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Archaeological and Anthropological Sciences

, Volume 11, Issue 7, pp 3065–3099 | Cite as

Documenting scarce and fragmented residues on stone tools: an experimental approach using optical microscopy and SEM-EDS

  • Elspeth HayesEmail author
  • Veerle Rots
Original Paper

Abstract

Residue analyses are widely applied to studies of stone tool function and can be a powerful method for determining the past tool use(s), especially when combined with other functional investigations such as usewear and technological analysis. Experimental work has shown that optical microscopes and the scanning electron microscope with energy dispersive X-ray spectroscopy (SEM-EDS) are reliable instruments for identifying intact tool residues. However, little experimental work has aimed to document residues that show various stages of degradation or when abundance is low. We combined traditional optical microscopy and the SEM-EDS to identify the advantages and challenges of each technique when looking at progressively smaller and more fragmented residues following more aggressive stages of cleaning, burial and soaking in a weak acid/base solution. We found that large quantities of intact residues on unwashed stone tools show distinctive morphological features under optical microscopes and the SEM-EDS can be used to document residues under extremely high magnifications and to determine their elemental compositions. After the various stages of washing, we found that residues became highly fragmented and were restricted to common stone features like the micro-cracks/scars along the working edge. These residues were often difficult to characterise using optical microscopes but the SEM-EDS proved highly useful. The weak acid/base solutions caused some residues to become physically altered or modified their elemental composition. Buried tools reduced the abundance of use-residues and introduced additional non-use-related contaminant particles that affected EDS measurements and lead to less reliable residue interpretations.

Keywords

Residue degradation Contamination Functional analysis Residue reference library 

Notes

Acknowledgements

This research was carried out in the TraceoLab at the University of Liège, Belgium, and was funded by the European Research Council under the European Union’s Seventh Framework Programme (FP/2007-2013)/ERC Grant Agreement n. 312283 (V. Rots), the Fund for Scientific Research (FNRS-FRS EQP) and the University of Liège (FSR). We thank Christian Lepers, Noora Taipale, Ewa Dutkiewicz and Dries Cnuts for providing experimental specimens for analysis. We are grateful to Philippe Compère and Sarah Smeets from the University of Liège for sputtering the extracted samples. Veerle Rots is also indebted to the Fund for Scientific Research (FNRS-FRS CQ). We would like to thank two anonymous reviewers for their useful comments that helped improve this manuscript.

References

  1. Albéric M & Reiche I (2015) Ivoire, in Message d'os. Archéométrie du squelette animal et humain. M Balasse et al (eds) 2015, éditions des archives contemporaines Paris, pp 53–68Google Scholar
  2. Albéric M, Gourrier A, Wagermaier W, Fratzl P, Reiche I (2018) The three-dimensional arrangement of the mineralized collagen fibers in elephant ivory and its relation to mechanical and optical properties. Acta Biomater 72:342–351Google Scholar
  3. Alvarez M, Fiore D, Favret E, Guerra RC (2001) The use of lithic artefacts for making rock art engravings: observation and analysis of use-wear traces in experimental tools through optical microscopy and SEM. J Archaeol Sci 28(5):457–464Google Scholar
  4. Anderson PC (1980) A scanning electron microscope study of microwear polish and diagnostic deposits on used stone tool working edges. Lithic Technol 9:32–33Google Scholar
  5. Anderson P, Formenti F (1996) Exploring the use of abraded obsidian “Cayönu tools” using experimentation, optical and SEM microscopy, and EDA analysis. Archaeometry 94:553–566Google Scholar
  6. Banks WT, Greenwood CT (1975) Starch and its components. Edinburgh University Press, EdinburghGoogle Scholar
  7. Barton H (2009) Starch granule taphonomy: the results of a two year field experiment. In: M Haslam, G Robertson, A Crowther, S Nugent & L Kirkwood (eds) Archaeological science under a microscope: studies in residue and ancient DNA analysis in honour of Thomas H. Loy ANU E Press, Canberra (Vol 30), pp 129–140Google Scholar
  8. Bonnichsen R, Hodges L, Ream W, Field KG, Kirner DL, Selsor K, Taylor RE (2001) Methods for the study of ancient hair: radiocarbon dates and gene sequences from individual hairs. J Archaeol Sci 28:775–785Google Scholar
  9. Bordes L, Prinsloo LC, Fullagar R, Sutikna T, Hayes E, Jatmiko, Wahyu Saptomo E, Tocheri MW, Roberts RG (2017) Viability of Raman microscopy to identify micro-residues related to tool-use and modern contaminants on prehistoric stone artefacts. J Raman Spectrosc 48(9):1212–1221Google Scholar
  10. Bordes L, Fullagar R, Prinsloo LC, Hayes EH, Kozlikin M, Shunkov M, Derevianko A, Roberts RG (2018) Raman spectroscopy of lipid micro-residues on Middle Palaeolithic stone tools from Denisova cave, Siberia. J Archaeol Sci 95:52–63Google Scholar
  11. Borel A, Ollé A, Vergés JM, Sala R (2014) Scanning electron and optical light microscopy: two complementary approaches for the understanding and interpretation of usewear and residues on stone tools. J Archaeol Sci 48:46–59Google Scholar
  12. Brunner H, Coman BJ (1974) The identification of mammalian hair. Inkata Press, MelbourneGoogle Scholar
  13. Byrne L, Ollé A, Vergès JM (2006) Under the hammer: residues resulting from production and microwear on experimental stone tools. Archaeometry 48(4):549–564Google Scholar
  14. Cattaneo C, Gelsthorpe K, Phillips P, Sokol RJ (1993) Blood residues on stone tools: indoor and outdoor experiments. World Archaeol 25:29–43Google Scholar
  15. Christensen M, Technologie de l'ivoire au Paléolithique supérieur (1999) British archaeological reports. In: JaE Hedges (ed) Vol 751. Archaeopress, OxfordGoogle Scholar
  16. Claasen C (1998) Shells. Cambridge University Press, CambridgeGoogle Scholar
  17. Cnuts D & Rots V (2017a) Taphonomie et analyse des résidus sur les pièces lithiques. TaphonomieS, pp 187–194Google Scholar
  18. Cnuts D, Rots V (2017b) Extracting residues from stone tools for optical analysis: towards an experiment-based protocol. Archaeol Anthropol Sci:1–20Google Scholar
  19. Cnuts D, Tomasso S, Rots V (2017) The role of fire in the life of an adhesive. J Archaeol Method Theory:1–24Google Scholar
  20. Cristiani E, Živaljević I, Borić D (2014) Residue analysis and ornament suspension techniques in prehistory: cyprinid pharyngeal teeth beads from late Mesolithic burials at Vlasac. J Archaeol Sci 46:292–310Google Scholar
  21. Croft S, Monnier G, Radini A, Little A & Milner N (2016) Lithic residue survival and characterisation at star Carr: a burial experiment. Internet archaeology, (42), 4DUMMY.  https://doi.org/10.11141/ia.42.5
  22. Croft S, Chatzipanagis K, Kröger R, Milner N (2018) Misleading residues on lithics from star Carr: identification with Raman microspectroscopy. J Archaeol Sci Rep 19:430–438Google Scholar
  23. Crowther A, Haslam M, Oakden N, Walde D, Mercader J (2014) Documenting contamination in ancient starch laboratories. J Archaeol Sci 49:90–104Google Scholar
  24. Dinnis R, Pawlik A, Gaillard C (2009) Bladelet cores as weapon tips? Hafting residue identification and micro-wear analysis of three carinated burins from the late Aurignacian of les Vachons, France. J Archaeol Sci 36(9):1922–1934Google Scholar
  25. Eastaugh N, Walsh V, Chaplin T, Siddal R (2008) Pigment compendium: a dictionary and optical microscopy of historical pigments. Elsevier Ltd., OxfordGoogle Scholar
  26. Eisele JA, Fowler DD, Haynes G, Lewis RA (1995) Survival and detection of blood residues on stone tools. Antiquity 69:36–46Google Scholar
  27. Evert RF (2006) Esau's plant anatomy. Wiley & Sons, Inc., New JerseyGoogle Scholar
  28. Fullagar R (1991) The role of silica in polish formation. J Archaeol Sci 18:1–25Google Scholar
  29. Fullagar R (2014) Residues and usewear. In: Balme J, Paterson A (eds) Archaeology Practice: A Student Guide to Archaeological Analyses. Blackwell Publishing, Maldon, pp 232–263Google Scholar
  30. Fullagar R, Matheson M ( 2013) Traceology: A summary. In: Smith, C. (Ed.), Encyclopedia of Global Archaeology. Springer, New York, pp 73–85Google Scholar
  31. Gott B, Barton H, Samuel D, Torrence R (2006) Biology of starch. In: Torrence R, Barton H (eds) Ancient Starch Research. Left Coast Press, Walnut Creek, California, pp 35–45Google Scholar
  32. Gurfinkel DM, Franklin UM (1988) A study of the feasibility of detecting blood residue on artifacts. J Archaeol Sci 15:83–97Google Scholar
  33. Haslam M (2004) The decomposition of starch grains in soils: implications for archaeological residue analyses. J Archaeol Sci 31:1715–1734Google Scholar
  34. Haslam M (2006) Potential misidentification of in situ archaeological tool residues: starch and conidia. J Archaeol Sci 33:114–121Google Scholar
  35. Hayes EH, Cnuts D, Lepers C, Rots V (2017) Learning from blind tests: determining the function of experimental grinding stones through use-wear and residue analysis. J Archaeol Sci Rep 11:245–260Google Scholar
  36. Helfman G, Collette BB, Facey DE, Bowen BW (2009) Skeleton, skin, and scales. In: Helfman G, Collette BB, Facey DE, Bowen BW (eds) The Diversity of Fishes: Biology, Evolution, and Ecology. Wiley-Blackwell, OxfordGoogle Scholar
  37. Hillman G, Wales S, McLaren F, Evans J, Butler A (1993) Identifying problematic remains of ancient plant foods: a comparison of the role of chemical, histological and morphological criteria. World Archaeol 25:94–121Google Scholar
  38. Huang J, Hess WM, Weber DJ, Purcell AE, Huber CS (1990) Scanning electron microscopy: tissue characteristics and starch granule variations of potatoes after microwave and conductive heating. Food Struct 9(2):113–122Google Scholar
  39. Jahren AH, Toth N, Schick K, Clark JD, Amundson RG (1997) Determining stone tool use: chemical and morphological analyses of residues on experimentally manufactured stone tools. J Archaeol Sci 24:245–250Google Scholar
  40. Kamminga J (1977) A functional study of use-polished elouras. In: Wright RVS (ed) Stone tools as cultural markers: change, evolution and complexity. Australian Institute of Aboriginal Studies, Canberra, pp 205–212Google Scholar
  41. Kamminga J (1982) Over the edge: occasional papers in anthropology, vol 12. University of Queensland Anthropological Museum, St LuciaGoogle Scholar
  42. Keeley LH (1977) The function of Palaeolithic flint tools. Sci Am 237:108–126Google Scholar
  43. Knecht L (2012) The use of hair morphology in the identification of mammals. In: Huffman JE, Wallace JR (eds) Wildlife forensics: methods and applications. Wiley Blackwell, Chichester, pp 129–144Google Scholar
  44. Knutsson K (1988) SEM-analysis of wear features on experimental quartz tools. In: Owen L, Unrath G (eds) Technical Aspects of Microwear Studies on Stone Tools. Tübingen, Archeologica Venatoria, pp 35–46Google Scholar
  45. Kraus EH, Hunt WF, Ramsdell LS (1959) Mineralogy: an introduction to the study of minerals and crystals. McGraw-Hill Book Company, New YorkGoogle Scholar
  46. Langejans GHJ (2010) Remains of the day-preservation of organic micro-residues on stone tools. J Archaeol Sci 37:971–985Google Scholar
  47. Langejans GHJ (2011) Discerning use-related micro-residues on tools: testing the multi-stranded approach for archaeological studies. J Archaeol Sci 38:985–1000Google Scholar
  48. Langejans GH (2012) Middle Stone Age pièces esquillées from Sibudu Cave, South Africa: an initial micro-residue study. J Archaeol Sci 39(6):1694–1704Google Scholar
  49. Langenheim JH (2003) Plant resins. Chemistry, evolution and ethnobotany. Timber Press, CambridgeGoogle Scholar
  50. Lieber RL (2002) Skeletal muscle structure, function, and plasticity. In the physiological basis of rehabilitation, 2nd edn. Lippincott, Williams, & Wilkins, PhiladelphiaGoogle Scholar
  51. Lillie R (1976) H.J. Conn’s biological stains. Williams and Wilkins, BaltimoreGoogle Scholar
  52. Lombard M (2008) Finding resolution for the Howiesons Poort through the microscope: microresidue analysis of segments from Sibudu cave, South Africa. J Archaeol Sci 35:26–41Google Scholar
  53. Lombard M, Wadley L (2007) The morphological identification of micro-residues on stone tools using light microscopy: progress and difficulties based on blind tests. J Archaeol Sci 34:155–165Google Scholar
  54. Loy TH, Dixon EJ (1998) Blood residues on fluted points from Beringia. Am Antiq 63(1):21–46Google Scholar
  55. Luong S, Hayes E, Flannery E, Sutikna T, Tocheri MW, Saptomo EW, Roberts RG (2017) Development and application of a comprehensive analytical workflow for the quantification of non-volatile low molecular weight lipids on archaeological stone tools. Anal Methods 9(30):4349–4362Google Scholar
  56. Lynch V, Miotti L (2017) Introduction to micro-residues analysis: systematic use of scanning electron microscope and energy dispersive X-rays spectroscopy (SEM-EDX) on Patagonian raw materials. J Archaeol Sci Rep 16:299–308Google Scholar
  57. Mansur-Franchomme ME (1983) Scanning electron microscopy of dry hide working tools: the role of abrasives and humidity in microwear polish formation. J Archaeol Sci 10:223–230Google Scholar
  58. Mauseth JD (1988) Plant anatomy, vol 560. Benjamin/Cummings Publishing Co., Menlo ParkGoogle Scholar
  59. Meeks ND, Sieveking GDG, Tite MS, Cook J (1982) Gloss and use-wear traces on flint sickles and similar phenomena. J Archaeol Sci 9(4):317–340Google Scholar
  60. Monnier GF, Ladwig JL, Porter ST (2012) Swept under the rug: the problem of unacknowledged ambiguity in lithic residue identification. J Archaeol Sci 40:3722–3739Google Scholar
  61. Monnier G, Frahm B, Luo E, Missal K (2017a) Developing FTIR microspectroscopy for the analysis of animal-tissue residues on stone tools. J Archaeol Method Theory:1–44Google Scholar
  62. Monnier G, Frahm B, Luo E, Missal K (2017b) Developing FTIR microspectroscopy for analysis of plant residues on stone tools. J Archaeol Sci 78:158–178Google Scholar
  63. Morris VJ (1990) Starch gelatinisation and retrogradation. Trends Food Sci Technol 1:2–6Google Scholar
  64. Nudelman F, Ami Gotliv B, Addadi L, Weiner S (2006) Mollusk shell formation: mapping the distribution of organic matrix components underlying a single aragonitic tablet in nacre. J Struct Biol 153:176–187Google Scholar
  65. Ollé A, Vergès JM (2008) SEM functional analysis and the mechanism of microwear formation. Prehistoric Technology 40:39–49Google Scholar
  66. Ollé A, Vergès JM (2014) The use of sequential experiments and SEM in documenting stone tool microwear. J Archaeol Sci 48:60–72Google Scholar
  67. Pawlik AF (2004) Identification of hafting traces and residues by scanning electron microscopy and energy-dispersive analysis of X-rays. Lithics in Action, 169–79Google Scholar
  68. Pawlik AF, Thissen JP (2011) Hafted armatures and multi-component tool design at the Micoquian site of Inden-Altdorf, Germany. J Archaeol Sci 38(7):1699–1708Google Scholar
  69. Pedergnana A, Ollé A (2018) Building an experimental comparative reference collection for lithic micro-residue analysis based on a multi-analytical approach. J Archaeol Method Theory 25(1):117–154Google Scholar
  70. Pedergnana A, Asryan L, Fernández-Marchena JL, Ollé A (2016) Modern contaminants affecting microscopic residue analysis on stone tools: a word of caution. Micron 86:1–21Google Scholar
  71. Pollard AM, Heron C (2008) Archaeological chemistry. The Royal Society of Chemistry, CambridgeGoogle Scholar
  72. Raven PH, Evert RF, Eichhorn SE (1999) Biology of plants, 6th edn. W.H. Freeman and Company publishers, New YorkGoogle Scholar
  73. Raven PH, Evert RF, Eichhorn SE (2005) Biology of plants. W.H. Freeman and Company publishers, New YorkGoogle Scholar
  74. Reeve RM (1954) Histological survey of conditions influencing texture in potatoes: effects of heat treatments on structure. J Food Sci 19(1–6):323–332Google Scholar
  75. Reiche I, Müller K (2018) Marqueur d’identification à micro-échelle de l’ivoire de mammouth dans les objets préhistoriques. L'Anthropologie 2018:316–326. https://doi.org/10.1016/j.anthro.2018.01.001 Google Scholar
  76. Rogers AF, Kerr PF (1942) Optical mineralogy. McGraw-Hill Book Company, Inc., New YorkGoogle Scholar
  77. Ross MH, Pawlina W (2011) Histology: a text and atlas. Loppincott Williams & Wilkins, BaltimoreGoogle Scholar
  78. Rots V, Hayes E, Cnuts D, Lepers C, Fullagar R (2016) Making sense of residues on flaked stone artefacts: learning from blind tests. PLoS One 11(3):e0150437Google Scholar
  79. Rots V, Lentfer C, Schmid VC, Porraz G, Conard NJ (2017) Pressureflaking to serrate bifacial points for the hunt during the MIS5 at Sibudu cave (South Africa). PLoS One 12(4):e0175151. https://doi.org/10.1371/journal.pone.0175151
  80. Shanks OC, Bonnichsen R, Vella AT, Ream W (2001) Recovery of protein and DNA trapped in stone tool microcracks. J Archaeol Sci 28:965–972Google Scholar
  81. Singh N, Singh J, Kaur L, Singh Sodhi N, Singh Gill B (2003) Morphological, thermal and rheological properties of starches from different botanical sources. Food Chem 81:219–231Google Scholar
  82. Smith KN, Wärmländer SK, Vellanoweth RL, Smith CM, Kendig WE (2015) Residue analysis links sandstone abraders to shell fishhook production on san Nicolas Island, California. J Archaeol Sci 54:287–293Google Scholar
  83. Steck TL (1989) Red cell shape. In: Stein WD, Bronner F (eds) Cell shape: determinants, regulation, and regulatory role. Academic Press, San Diego, pp 205–246Google Scholar
  84. Stephenson B (2015) A modified Picro-Sirius red (PSR) staining procedure with polarization microscopy for identifying collagen in archaeological residues. J Archaeol Sci 61:235–243Google Scholar
  85. Stern B, Lampert Moore CD, Heron C, Pollard AM (2008) Bulk stable light isotopic ratios in recent and archaeological resin: towards detecting the transport of resins in antiquity? Archaeometry 50(2):351–370Google Scholar
  86. Su XW, Cui FZ (1999) Hierarchical structure of ivory: from nanometer to centimetre. Mater Sci Eng C 7(1):19–29Google Scholar
  87. Sussman C (1988) A microscopic analysis of use-wear and polish formation on experimental quartz tools. In: BAR international series, 395. British Archaeological Reports, OxfordGoogle Scholar
  88. Tester RF, Karkalas J, Qi X (2004) Starch—composition, fine structure and architecture. Journal of Cereal Science, 39(2):151–165Google Scholar
  89. Teerink BJ (1991) Hair of west European mammals. Atlas and identification key. Cambridge University Press, CambridgeGoogle Scholar
  90. Unger-Hamilton R (1984) The formation of use-wear polish on flint: beyond the “deposit versus abrasion” controversy. J Archaeol Sci 11:91–98Google Scholar
  91. Wadley L, Lombard M (2007) Small things in perspective: the contribution of our blind tests to micro-residue studies on archaeological stone tools. J Archaeol Sci 34:1001–1010Google Scholar
  92. Wadley L, Lombard M, Williamson BS (2004) The first residue analysis blind tests: results and lessons learnt. J Archaeol Sci 31:1491–1501Google Scholar
  93. Wheater PR, Burkitt HG, Daniels VG (1987) Functional histology: a text and colour atlas. Longman Group UK limited, EdinburghGoogle Scholar
  94. Wojcieszak M, Wadley L (2018) Raman spectroscopy and scanning electron microscopy confirm ochre residues on 71 000-year-old bifacial tools from Sibudu, South Africa. Archaeometry 60:1062–1076. https://doi.org/10.1111/arcm.12369 Google Scholar
  95. Xhauflair H, Pawlik A, Forestier H, Saos T, Dizon E, Gaillard C (2017) Use-related or contamination? Residue and use-wear mapping on stone tools used for experimental processing of plants from Southeast Asia. Quat Int 427:80–93Google Scholar

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© Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  1. 1.Centre for Archaeological ScienceUniversity of WollongongWollongongAustralia
  2. 2.TraceoLabUniversity of LiègeLiègeBelgium
  3. 3.Chercheur Qualifié du FNRS, TraceoLabUniversity of LiègeLiègeBelgium
  4. 4.Institute for Early Prehistory and Quaternary EcologyUniversity of TübingenTübingenGermany

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