\u003c/p\u003e\n\u003cp\u003eIt should be noted that also other Pb objects have been assumed to originate in the Massif Central, including the artefacts found in Germania [23]. Recently, another assemblage of Roman and Byzantine Cu and Cu-alloy coins \u003cem\u003enummi minimi\u003c/em\u003e from the 4\u003csup\u003eth\u003c/sup\u003e \u0026ndash; 8\u003csup\u003eth\u003c/sup\u003e century AD was found to be consistent with the deposits in the Massif Central, suggesting a long-term mining tradition of local mineral resources [81]. On the other hand, critical notes have also cast some doubt on the Lyon crucibles, pointing out their lack of technical properties [6]. Nevertheless, based on the reasons presented above, we are confident that our data, in fact, indicate the early Roman cementation in the south-eastern part of the Massif Central, and the increasing evidence for the Imperial exploitation of Cu, Zn and Pb in general [63, 70] supports the original interpretation of the Lyon crucibles [73, 74].\u003c/p\u003e\n\u003cp\u003eThe origin of most of the brass found in Bohemia in the Massif Central, and possibly their fabrication directly in Lyon, is not entirely impossible, as it is in accordance with the recent research, regularly pointing out the Gallic production [70, 23, 63, 2]. Consistency of these deposits with the data from an entirely different cultural tradition may appear surprising at first; however, they only point out the complexity of the socio-economic networks and the organisation of the metal supplies taking place already in the Early Roman period. Given the presence of the mint in Lugdunum (Lyon), a hypothetical origin of brass for the imperial coinage in the Massif Central seems to be very likely and should be verified by further analyses. The proximity of numerous rich ore deposits to Lugdunum was undoubtedly crucial for its economic importance. These indices could have been underestimated before the publication of geochemical data from this area that supported the ancient exploitation of local resources. Furthermore, the consistency of the Pb isotope compositions \u0026nbsp;with samples from the late Iron Age may indicate a long-distance distribution of these mineral resources as soon as around the middle of the 1\u003csup\u003est\u003c/sup\u003e century BC, i.e. the time directly around Caesar\u0026apos;s military campaigns in Gaul.\u0026nbsp;\u003c/p\u003e"},{"header":"5. Conclusions","content":"\u003cp\u003eThe majority of samples from this study were made of high-quality brass, arguably of a Roman origin. The Pb isotope data show a clear consistency with ore deposits in the Massif Central, especially with Pb-Zn deposits near Les Malines. In addition, a high degree of homogeneity of the analysed samples in terms of their Pb isotope ratios probably excludes recycling using significantly different resources. Whether the Massif Central connection is provided by the Pb contained in the Cu source (metallic or geological), or is a result of the cementation process, cannot be unambiguously distinguished. Given the high purity of the Roman Cu \u0026ndash; known from the Cu ingots and Cu-based coinage \u0026ndash; with low Pb levels compared to slightly Pb-enriched brass samples, a lead isotope signal linked to the Pb-Zn ores is more likely. Nevertheless, as indicated by non-brass samples from our assemblage and local provenance of the AES coins of the first altar series from Lyon [63], even the copper could come from the same territory.\u003c/p\u003e \u003cp\u003eThe archaeological cultural groups used to categorise samples appear to have only a moderate significance in the pattern of trace element composition; even the Pb-isotope ratios were not influenced so significantly compared to categorisation of the samples according to dating. If we accept the possibility that the Pb isotope values refer to lead originating in the cementation medium, the variation in trace element patterns may point to various copper sources, or it may be a result of some further admixtures. Such fact does not contradict a possible different origin of a given artefact suggested by its typological classifications and refers solely to the material used for its fabrication.\u003c/p\u003e \u003cp\u003eAn important message provided by the geochemical analysis is the inconsistency of brass objects with contemporary brass coinage, the Roman \u003cem\u003esestertii\u003c/em\u003e. However, this finding requires verification by further analysis of a more varied selection of brass coins using state-of-the-art analytical methods.\u003c/p\u003e \u003cp\u003eThe best level of consistency is found among samples with high Zn content from the phase R B1, i.e. a period around the turn of the Era and the following five decades of the 1st century AD. Already the objects from the late Iron Age do not fall outside the range of Pb isotope ratios of the Massif Central deposits. Therefore, it can be assumed that the brass production might have started in the Massif Central as early as around the middle of the 1st century BC. The existence of Gallic brass coins from the time of Caesar's military campaigns in Gaul supports this hypothesis [61]. Also, there is evidence of large-scale exploitation of gold in the Massif Central that took place already before the Roman conquest [82, 83, 84]. It is generally accepted that the Romans benefited from the developed tradition of local Gallic mining [79]. The importance of natural resources in the Massif Central for the expanding Roman Empire is underlined by the intensive iron production around the Montagne Noire area that became significant in the 1st century AD. According to archaeometric analyses, local iron was distributed widely via long-distance trade and served as a vital source of material for the Roman army [85, 86].\u003c/p\u003e \u003cp\u003eThe influx of brass to the territories north of the Alps occurred as early as in southern Europe and the Gaul, thus indicating the instant popularity of the new and attractive material. The earliest evidence of brass used in diplomatic contacts with the indigenous populations can be already seen in the late Iron Age. The nature of its distribution mechanisms is hard to evaluate, but in that period, brass was still a rare commodity. Massive-scale and, perhaps more importantly, a regular occurrence is dated no earlier than the Augustan and Tiberian Era. Brass became a ubiquitous yet still highly valued commodity in Germanic society. Its special social status was derived from its distinctive visual qualities and, initially, its exclusive Roman provenance. The level of dependency of the Barbarian society on an external material supply from the Romans seems to be very high. Based on the current scientific evidence, the importance of brass in political relations between the Romans and Barbarians, possibly similar to the role of the silver coins in northern Britain [87] can be assumed. This material with the connotations of prestige and luxury could serve as an effective medium in determining the quality of relations among different Barbarian groups. The 'value: cost-effectiveness ratio' for the material such as brass seems to have played in the Roman favour. The archaeological evidence from other regions beyond Bohemia suggests that a similar strategy of diplomatic contacts may also apply to other territories where early Roman brass objects occur (i.e. Slovakia, Poland, Germany) [88].\u003c/p\u003e \u003cp\u003eGiven the sufficient influx of the Roman brass into the Barbarian territories, the recycling has not affected the geochemical properties attributed to the original Roman \u003cem\u003eaurichalcum\u003c/em\u003e as much as is observed for materials from the 2nd century AD [60, 89]. Only the samples from the earliest phase of the Early Roman period (R A) may have had their Pb isotope ratios influenced by Iberian Cu sources. A specificity of data from the latest phase (R B2) could be explained at this point by exploitation of different deposits in the Massif Central than in the early stages of brass production. Such a hypothesis is also supported by the 2nd century AD brass ingots from the shipwreck of Al\u0026eacute;ria that share the Pb isotope signature with our samples and is also thought to be produced in the Massif Central.\u003c/p\u003e \u003cp\u003eThe volume of material entering the Germania Magna in the Early Roman period is hard to estimate and represents a research topic on its own. There have been some rough estimations in the work of Becker [90] for the Barbarian territory of the late Roman Germania, which led to an estimated 2.5 tons of material just for brooches. Given the larger dimensions of the Early Roman brooches compared to Late Roman types, plus the overall abundance of the metallic goods in the Early Roman graves, the quantity of consumed material must have been probably higher than that estimated.\u003c/p\u003e"},{"header":"6. Methods","content":"\u003cp\u003eSelected objects were drilled to the metal core to avoid the corrosion layers and collect the minimum sufficient amount of material for the chemical and Pb isotope analyses. Due to the small sizes of the objects and the high corrosion stage of some, the sample weight varied between 0.01 and 0.05 g. Because of the sample preparation methodology, As contents were not determined.\u003c/p\u003e \u003cp\u003eSamples of drilled-out bronze/brass materials were carefully weighed into pre-cleaned Savillex beakers, dissolved in a mixture of 6M HCl\u0026ndash;7M HNO\u003csub\u003e3\u003c/sub\u003e (3:1 v/v) with several drops of 23M HF and placed on a hotplate for 24 hours at 50\u0026deg;C. For the measurements of element abundances, freshly prepared solutions were dried down and re-dissolved in 2% HNO\u003csub\u003e3\u003c/sub\u003e. The abundances of selected elements were determined using an Agilent 7900x inductively coupled plasma mass spectrometer (ICP-MS), housed at the Czech Geological Survey.\u003c/p\u003e \u003cp\u003eThe chemical procedures for Pb isolation and purification employed two chromatographic columns. The first step was modified from Pin et al. [91] and used pre-cleaned and pre-conditioned Sr.Spec resin (50\u0026ndash;100 mesh; Triskem, France) packed in 0.2 mL columns. Samples were dried down and re-dissolved in 2M HCl. Lead was eluted with 6M HCl. The second step employed anion-exchange resin BioRad AG 1x8 (100\u0026ndash;200 mesh) combined with HCl and HBr as elution media, following the methodology outlined in Romer et al. [92]. The eluted Pb fraction was then dried down and repeatedly re-dissolved with 50 \u0026micro;l 14M HNO\u003csub\u003e3\u003c/sub\u003e to remove any residual organic material.\u003c/p\u003e \u003cp\u003ePrior to Pb isotope measurements, the dried Pb fractions were re-dissolved in 1 mL 2% HNO\u003csub\u003e3\u003c/sub\u003e and doped with Tl solution (NIST SRM 997; \u003csup\u003e205\u003c/sup\u003eTl/\u003csup\u003e203\u003c/sup\u003eTl = 2.3871). Lead isotope compositions were determined using an Aridus 2 desolvating unit (Cetac) coupled to a Neptune multi-collector ICPMS (ThermoFisher), housed at the Czech Geological Survey, in static mode. Sample analysis followed a conventional standard\u0026ndash;sample\u0026ndash;standard bracketing protocol in which the SRM-981 reference material solution was run after every unknown sample. Potential \u003csup\u003e204\u003c/sup\u003eHg isobaric interference on \u003csup\u003e204\u003c/sup\u003ePb was monitored at mass \u003csup\u003e202\u003c/sup\u003eHg and corrected by assuming natural Hg isotope ratios (\u003csup\u003e202\u003c/sup\u003eHg/\u003csup\u003e204\u003c/sup\u003eHg = 4.35). Correction of the measured Pb isotope ratios for mass discrimination utilised a generalised power law and natural isotope composition of Tl [93]. The results were then normalised off-line to the certified values for SRM 981, and the combined statistics for three measurements of each unknown sample were calculated. Data represent the uncertainty-weighted mean of three replicate measurements. Repeat measurements of NBS 981 yielded mean \u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb, \u003csup\u003e207\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb and \u003csup\u003e208\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb ratios of 16.942\u0026thinsp;\u0026plusmn;\u0026thinsp;0.003, 15.4998\u0026thinsp;\u0026plusmn;\u0026thinsp;0.0030 and 36.725\u0026thinsp;\u0026plusmn;\u0026thinsp;0.007 (2SEM, n\u0026thinsp;=\u0026thinsp;66), respectively.\u003c/p\u003e \u003cp\u003eSamples dated into the La T\u0026egrave;ne period and comparative Iron Age samples were processed with a slightly different methodology detailed elsewhere [28].\u003c/p\u003e \u003cp\u003eFor consistency in the data evaluation, the ore deposits data were prepared for the comparative analysis by removing multivariate outliers detected using the Mahalanobis distance [68]. This step is a prerequisite to fitting linear models to the data or using any other method to visualise the trends. By outliers, we understand data points with extreme values regarding the shape of the whole data distribution in a multidimensional setting defined by lead isotopic ratios (\u003csup\u003e206\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb, \u003csup\u003e207\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb, \u003csup\u003e208\u003c/sup\u003ePb/\u003csup\u003e204\u003c/sup\u003ePb, \u003csup\u003e207\u003c/sup\u003ePb/\u003csup\u003e206\u003c/sup\u003ePb and \u003csup\u003e208\u003c/sup\u003ePb/\u003csup\u003e206\u003c/sup\u003ePb, respectively).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eAcknowledgements\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThis work was supported by the Czech Science Foundation project 18-20096S [Mobility of materials and life cycles of artefacts: archaeometry of metals and glass of the La T\u0026egrave;ne and Early Roman period]. TM, JM and ZR contributed through the Strategic Research Plan of the Czech Geological Survey (DKRVO/ČGS 2018\u0026ndash;2022).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAuthors\u0026apos; contributions\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eAD and DB\u003cstrong\u003e\u0026nbsp;\u003c/strong\u003edesigned the research project (Grant 18-20096 S). DB, AD and TM performed statistical analyses, were responsible for the interpretation of the data, designed the manuscript and the figures. PP performed provenance and comparative analyses. TM, JM and ZR performed the analyses of Roman period samples. TM supervised the data quality. JT and LS contributed with the measurements of La T\u0026egrave;ne period samples.\u0026nbsp;\u003c/p\u003e"},{"header":"References","content":"\u003cp\u003e[1] Craddock, P. T. The composition of the copper alloys used by the Greek, Etruscan and Roman civilizations. \u003cem\u003eJournal of Archaeological Science\u003c/em\u003e\u003cstrong\u003e5\u003c/strong\u003e, 1\u0026ndash;16 (1978).\u003c/p\u003e\n\u003cp\u003e[2] Hanel, N., Bode, M. Messingbarren aus einem r\u0026ouml;mischen Schiffswrack bei Al\u0026eacute;ria (Korsika). In K\u0026ouml;rlin, G., Prange, M.,\u0026nbsp;St\u0026ouml;llner, Th. \u0026amp; Yalcin, \u0026Uuml;. (eds\u003cem\u003e.\u003c/em\u003e) \u003cem\u003eFrom Bright Ores to Shiny Metals. Festschrift for Andreas Hauptmann on the Occasion of 40 Years Research in\u0026nbsp;\u003c/em\u003e\u003cem\u003eArchaeometallury and Archaeometry,\u0026nbsp;\u003c/em\u003eMontanhistorische Zeitschrift.\u0026nbsp;Der Anschnitt Beiheft \u003cstrong\u003e29\u003c/strong\u003e, 167\u0026ndash;181 (Bochum, 2016).\u003c/p\u003e\n\u003cp\u003e[3] Caley, E. R. Orichalcum and related ancient alloys. 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(Kabitzsch / Leipzig, 1923).\u003c/p\u003e"},{"header":"Tables","content":"\u003cp\u003eDue to technical limitations, table 2-4 is only available as a download in the Supplemental Files section.\u003c/p\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"scientific-reports","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"scirep","sideBox":"Learn more about [Scientific Reports](http://www.nature.com/srep/)","snPcode":"","submissionUrl":"","title":"Scientific Reports","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Scientific Reports","inReviewEnabled":true,"inReviewRevisionsEnabled":true},"keywords":"Shining, gold, Ancient brass (aurichalcum), commodity, Antiquity, notably, brass fabrication, material, western Mediterranean","lastPublishedDoi":"10.21203/rs.3.rs-715158/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-715158/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eAncient brass (\u003cem\u003eaurichalcum\u003c/em\u003e) was a valued commodity in the Antiquity, notably because of its gold-like appearance. After mastering brass fabrication using the cementation procedure in the 1\u003csup\u003est\u003c/sup\u003e century BC in the Mediterranean, this material became widely used by the Romans for coins, jewellery and other objects. Because of its visual qualities, it is believed that since this period, brass played an important role in diplomatic and economic contacts with indigenous communities, notably Celtic and Germanic tribes north of Danube and west of Rhine. To test this hypothesis, we performed for the first time the archaeometric and advanced statistical multivariate analysis of a suite of late Iron Age and Early Roman period (1\u003csup\u003est\u003c/sup\u003e century BC – 1\u003csup\u003est\u003c/sup\u003e century AD) brass and other copper-alloy objects from the territory of Bohemia to constrain their provenance. The new results for brass objects from this early phase of the massive occurrence of Roman \u003cem\u003eaurichalcum\u003c/em\u003e in the Barbarian territories point to the ore deposits in the western Mediterranean or the Massif Central area in Gaul, consistent with historical events. These new findings underscore the great economic and political importance of the new and rich mineral resources in the Transalpine Gaul acquired due to Caesar's military campaigns\u003c/p\u003e","manuscriptTitle":"Shining Like Gold and New: The Emergence of Brass North of the Alps Around the Turn of the Era.","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2021-07-23 17:20:00","doi":"10.21203/rs.3.rs-715158/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Major revision","date":"2021-09-14T01:58:15+00:00","index":"","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2021-07-29T13:55:29+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"1e99fe25-82e0-48e2-b207-f283809e9cdc","date":"2021-07-22T13:20:26+00:00","index":"hide","fulltext":""},{"type":"reviewersInvited","content":"","date":"2021-07-22T12:09:23+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2021-07-22T12:08:08+00:00","index":"","fulltext":""},{"type":"editorInvited","content":"","date":"2021-07-21T23:25:22+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2021-07-21T23:22:58+00:00","index":"","fulltext":""},{"type":"submitted","content":"Scientific Reports","date":"2021-07-14T09:13:43+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"scientific-reports","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"scirep","sideBox":"Learn more about [Scientific Reports](http://www.nature.com/srep/)","snPcode":"","submissionUrl":"","title":"Scientific Reports","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Scientific Reports","inReviewEnabled":true,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"400c5fbc-3b1c-4873-b0bf-16fa9a91bad3","owner":[],"postedDate":"July 23rd, 2021","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[{"id":5933986,"name":"Archaeology"},{"id":5933987,"name":"Geochemistry"}],"tags":[],"updatedAt":"2021-12-08T04:29:11+00:00","versionOfRecord":[],"versionCreatedAt":"2021-07-23 17:20:00","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-715158","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-715158","identity":"rs-715158","version":["v1"]},"buildId":"WrCJVZZCHTDjtuVLN7oU0","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}