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During the gunpowder-driven military revolution in early modern Japan, a huge amount of ammunition and its ingredients was imported from western countries and manufactured locally. A sum total of 24 gunpowder ingredients which survived from during the time was analyzed for delta N-15(saltpetre-nitrogen), delta S-34(native) (sulfur) and delta C-13(charcoal) carbon. delta C-13(charcoal) (carbon), and these analyses revealed values in a narrow range from -27.6 to -25.7 parts per thousand indicating a C-3 dominant wood carbon source. In contrast, delta S-34(native) (sulfur) showed fairly large variation (-1.1 to +12.3 parts per thousand), and this variation reflects distinct source sulfur. High delta S-34(native) (sulfur) values (around +10 parts per thousand) correspond to Sicilian sulfur (Italy) which prevailed in the world sulfur market at the time. Low delta S-34(native) (sulfur) values (similar to-1.1 parts per thousand) were observed for a few gunpowders (Enfield rifle, Le Faucheux revolver and artillery guns), implying a predominance of Japanese volcanic sulfur.

delta N-15 values of nitrate-nitrogen in the form of saltpetre also varied from -2.0 to +22.0 parts per thousand. Such variation was interpreted in terms of contributing two end-member nitrates, i.e., nitrate formed by a nitrification process (microbial origin), and nitrate from desert nitrate (meteoric origin: around 0%). An anomalously high delta N-15 value (+22.0 parts per thousand) observed for a cannon type artillery was likely a residue that was subjected to denitrification during burial in soils. Information from stable isotope analysis for saltpetre and native sulfur, but not from charcoal carbon, provides strong evidence for the provenance reflecting worldwide trading lead by some advanced nations. (C) 2014 Elsevier Ltd. All rights reserved.