Microchemical characterisation of natural gold and artefact gold as a tool for provenancing prehistoric gold artefacts: a case study in Ireland

The importance of Au to ancient societies has encouraged many archaeologists to search for the sources exploited in antiquity. These projects generally involve detailed studies of artefacts and comparison of their chemical characteristics with those reported for natural Au. However, descriptions of natural Au are frequently inadequate for provenancing studies, and the compositional variability of the material is not widely recognised. The present study describes a new approach to gold provenancing using the technique of microchemical characterisation in which populations of gold grains are classified according to the alloy compositions and the assemblages of microinclusions of other minerals. This technique, originally developed to identify sources of alluvial gold during Au exploration, has proved applicable to provenancing studies in four main areas. Firstly, microchemical characterisation of artefacts grouped according to archaeological criteria can indicate the number of sources exploited in relation to time and artefact taxonomy. Secondly, knowledge of the total variation in chemical characteristics of natural Au from a particular region provides an excellent database for provenancing and reduces the need for exhaustive sampling. Thirdly, it is possible to predict how Au alloys were modified during fabrication as a consequence of assimilation of mineral inclusions. Finally, identification of inclusion phases in artefact Au can provide information on metallurgical practices. These principles have been applied to the search for the source of Au used for the unique traditions of prehistoric Irish metalworking. Studies of 180 Irish Au artefacts belonging to four major metalworking traditions dating from the Early Bronze Age (2400 BC) to the Iron Age, (150 BC) show that each group exhibits distinctive Ag and Cu contents. Parallel studies of 2267 natural Au grains from 58 alluvial localities and four bedrock localities throughout Ireland reveal a broad pattern of alloy compositions consistent with style of mineralisation and host geology. The ranges of Ag contents of Early Bronze Age and Middle Bronze Age artefacts suggests that the Au source lies within Lower Palaeozoic sedimentary rocks of the Southern Uplands Terrane and significantly, that the same source (or sources) were used in both periods. A different source of relatively Ag-rich Au (most probably at Croagh Patrick, Co. Mayo), was exploited in the Late Bronze Age. Iron Age artefacts have Ag contents higher than natural Irish Au. Evidence for evolution of metallurgical practice during the Bronze Age is provided by the increasing Cu content of the gold alloys (to levels far in excess of natural gold) and the nature of inclusions in artefacts of different ages. Elevated Sn in Cu-rich alloys suggests deliberate or accidental alloying with bronze. This approach has provided the first clear indication that only a few individual indigenous Irish sources of Au were used during the Bronze Age and that their relative importance changed over time. Future archaeological investigations may adopt a geographical focus that was not previously possible