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

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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.

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References

  • 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 53–68

  • 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 72:342–351

    Article  Google Scholar 

  • 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):457–464

    Article  Google Scholar 

  • Anderson PC (1980) A scanning electron microscope study of microwear polish and diagnostic deposits on used stone tool working edges. Lithic Technol 9:32–33

    Google Scholar 

  • Anderson P, Formenti F (1996) Exploring the use of abraded obsidian “Cayönu tools” using experimentation, optical and SEM microscopy, and EDA analysis. Archaeometry 94:553–566

    Google Scholar 

  • Banks WT, Greenwood CT (1975) Starch and its components. Edinburgh University Press, Edinburgh

    Google Scholar 

  • 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 129–140

  • 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 28:775–785

    Article  Google Scholar 

  • 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):1212–1221

    Article  Google Scholar 

  • 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 95:52–63

    Article  Google Scholar 

  • 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 48:46–59

    Article  Google Scholar 

  • Brunner H, Coman BJ (1974) The identification of mammalian hair. Inkata Press, Melbourne

    Google Scholar 

  • Byrne L, Ollé A, Vergès JM (2006) Under the hammer: residues resulting from production and microwear on experimental stone tools. Archaeometry 48(4):549–564

    Article  Google Scholar 

  • Cattaneo C, Gelsthorpe K, Phillips P, Sokol RJ (1993) Blood residues on stone tools: indoor and outdoor experiments. World Archaeol 25:29–43

    Article  Google Scholar 

  • Christensen M, Technologie de l'ivoire au Paléolithique supérieur (1999) British archaeological reports. In: JaE Hedges (ed) Vol 751. Archaeopress, Oxford

  • Claasen C (1998) Shells. Cambridge University Press, Cambridge

    Google Scholar 

  • Cnuts D & Rots V (2017a) Taphonomie et analyse des résidus sur les pièces lithiques. TaphonomieS, pp 187–194

  • Cnuts D, Rots V (2017b) Extracting residues from stone tools for optical analysis: towards an experiment-based protocol. Archaeol Anthropol Sci:1–20

  • Cnuts D, Tomasso S, Rots V (2017) The role of fire in the life of an adhesive. J Archaeol Method Theory:1–24

  • 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 46:292–310

    Article  Google Scholar 

  • 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

  • Croft S, Chatzipanagis K, Kröger R, Milner N (2018) Misleading residues on lithics from star Carr: identification with Raman microspectroscopy. J Archaeol Sci Rep 19:430–438

    Google Scholar 

  • Crowther A, Haslam M, Oakden N, Walde D, Mercader J (2014) Documenting contamination in ancient starch laboratories. J Archaeol Sci 49:90–104

    Article  Google Scholar 

  • 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):1922–1934

    Article  Google Scholar 

  • Eastaugh N, Walsh V, Chaplin T, Siddal R (2008) Pigment compendium: a dictionary and optical microscopy of historical pigments. Elsevier Ltd., Oxford

    Google Scholar 

  • Eisele JA, Fowler DD, Haynes G, Lewis RA (1995) Survival and detection of blood residues on stone tools. Antiquity 69:36–46

    Article  Google Scholar 

  • Evert RF (2006) Esau's plant anatomy. Wiley & Sons, Inc., New Jersey

    Book  Google Scholar 

  • Fullagar R (1991) The role of silica in polish formation. J Archaeol Sci 18:1–25

    Article  Google Scholar 

  • Fullagar R (2014) Residues and usewear. In: Balme J, Paterson A (eds) Archaeology Practice: A Student Guide to Archaeological Analyses. Blackwell Publishing, Maldon, pp 232–263

    Google Scholar 

  • Fullagar R, Matheson M ( 2013) Traceology: A summary. In: Smith, C. (Ed.), Encyclopedia of Global Archaeology. Springer, New York, pp 73–85

  • 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 35–45

    Google Scholar 

  • Gurfinkel DM, Franklin UM (1988) A study of the feasibility of detecting blood residue on artifacts. J Archaeol Sci 15:83–97

    Article  Google Scholar 

  • Haslam M (2004) The decomposition of starch grains in soils: implications for archaeological residue analyses. J Archaeol Sci 31:1715–1734

    Article  Google Scholar 

  • Haslam M (2006) Potential misidentification of in situ archaeological tool residues: starch and conidia. J Archaeol Sci 33:114–121

    Article  Google Scholar 

  • 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 11:245–260

    Google Scholar 

  • 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, Oxford

    Google Scholar 

  • 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 25:94–121

    Article  Google Scholar 

  • 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):113–122

    Google Scholar 

  • 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 24:245–250

    Article  Google Scholar 

  • 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 205–212

    Google Scholar 

  • Kamminga J (1982) Over the edge: occasional papers in anthropology, vol 12. University of Queensland Anthropological Museum, St Lucia

    Google Scholar 

  • Keeley LH (1977) The function of Palaeolithic flint tools. Sci Am 237:108–126

    Article  Google Scholar 

  • 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 129–144

    Chapter  Google Scholar 

  • 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 35–46

    Google Scholar 

  • Kraus EH, Hunt WF, Ramsdell LS (1959) Mineralogy: an introduction to the study of minerals and crystals. McGraw-Hill Book Company, New York

    Google Scholar 

  • Langejans GHJ (2010) Remains of the day-preservation of organic micro-residues on stone tools. J Archaeol Sci 37:971–985

    Article  Google Scholar 

  • Langejans GHJ (2011) Discerning use-related micro-residues on tools: testing the multi-stranded approach for archaeological studies. J Archaeol Sci 38:985–1000

    Article  Google Scholar 

  • Langejans GH (2012) Middle Stone Age pièces esquillées from Sibudu Cave, South Africa: an initial micro-residue study. J Archaeol Sci 39(6):1694–1704

  • Langenheim JH (2003) Plant resins. Chemistry, evolution and ethnobotany. Timber Press, Cambridge

    Google Scholar 

  • Lieber RL (2002) Skeletal muscle structure, function, and plasticity. In the physiological basis of rehabilitation, 2nd edn. Lippincott, Williams, & Wilkins, Philadelphia

    Google Scholar 

  • Lillie R (1976) H.J. Conn’s biological stains. Williams and Wilkins, Baltimore

    Google Scholar 

  • Lombard M (2008) Finding resolution for the Howiesons Poort through the microscope: microresidue analysis of segments from Sibudu cave, South Africa. J Archaeol Sci 35:26–41

    Article  Google Scholar 

  • 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 34:155–165

    Article  Google Scholar 

  • Loy TH, Dixon EJ (1998) Blood residues on fluted points from Beringia. Am Antiq 63(1):21–46

    Article  Google Scholar 

  • 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):4349–4362

    Article  Google Scholar 

  • 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 16:299–308

    Google Scholar 

  • 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 10:223–230

    Article  Google Scholar 

  • Mauseth JD (1988) Plant anatomy, vol 560. Benjamin/Cummings Publishing Co., Menlo Park

    Google Scholar 

  • 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):317–340

    Article  Google Scholar 

  • Monnier GF, Ladwig JL, Porter ST (2012) Swept under the rug: the problem of unacknowledged ambiguity in lithic residue identification. J Archaeol Sci 40:3722–3739

    Article  Google Scholar 

  • 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:1–44

  • Monnier G, Frahm B, Luo E, Missal K (2017b) Developing FTIR microspectroscopy for analysis of plant residues on stone tools. J Archaeol Sci 78:158–178

    Article  Google Scholar 

  • Morris VJ (1990) Starch gelatinisation and retrogradation. Trends Food Sci Technol 1:2–6

    Article  Google Scholar 

  • 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 153:176–187

    Article  Google Scholar 

  • Ollé A, Vergès JM (2008) SEM functional analysis and the mechanism of microwear formation. Prehistoric Technology 40:39–49

    Google Scholar 

  • Ollé A, Vergès JM (2014) The use of sequential experiments and SEM in documenting stone tool microwear. J Archaeol Sci 48:60–72

    Article  Google Scholar 

  • Pawlik AF (2004) Identification of hafting traces and residues by scanning electron microscopy and energy-dispersive analysis of X-rays. Lithics in Action, 169–79

  • 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):1699–1708

    Article  Google Scholar 

  • 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):117–154

    Article  Google Scholar 

  • Pedergnana A, Asryan L, Fernández-Marchena JL, Ollé A (2016) Modern contaminants affecting microscopic residue analysis on stone tools: a word of caution. Micron 86:1–21

    Article  Google Scholar 

  • Pollard AM, Heron C (2008) Archaeological chemistry. The Royal Society of Chemistry, Cambridge

    Google Scholar 

  • Raven PH, Evert RF, Eichhorn SE (1999) Biology of plants, 6th edn. W.H. Freeman and Company publishers, New York

    Google Scholar 

  • Raven PH, Evert RF, Eichhorn SE (2005) Biology of plants. W.H. Freeman and Company publishers, New York

    Google Scholar 

  • Reeve RM (1954) Histological survey of conditions influencing texture in potatoes: effects of heat treatments on structure. J Food Sci 19(1–6):323–332

    Article  Google Scholar 

  • 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

    Article  Google Scholar 

  • Rogers AF, Kerr PF (1942) Optical mineralogy. McGraw-Hill Book Company, Inc., New York

    Google Scholar 

  • Ross MH, Pawlina W (2011) Histology: a text and atlas. Loppincott Williams & Wilkins, Baltimore

    Google Scholar 

  • 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):e0150437

    Article  Google Scholar 

  • 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

  • Shanks OC, Bonnichsen R, Vella AT, Ream W (2001) Recovery of protein and DNA trapped in stone tool microcracks. J Archaeol Sci 28:965–972

    Article  Google Scholar 

  • 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 81:219–231

    Article  Google Scholar 

  • 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 54:287–293

    Article  Google Scholar 

  • Steck TL (1989) Red cell shape. In: Stein WD, Bronner F (eds) Cell shape: determinants, regulation, and regulatory role. Academic Press, San Diego, pp 205–246

    Chapter  Google Scholar 

  • Stephenson B (2015) A modified Picro-Sirius red (PSR) staining procedure with polarization microscopy for identifying collagen in archaeological residues. J Archaeol Sci 61:235–243

    Article  Google Scholar 

  • 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):351–370

    Article  Google Scholar 

  • Su XW, Cui FZ (1999) Hierarchical structure of ivory: from nanometer to centimetre. Mater Sci Eng C 7(1):19–29

    Article  Google Scholar 

  • Sussman C (1988) A microscopic analysis of use-wear and polish formation on experimental quartz tools. In: BAR international series, 395. British Archaeological Reports, Oxford

    Google Scholar 

  • Tester RF, Karkalas J, Qi X (2004) Starch—composition, fine structure and architecture. Journal of Cereal Science, 39(2):151–165

  • Teerink BJ (1991) Hair of west European mammals. Atlas and identification key. Cambridge University Press, Cambridge

    Google Scholar 

  • Unger-Hamilton R (1984) The formation of use-wear polish on flint: beyond the “deposit versus abrasion” controversy. J Archaeol Sci 11:91–98

    Article  Google Scholar 

  • 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 34:1001–1010

    Article  Google Scholar 

  • Wadley L, Lombard M, Williamson BS (2004) The first residue analysis blind tests: results and lessons learnt. J Archaeol Sci 31:1491–1501

    Article  Google Scholar 

  • Wheater PR, Burkitt HG, Daniels VG (1987) Functional histology: a text and colour atlas. Longman Group UK limited, Edinburgh

    Google Scholar 

  • 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

    Article  Google Scholar 

  • 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 427:80–93

    Article  Google Scholar 

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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.

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Hayes, E., Rots, V. Documenting scarce and fragmented residues on stone tools: an experimental approach using optical microscopy and SEM-EDS. Archaeol Anthropol Sci 11, 3065–3099 (2019). https://doi.org/10.1007/s12520-018-0736-1

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