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Analyses of Native American pottery found in northern New England have typically followed a normative approach focusing on formal variability, intended to address questions of culture history and chronology. Although these methods and goals are essential to laying the groundwork for further study, they are by no means the end goal of archaeological research. Since the 1950s, archaeologists have increasingly adopted analytical methods grounded in the realm of the physical sciences to examine sources and methods of artifact production. The resulting interdisciplinary field, referred to as archaeometry, draws together anthropology, physics, chemistry, and geology to identify the decisions made by prehistoric cultures. Recent nuclear and geological analyses of natural clays and prehistoric pottery from Vermont and New Hampshire serve to demonstrate how archaeologists may employ techniques grounded in the physical sciences and move beyond asking “Who?” and “When?” to begin pursuing the “How?” and “Why?” of the archaeological record. These data suggest there is significant chemical variation among clay sources in the region, and that this chemical variation may be related to depositional regimes. Further, comparison of archaeological pottery samples reveals decisions made concerning clay and temper acquisition, as well as suggesting evidence for intraregional trade and other forms of human interaction.