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Manganese coating of the Tabun faunal assemblage: Implications for modern human behaviour in the Levantine Middle Palaeolithic
Quaternary International xxx (2013) 1e9
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Manganese coating of the Tabun faunal assemblage: Implications for modern human behaviour in the Levantine Middle Palaeolithic Ana B. Marín-Arroyo a, *, Ma Dolores Landete-Ruiz b, Romualdo Seva-Román b, Mark Lewis c a
Instituto Internacional de Investigaciones Prehistóricas, Universidad de Cantabria, Avda. de los Castros s/n, E-39005 Santander, Spain Unidad de Arqueometría, Universidad de Alicante, Facultad de Ciencias II, E-03080 Alicante, Spain c Dept.of Earth Sciences, Natural History Museum, Cromwell Rd., London SW7 5BD, UK b
a r t i c l e i n f o
a b s t r a c t
Article history: Available online xxx
During the taphonomic and archaeozoological reappraisal of Garrod’s material from Tabun Cave (Mount Carmel, Israel) a distinctive dark colouring of bones was observed in the Level C and D assemblages. Based on several geochemical tests, the presence of insoluble manganese oxides in those coatings was confirmed. The origin of this mineral, given the geological context, could be attributed to the decomposition of large quantities of organic matter due to an intensive human occupation of the site in MIS 5. This fact reinforces the hypothesis of the existence of a larger logistic mobility around more permanent residential sites among anatomical modern humans in the Levantine Middle Palaeolithic, which constitutes early evidence of a more complex economic behaviour. Ó 2013 Elsevier Ltd and INQUA. All rights reserved.
1. Introduction
recently been the object of an exhaustive taphonomic study (Marín-Arroyo, 2013a,b), proving the anthropic origin of Levels C and D, unlike Level B, which was probably the result of a natural accumulation. This analysis also noted significant differences in the appearance of bones, which displayed a dark red-brownish-black colouring in Levels C and D, contrasting with the lighter tone of the remains from Level B. The presence of dark-coloured faunal material at archaeological sites is usually related to the action of fire (Shahack-Gross et al., 1997; Michel et al., 2006; Berna et al., 2012), for example as a consequence of preparing meat for consumption, of cleaning up dwelling spaces, or even of using the bones as fuel (Morin, 2010). However, this apparently unequivocal relationship is not always the case, as some diagenetic modifications, such as mineral staining and micro-organism interaction (Abdel-Maksoud and Abdel-Hady, 2011; Hill, 1982; Kuczumow et al., 2010; López-González et al., 2006; Marín-Arroyo et al., 2008; Potter and Rossman, 1979; Tebo et al., 2005) may also produce a dark colouring of bones, which may in turn have interesting implications for the formation of the deposit. To the naked eye, it is not easy to discern the reason for this type of colouration, and therefore geochemical tests are needed to reveal its true cause. The results of such tests on the faunal remains from Levels C and D at Tabun have shown that the colouring is linked to the presence of manganese oxides. Due to the geological setting of the cave, the most likely sources of this mineral would be the decomposition of organic matter deposited on the cave floor, above all during its occupation by modern humans in MIS 5, and favoured
The archaeological excavations conducted by Dorothy Garrod in the late 1920s and early 1930s on Mount Carmel, in the Wadi elMughara Valley (Israel), were of extraordinary importance in the fields of archaeology and palaeoanthropology (Garrod and Bate, 1937; Smith, 2009). Her research at the caves of Tabun, el-Wad and Skhul not only revealed a long chronological and cultural range, but also provided a large collection of fossil human remains (McCown and Keith, 1939), which later enabled the proposal of the hypothesis of a unique event of alternating occupation of the Near East by Neanderthals and anatomically modern humans (AMH) (Bar-Yosef, 1992). In the case of Tabun Cave, Garrod established a stratigraphic sequence comprising five levels (A, B, C, D and E), which was later reinterpreted by Jelinek (1982) and Jelinek et al. (1973). At present, Levels B, C and D are confidently attributed to the Middle Palaeolithic. Thus, available absolutes dates obtained by means of thermoluminescence, electron spin resonance and U-series (Grün and Stringer, 2000: 602; Mercier and Valladas, 2003) place Level D, related to archaic human species, at the end of MIS 8 or second half of MIS 7; Level C, with AMH fossils, in the first part of MIS 5; and Level B, with Neanderthal remains, at the end of MIS 5 (Shea, 2003, 2008). The macromammal remains found in these three levels have
* Corresponding author. E-mail address: [email protected] (A.B. Marín-Arroyo). 1040-6182/$ e see front matter Ó 2013 Elsevier Ltd and INQUA. All rights reserved. http://dx.doi.org/10.1016/j.quaint.2013.07.016
Please cite this article in press as: Marín-Arroyo, A.B., et al., Manganese coating of the Tabun faunal assemblage: Implications for modern human behaviour in the Levantine Middle Palaeolithic, Quaternary International (2013), http://dx.doi.org/10.1016/j.quaint.2013.07.016
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by the likely environmental conditions inside the cave. This hypothesis would support the residential use of the site at that time and endorse the existence of an increase in logistic mobility with the arrival of populations that were better adapted to travel long distances (Marín-Arroyo, 2013a).
2. Materials and methods 2.1. Taphonomic characteristics of the bone remains The bone assemblage from Tabun Cave was collected during Garrod’s excavations and is currently curated at the Natural History Museum (NHM) in London. According to the results of the recent archaeozoological study (Marín-Arroyo, 2013b), most of the macromammal remains belong to gazelle and fallow deer, although the presence of aurochs is also remarkable due to the possible relevant role this species could have played in the diet of the human populations that occupied the cave. As a consequence of the expedite excavation methods of that time, the assemblage is dominated by nearly whole and easily identifiable bones. During the recent study, a differential colouring of the material was recognized, which was lighter in Level B and darker in the lower Levels C and D. Following the procedure previously applied at El Mirón Cave by Marín-Arroyo et al. (2008), the bone remains were classified in the following categories, according to their colour (see Fig. 1 for an example of each): Type 0: Bones with typical light coloration. Type 1: Bones with a light surface and small, dark brown, circular, internal stains. Type 2: Bones with a uniformly light brown tone and glossy appearance. Type 3: Bones with a uniformly dark brown tone and matt appearance. Type 4: Completely blackened bones with occasional irregular bluish stains superimposed on the black pigmentation The bone remains were not labelled with catalogue codes and no written record existed of their exact provenance, apart from an indication of the level they came from (Tb for Level B, Tc for Level C and Td for Level D). Consequently, there is no data about the precise horizontal and vertical position where each bone was found within the deposit, which has prevented the study of the spatial dispersion of the remains according to their colouring. However, a Colouring Index has been calculated for each level with the following formula:
IC ¼
X
%WTPi $Factori
where %WTPi is the percentage in weight of the bones corresponding to each type of colouring and Factori a value indicating
the intensity of the colouring (Type 0: 0, Type 1: 1, Type 2: 2, Type 3: 3, Type 4: 4). From Levels C and D, 14 dark-coloured bones were selected for geochemical analysis. They are identified in Table 1. Only nine of these had a NHM registry number.
Table 1 Bone samples chosen for analysis. N NHM
Level
Species
Bone element
M82676 M82677 M82678a M82679 M82680 M82681 M82682 M82683 M82684 S1 S2 S3 S4 S5
C C C C C C D D D C C C D D
Dama sp. Dama sp. Indeterminate Gazella sp. Gazella sp. Gazella sp. Capreolus sp. Dama sp. Gazella sp. Gazella sp. Sus scrofa Bos primigenius Indeterminate Gazelle
Phalanx Cranial frg. Humero Radio Ulna Metacarpal Mandible Phalanx Phalanx Phalanx Carpal Phalanx Long bone shaft Mandible
a
With soil attached analysed also in this study.
2.2. Mount Carmel geology Tabun Cave is located in the Valley of Kings (Wadi el-Mughara), some 5 km from the modern coastline, at an altitude of 45 m above sea level (see Fig. 2). The sedimentary structure of the site is linked to the geological history of Mount Carmel. This region is dominated by undifferentiated Upper Cretaceous volcanic rocks (basalt, gabro, ultramafics/pyroclastics and flows) and by Albian, Cenomanian and Turonian sedimentary rocks, intercalating limestone with dolostone, marl, chalk and chert (Sneh et al., 1998). Pliocene gypsum, oolitic limestone, conglomerates and sandstone units are also present in the area. Over these units, quaternary alluvial sedimentation can appear, consisting of gravel, sand, silt and clay. This geological context indicates that the geology of Mount Carmel was formed in magnesium-rich, shallow marine environments and not in deep and benthic marine environments related to contact zones, where igneous emulsions with benthic clays or bentonites with high manganese content usually occur. 2.3. Sedimentology in Tabun Cave Sediment samples from the levels being studied have not been accessible, apart from the material adhering to some of the bones. This lack of potential information has been overcome by making use of the results of the sedimentological studies carried out in the
Fig. 1. Example of the colouration in each category. (Photos by Eduardo Palacio, IIIPC). (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)
Please cite this article in press as: Marín-Arroyo, A.B., et al., Manganese coating of the Tabun faunal assemblage: Implications for modern human behaviour in the Levantine Middle Palaeolithic, Quaternary International (2013), http://dx.doi.org/10.1016/j.quaint.2013.07.016
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Fig. 2. Geographical location of Tabun Cave in Israel (a) and geological map of the Mount Carmel area (b).
past, initially during Garrod’s excavations and later during Jelinek’s work. Garrod describes Level B as red clay, Level C as dark brown loam and Level D as brown sandy loam (Garrod and Bate, 1937: 128). The permeability of the substrate would increase with depth. The organic matter content, determined by chemical analysis on bulk sediment (Jelinek et al., 1973), was low in the upper level (0.31%) and significant in the two lower levels (2.73% in Level C and 2.04% in Level D) (Fig. 3). Jelinek et al. (1973) attribute the origin of Level B to clay soils formed by the erosion of the limestone bedrock, which is abundant on the plateau beneath the cave location and which would have been washed down the shaft opening into the cave. For the same authors, Level C is a continuation of B, with the added peculiarity of the presence of fine intercalated dark red, white and black layers produced by repeated fires. The organic matter content in this stratum varies between 1 and 7%, which is clearly the highest percentage in the stratigraphic sequence. Finally, Level D, as the rest of the lower sequence, differs from the upper levels in its predominantly aeolian origin and its silty-sandy texture. Farrand (1979) defined Level C as a transition between the two main sedimentary processes in the cave: the inwashing of surface clays and the aeolian transport of sand and silt. The same author
also stressed the high mineral content in Levels B and C compared with the rest of the sequence. The previous stratigraphy would be coherent with the occurrence of ponding on the cave floor, which would have been less frequent in the older levels due to their greater permeability. 2.4. Environmental conditions The environmental conditions in which the strata of Tabun Cave were formed can be outlined through the 18O and 13C isotope record obtained by Bar-Matthews et al.’s (2003) from speleothems in the caves of Peqiin (northern Israel) and Soreq (central Israel). By applying the model of Frumkin et al. (1999), the climatic interpretation shown in Fig. 4 can be inferred. As can be seen, the three levels being studied here, attributed to the MIS 7 and MIS 5 interglacial periods, correspond to a temperate and relatively wet climate. 2.5. Geochemical tests The instruments and techniques used to analyse the samples and their justifications are listed below:
Please cite this article in press as: Marín-Arroyo, A.B., et al., Manganese coating of the Tabun faunal assemblage: Implications for modern human behaviour in the Levantine Middle Palaeolithic, Quaternary International (2013), http://dx.doi.org/10.1016/j.quaint.2013.07.016
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Fig. 3. Stratigraphic section of Tabun Cave, showing levels B, C and D.
Scanning electron microscopy (SEM). This technique was applied in order to obtain the elemental composition of the samples (percentages of main chemical elements) by means of an energy-dispersive X-ray microanalysis probe (EDX). A HITACHI S-3000N device was used, equipped with a secondary electron detector (photomultiplier type e 3.5 nm resolution), a semiconductor backscattered electron detector (5 nm resolution), as well as an X-ray detector that was able to detect from Carbon to Uranium. X-ray micro-fluorescence spectrometry (mXRF). This technique of elemental analysis enables the examination of very specific parts of a sample. It is a non-destructive test that, in contrast with conventional X-ray fluorescence, makes use of X-ray optical elements to get a thinner X-ray beam that can focus on a small spot on the sample’s surface. An Orbis Micro-XRF Analyzer from EDAX, with fast and simultaneous multielemental detection from Sodium to Uranium, was used here. Data on the qualitative and quantitative spatial distribution of atomic elements were obtained. X-ray photoelectron spectroscopy (XPS). This technique, which provides binding energy values, allowed the analysis of the superficial coating of bone remains in order to identify the oxidation state of the existing chemical compounds. A VG Scientific, Microtech Multilab spectrometer with a MgKa X-ray source (1253.6 eV) operating at 15 keV and 300 W and applying a pass energy of 50 eV was used here. The pressure inside the analysis chamber was held below 5 108 Torr during the course of the analysis. Binding energies were referenced to the C1 s at 285.0 eV. Multicomponent C1 s photopeaks were curve-fitted using 30% Gaussian/Lorentzian function with a full-width at half-maximum (FWHM) of 1.80 eV. X-ray diffraction (XRD). This technique was used with small samples of soil attached to some bone remains. They were examined on a Bruker D8 Advance X-ray Diffractometer with CuKa radiation (40 kV, 40 mA). Each sample was scanned over the 2-theta range 4e80 with a step size of 0.05 and a count
Fig. 4. Climatic reconstruction of the Levant based on the oxygen-isotope and carbon-isotope profiles from Peqiin and Soreq caves, Israel.
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Fig. 5. Elemental composition of Sample M82679. Test 1.
time of 3 s per step. The diagnostic peaks used as reference and the degree in which reflection is produced were based on the intensities provided by the Joint Committee on Power Diffraction Standards.
Table 3 Manganese and iron content in the samples.
3. Results 3.1. Presence of diagenetic alteration within the sequence The absence of data about the exact position of the bone remains has not allowed the spatial distribution of the phenomenon to be determined precisely. However, it has been possible to appreciate colouring differences in the sequence. Table 2 gives, for each level, the percentages of bones classified in each of the established categories. The darkest colouring occurs in Level C, coinciding with the greatest content of organic matter in the sediment. The degree of staining in Level D is also significant. Table 2 Abundance of each type of colouring categories.
% Type 0 % Type 1 % Type 2 % Type 3 % Type 4 Colouring Index
sodium and magnesium) and large amounts of iron and manganese (see Table 3). The two samples with the darkest colouration (M82679 and S5) were the ones that bore the largest manganese content (see Table 4 and Fig. 5).
Level B
Level C
Level D
26.6 69.3 1.2 1.5 1.4 0.8
4.3 5.5 10.1 40.5 34.0 2.8
22.9 22.9 16.7 30.2 7.3 1.8
3.2. Geochemical tests Firstly, using the Scanning Electron Microscope (SEM-EDX) the elementary composition of each of the samples was determined. Each bone was tested twice in two different areas of its surface. In addition to the components of the bones themselves (calcium, phosphorus and oxygen from apatite and hydroxyapatite), typical clay elements were identified (silicon, aluminium, potassium,
N NHM
Level
% Mn
M82676 M82677 M82678 M82679 M82680 M82681 M82682 M82683 M82684 S1 S2 S3 S4 S5
C C C C C C D D D C C C D D
e e e 1e17% e 0e1% 1e3% 1% 0e2% 0.6% 0.5e1% 1% 0 0.6e9%
% Fe
5e7% 0.3e1% 2e6% 1% 1e2% 3% 1e3% 4% >6% 3e5%
Table 4 Elemental composition (%) of the SEM-EDX analysis of the samples M82679 and S5. Element
C Na Mg Al Si P Cl K Ca Ti Mn Fe O
Sample M82679
Sample S5
Analysis 1
Analysis 2
Analysis 1
Analysis 2
3.51 0.47 0.26 2.92 7.05 6.98 0.47 0.78 19.54 1.26 16.87 5.53 34.36
1.86 0.03 0.35 5.05 11.90 6.46 0.10 0.81 23.06 0.69 0.62 7.26 41.81
2.27 0.66 0.40 2.95 6.41 9.58 0.52 0.40 23.47 e 3.10 3.04 47.20
3.35 0.29 0.11 3.88 7.88 4.29 0.39 0.70 16.99 0.67 8.90 4.83 47.72
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These results were confirmed by the X-ray micro-fluorescence spectrometry (mXRF) analysis. As in the case of the SEM-EDX tests, the samples exhibiting the largest manganese content were M82679 and S5. Both samples also yielded large percentages of calcium and phosphorus from the bone matrix, and small amounts of other elements (iron, silicon, aluminium, potassium and titanium) originating from the sediment. To avoid the interference caused by the main chemical elements of bones (calcium and phosphorus), a small sample of the surface patina of Sample S5 was taken and analysed by mXRF. In this case, the predominance of manganese was made clearer, with a percentage of 43%, followed by calcium, iron, titanium and
potassium, the latter two elements in smaller percentages (see Fig. 6). Sample 5 was also analysed by X-ray photoelectron spectroscopy (see Table 5 and Fig. 7) In this way, the manganese could be assigned to a IV valence, probably corresponding to manganese oxides/hydroxides (transition of manganese 2p3/2, 642.0 eV) (Moulder et al., 1992). In this state, the manganese, which is black in colour, is insoluble in water. Finally, the mineralogy determined by the XRD analysis of the sediment taken from bone M82678 (Fig. 8) displays a composition of igneous and sedimentary origin, in accordance with the geological surroundings of the site. Dahllite has also been identified
Fig. 6. X-ray micro-fluorescence spectrometry of the surface patina of Sample S5.
Please cite this article in press as: Marín-Arroyo, A.B., et al., Manganese coating of the Tabun faunal assemblage: Implications for modern human behaviour in the Levantine Middle Palaeolithic, Quaternary International (2013), http://dx.doi.org/10.1016/j.quaint.2013.07.016
A.B. Marín-Arroyo et al. / Quaternary International xxx (2013) 1e9 Table 5 Atomic and masic percentages of elements of Sample S5.
S S S S S S S
(C) (O) (Ca) (Al) (Si) (Mn) (Fe)
Area T
% Atomic
% Masic
32677,801 223435,8 37972,74 17535,078 11024,88 16393,34 9505,633
19,94288186 51,65161736 5,517695604 14,46142452 6,229959284 1,471274224 0,725147157
12,1370392 41,8729245 11,205497 19,7696369 8,8671207 4,09569827 2,05208336
in the sediment. This mineral compound is linked to the bone remains themselves and comes from the transformation of the apatite, as has previously been observed at the nearby cave of Hayonim (Weiner et al., 2002). In addition to these compounds, phyllosilicates are also present (peak 4.45e4.50 of the XRD). They are in an advanced state of lithification, consequently carbonation processes of clay.
4. Discussion The presence of large numbers of dark-coloured bone remains in Levels C and D at Tabun Cave might at first be attributed to the effect of fire, which would be in accordance with Jelinek et al.’s (1973) observations on the sedimentology of the deposit. However, the results of the geochemical tests performed here on several bone samples from these two levels reveal the existence of a large percentage of manganese IV, black in colour and insoluble in water. This suggests that a series of post-depositional biochemical processes within a certain sedimentary matrix were responsible for the staining of the bones. The source of the manganese should not be geological, as the surroundings of the site are dominated by reef coral calcareous formations intercalated with igneous and sedimentary soils, none of them associated with the presence of manganese. In this scenario, the hypothesis of an organic origin is more likely. In fact, the high proportion of organic matter observed in sedimentological studies and focused primarily on Level C, which contains clear evidence of residential human occupation, in combination with a fairly high degree of humidity, could have favoured the growth of saprophytic micro-organisms, above all within ponding conditions
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like the ones that may have occurred in Tabun Cave (Jelinek et al., 1973). These micro-organisms may have caused the decomposition and mineralisation of the animal and plant organic remains abandoned on the cave floor (Albert et al., 1999, 2000; MarínArroyo, 2013), in the process freeing the metallic ions present in them (Northup and Lavoie, 2001). For example, bacteria like Anthrobacter and Leptothrix are capable of oxidising Mn(II) to Mn(IV) by accumulating MnO2 in their structure (Paul and Clark, 1989; Tebo et al., 2005). During the process of decomposition of the organic matter, simpler substances would be produced, such as polysaccharides, proteins, sugars, amino-acids and humic substances (fulvic, and humic acids and humins) (Porta et al., 1996). The latter, in addition to favouring acidic conditions on the surface, are capable of interacting with Mn cations to create mixed organic-metallic compounds by the intervention of chelating agents in a process called biolixiviation (Brady and Weil, 1996; Vullo, 2003). With this, manganese would be mobilised and could migrate downwards through the sedimentary matrix (the smaller proportion of finer sediments in Levels C and D would permit this progressive infiltration). As the redox and pH conditions of the substrate varied with depth, the behaviour of the manganese compounds could be altered (Porta et al., 1996). The increase in pH, caused for example by the progressive percolation of carbonates from the bedrock or by the combustion in the hearths, in combination with more oxidising conditions associated with drier soils, would favour the transformation of soluble valence II manganese into insoluble forms with valence IV (Dorronsoro et al., 2006). As a result, the manganese would precipitate in the form of oxides and hydroxides (Hill, 1982), and the bone remains would become their main receptors due to their porosity. The staining process would therefore be similar to that identified at the nearby Hayonim Cave (ShahackGross et al., 1997) and at El Mirón Cave, in the north of the Iberian Peninsula (Marín-Arroyo et al., 2008). The verification of the occurrence of this process has implications for the interpretation of the deposit. The greater colouring intensity of bone remains in Level C in comparison with Level D is coherent with a more important human occupation in the former level, which would have resulted in the accumulation of a larger amount of organic matter on the cave floor and in more manganese being freed in the subsequent decomposition process. In a recent
Fig. 7. Manganese XPS spectrum of Sample S5.
Please cite this article in press as: Marín-Arroyo, A.B., et al., Manganese coating of the Tabun faunal assemblage: Implications for modern human behaviour in the Levantine Middle Palaeolithic, Quaternary International (2013), http://dx.doi.org/10.1016/j.quaint.2013.07.016
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Fig. 8. X-ray diffraction pattern of the sediment attached to Bone M82678.
interpretation of the faunal record at Tabun Cave, Marín-Arroyo (2013a,b) studied the skeletal profiles recovered at the site, and their relationship with the topography of the surrounding area. It was suggested there that the site mainly acted as a residential settlement during MIS 5, which would imply that the anatomically modern humans who were responsible for Tabun Level C would have adopted a subsistence strategy based on greater logistic mobility around more permanent residential sites. This hypothesis is coherent with the results obtained by Wallace and Shea (2006) while studying the differences in lithic tool production, and with Lieberman’s (1998) research on the age of death of gazelle individuals to infer the seasonality of human occupations. The new data provided by the geochemical analysis of the staining on bone remains at Tabun Cave support this idea, which would mean that, despite sharing the same technology, modern humans would have occupied the territory in a different way than archaic populations. This particular mobility pattern could be explained by the anatomical differences between both human species. Thus, anatomically modern humans would be more slender and lighter, with longer lower limbs, which would reduce the energetic expenditure involved in travelling between base camps and hunting territories (Steudel-Numbers and Tilkens, 2004; Weaver and Steudel-Numbers, 2005; MacDonald et al., 2009). This would allow them to exploit resources, either located further away or larger in size, with greater efficiency (Cannon, 2003; Marín-Arroyo, 2009). This would therefore be one of the
earliest evidences of intensification in productivity among human species, which in the case of the Levant would also be reflected in the more frequent capture of adult individuals and high-ranked prey (Rabinovich and Tchernov, 1995; Stiner, 2005; Marín-Arroyo, 2013). Hence, the reduction in the amount of resources in the vicinity of the residential site, as a consequence of more persistent occupations, could have obliged these human groups to face economic decisions of greater importance, due to the need to maximise the productivity associated with the consumption of prey of different sizes and/or located at different distances. Acknowledgements The authors would personally like to thank the staff at the Natural History Museum in London for their help during the archaeozoological study of the material, especially Adrian Lister and Andy Currant. We would also like to acknowledge the collaboration of the X Ray and Microscopy Units of the Research Technical Services at the University of Alicante. In addition, we are also grateful to the organisers of the 2nd Taphonomy Working Group Meeting for giving us the opportunity to participate. This research was funded by the Vice-Rectorate at the University of Alicante and by the British Academy. ABMA is currently Ramon y Cajal Research Fellow (RYC-2011-00695) at the University of Cantabria. Finally, ABMA would like to thank David Ocio for his support during this research.
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derived manganese coatings: a study of blackened bones in El Mirón Cave, Cantabrian Spain. Journal of Archaeological Science 35 (3), 801e813. Marín-Arroyo, A.B., 2013a. Palaeolithic human subsistence in Mount Carmel (Israel). A taphonomic assessment of Middle and Early Upper Palaeolithic faunal remains from Tabun, Skhul and el-Wad. International Journal of Osteoarchaeology 23 (3), 254e273. Marín-Arroyo, A.B., 2013b. New opportunities for previously excavated sites: paleoeconomy as a human evolutionary indicator at Tabun Cave (Israel). In: Clark, J., Speth, J. (Eds.), Zooarchaeology and Modern Human Origins. Human Hunting Behavior during the Later Pleistocene. Vertebrate Paleobiology and Paleoanthropology, pp. 59e75. McCown, T.D., Keith, A., 1939. The Stone Age of Mt. Carmel. In: The Fossil Human Remains from the Levallois-Mousterian, vol. 2. Clarendon Press, Oxford. Mercier, N., Valladas, H., 2003. Reassessment of TL age estimates of burnt flints from the Paleolithic site of Tabun Cave, Israel. Journal of Human Evolution 45, 401e 409. Michel, V., Bocherens, H., Théry-Parisot, I., Valoch, K., Valensi, P., 2006. Coloring and preservation state of faunal remains from the Neanderthal levels of Kulna Cave, Czech Republic. Geoarchaeology: An International Journal 21, 479e501. Moulder, J.F., Stickle, W.F., Sobol, P.E., Bomben, K.D. (Eds.), 1992. Handbook of X-ray Photoelectron Spectroscopy. Perkin-Elmer Corp. Minn, USA, Eden Prairie. Morin, E., 2010. Taphonomic implications of the use of bone as fuel. In: ThéryParisot, I., Chabal, L. (Eds.), The Taphonomy of Burned Organic Residues and Combustion Features in Archaeological Contexts. In: Costamagno, S. (Ed.), Proceedings of the Round Table, Valbonne, May 27e29 2008. P@lethnologie, vol. 2, pp. 209e217. Northup, D.E., Lavoie, K.H., 2001. Geomicrobiology of caves: a review. Geomicrobiology Journal 18 (3), 199e220. Paul, E.A., Clark, F.E., 1989. Soil Microbiology and Biochemistry. Academic Press, Inc, San Diego, California. Potter, R.M., Rossman, G.R., 1979. Mineralogy of manganese dendrites and coatings. American Mineralogist 64, 1219e1226. Porta, J., López-Acevedo, M., Roquero, C., 1996. Edafología para la agricultura y el medio ambiente. Mundi-Prensa, Madrid. Rabinovich, R., Tchernov, E., 1995. Chronological, paleoecological and taphonomical aspects of the Middle Paleolithic site of Qafzeh, Israel. In: Buitenhuis, H., Uerpmann, H.P. (Eds.), Archaeozoology of the Near East II. H. Backhuys, Leiden, pp. 5e44. Shahack-Gross, R., Bar-Yosef, O., Weiner, S., 1997. Black-coloured bones in Hayonim Cave, Israel: differentiating between burning and oxide staining. Journal of Archaeological Science 24, 439e446. Shea, J.J., 2003. The Middle Paleolithic of the East Mediterranean Levant. Journal of World Prehistory 17 (4), 313e394. Shea, J.J., 2008. Transitions or turnovers? Climatically-forced extinctions of Homo sapiens and Neanderthals in the east Mediterranean Levant. Quaternary Science Reviews 27, 2253e2270. Smith, P.J., 2009. A Splendid Idiosyncrasy: Prehistory at Cambridge 1915e50. In: BAR International Series 485. Oxford. Sneh, A., Bartov, Y., Weissbrod, T., Rosensaft, M., 1998. Geological Map of Israel, 1: 200,000. Geological Survey of Israel (4 sheets). Items’s URL http://www.gsi.gov. il/Eng/Index.asp?ArticleID¼172&CategoryID¼119&Page¼1 (accessed 21.10.11.). Steudel-Numbers, K., Tilkens, M., 2004. The effect of lower limb length on the energetic cost of locomotion: implications for fossil hominids. Journal of Human Evolution 47, 95e109. Stiner, M.C., 2005. The Faunas of Hayonim Cave (Israel): a 200,000-year Record of Paleolithic Diet, Demography and Society. Peabody Museum of Archaeology and Ethnology, Cambridge. Tebo, B., Johnson, H., McCarthy, J., Templeton, A., 2005. Geomicrobiology of manganese(II) oxidation. Trends in Microbiology 13 (9), 421e428. Vullo, D.L., 2003. Microorganismos y metales pesados: una interacción en beneficio del medio ambiente. Revista Química Viva 2 (3). Items’s URL http://www. quimicaviva.qb.fcen.uba.ar/Actualizaciones/metales/metales.html (accessed 12.09.11.). Wallace, I., Shea, J., 2006. Mobility patterns and core technologies in the Middle Paleolithic of the Levant. Journal of Archaeological Science 33, 1293e1309. Weaver, T., Steudel-Numbers, K., 2005. Does climate or mobility explain the differences in body proportions between Neanderthals and their Upper Paleolithic successors? Evolutionary Anthropology 14, 218e223. Weiner, S., Goldberg, P., Bar-Yosef, O., 2002. Three-dimensional distribution of minerals in the sediments of Hayonim Cave, Israel: diagenetic processes and archaeological implications. Journal of Archaeological Science 29, 1289e 1308.
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Manganese coating of the Tabun faunal assemblage: Implications for modern human behaviour in the Levantine Middle Palaeolithic Ana B. Marín-Arroyo a, *, Ma Dolores Landete-Ruiz b, Romualdo Seva-Román b, Mark Lewis c a
Instituto Internacional de Investigaciones Prehistóricas, Universidad de Cantabria, Avda. de los Castros s/n, E-39005 Santander, Spain Unidad de Arqueometría, Universidad de Alicante, Facultad de Ciencias II, E-03080 Alicante, Spain c Dept.of Earth Sciences, Natural History Museum, Cromwell Rd., London SW7 5BD, UK b
a r t i c l e i n f o
a b s t r a c t
Article history: Available online xxx
During the taphonomic and archaeozoological reappraisal of Garrod’s material from Tabun Cave (Mount Carmel, Israel) a distinctive dark colouring of bones was observed in the Level C and D assemblages. Based on several geochemical tests, the presence of insoluble manganese oxides in those coatings was confirmed. The origin of this mineral, given the geological context, could be attributed to the decomposition of large quantities of organic matter due to an intensive human occupation of the site in MIS 5. This fact reinforces the hypothesis of the existence of a larger logistic mobility around more permanent residential sites among anatomical modern humans in the Levantine Middle Palaeolithic, which constitutes early evidence of a more complex economic behaviour. Ó 2013 Elsevier Ltd and INQUA. All rights reserved.
1. Introduction
recently been the object of an exhaustive taphonomic study (Marín-Arroyo, 2013a,b), proving the anthropic origin of Levels C and D, unlike Level B, which was probably the result of a natural accumulation. This analysis also noted significant differences in the appearance of bones, which displayed a dark red-brownish-black colouring in Levels C and D, contrasting with the lighter tone of the remains from Level B. The presence of dark-coloured faunal material at archaeological sites is usually related to the action of fire (Shahack-Gross et al., 1997; Michel et al., 2006; Berna et al., 2012), for example as a consequence of preparing meat for consumption, of cleaning up dwelling spaces, or even of using the bones as fuel (Morin, 2010). However, this apparently unequivocal relationship is not always the case, as some diagenetic modifications, such as mineral staining and micro-organism interaction (Abdel-Maksoud and Abdel-Hady, 2011; Hill, 1982; Kuczumow et al., 2010; López-González et al., 2006; Marín-Arroyo et al., 2008; Potter and Rossman, 1979; Tebo et al., 2005) may also produce a dark colouring of bones, which may in turn have interesting implications for the formation of the deposit. To the naked eye, it is not easy to discern the reason for this type of colouration, and therefore geochemical tests are needed to reveal its true cause. The results of such tests on the faunal remains from Levels C and D at Tabun have shown that the colouring is linked to the presence of manganese oxides. Due to the geological setting of the cave, the most likely sources of this mineral would be the decomposition of organic matter deposited on the cave floor, above all during its occupation by modern humans in MIS 5, and favoured
The archaeological excavations conducted by Dorothy Garrod in the late 1920s and early 1930s on Mount Carmel, in the Wadi elMughara Valley (Israel), were of extraordinary importance in the fields of archaeology and palaeoanthropology (Garrod and Bate, 1937; Smith, 2009). Her research at the caves of Tabun, el-Wad and Skhul not only revealed a long chronological and cultural range, but also provided a large collection of fossil human remains (McCown and Keith, 1939), which later enabled the proposal of the hypothesis of a unique event of alternating occupation of the Near East by Neanderthals and anatomically modern humans (AMH) (Bar-Yosef, 1992). In the case of Tabun Cave, Garrod established a stratigraphic sequence comprising five levels (A, B, C, D and E), which was later reinterpreted by Jelinek (1982) and Jelinek et al. (1973). At present, Levels B, C and D are confidently attributed to the Middle Palaeolithic. Thus, available absolutes dates obtained by means of thermoluminescence, electron spin resonance and U-series (Grün and Stringer, 2000: 602; Mercier and Valladas, 2003) place Level D, related to archaic human species, at the end of MIS 8 or second half of MIS 7; Level C, with AMH fossils, in the first part of MIS 5; and Level B, with Neanderthal remains, at the end of MIS 5 (Shea, 2003, 2008). The macromammal remains found in these three levels have
* Corresponding author. E-mail address: [email protected] (A.B. Marín-Arroyo). 1040-6182/$ e see front matter Ó 2013 Elsevier Ltd and INQUA. All rights reserved. http://dx.doi.org/10.1016/j.quaint.2013.07.016
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by the likely environmental conditions inside the cave. This hypothesis would support the residential use of the site at that time and endorse the existence of an increase in logistic mobility with the arrival of populations that were better adapted to travel long distances (Marín-Arroyo, 2013a).
2. Materials and methods 2.1. Taphonomic characteristics of the bone remains The bone assemblage from Tabun Cave was collected during Garrod’s excavations and is currently curated at the Natural History Museum (NHM) in London. According to the results of the recent archaeozoological study (Marín-Arroyo, 2013b), most of the macromammal remains belong to gazelle and fallow deer, although the presence of aurochs is also remarkable due to the possible relevant role this species could have played in the diet of the human populations that occupied the cave. As a consequence of the expedite excavation methods of that time, the assemblage is dominated by nearly whole and easily identifiable bones. During the recent study, a differential colouring of the material was recognized, which was lighter in Level B and darker in the lower Levels C and D. Following the procedure previously applied at El Mirón Cave by Marín-Arroyo et al. (2008), the bone remains were classified in the following categories, according to their colour (see Fig. 1 for an example of each): Type 0: Bones with typical light coloration. Type 1: Bones with a light surface and small, dark brown, circular, internal stains. Type 2: Bones with a uniformly light brown tone and glossy appearance. Type 3: Bones with a uniformly dark brown tone and matt appearance. Type 4: Completely blackened bones with occasional irregular bluish stains superimposed on the black pigmentation The bone remains were not labelled with catalogue codes and no written record existed of their exact provenance, apart from an indication of the level they came from (Tb for Level B, Tc for Level C and Td for Level D). Consequently, there is no data about the precise horizontal and vertical position where each bone was found within the deposit, which has prevented the study of the spatial dispersion of the remains according to their colouring. However, a Colouring Index has been calculated for each level with the following formula:
IC ¼
X
%WTPi $Factori
where %WTPi is the percentage in weight of the bones corresponding to each type of colouring and Factori a value indicating
the intensity of the colouring (Type 0: 0, Type 1: 1, Type 2: 2, Type 3: 3, Type 4: 4). From Levels C and D, 14 dark-coloured bones were selected for geochemical analysis. They are identified in Table 1. Only nine of these had a NHM registry number.
Table 1 Bone samples chosen for analysis. N NHM
Level
Species
Bone element
M82676 M82677 M82678a M82679 M82680 M82681 M82682 M82683 M82684 S1 S2 S3 S4 S5
C C C C C C D D D C C C D D
Dama sp. Dama sp. Indeterminate Gazella sp. Gazella sp. Gazella sp. Capreolus sp. Dama sp. Gazella sp. Gazella sp. Sus scrofa Bos primigenius Indeterminate Gazelle
Phalanx Cranial frg. Humero Radio Ulna Metacarpal Mandible Phalanx Phalanx Phalanx Carpal Phalanx Long bone shaft Mandible
a
With soil attached analysed also in this study.
2.2. Mount Carmel geology Tabun Cave is located in the Valley of Kings (Wadi el-Mughara), some 5 km from the modern coastline, at an altitude of 45 m above sea level (see Fig. 2). The sedimentary structure of the site is linked to the geological history of Mount Carmel. This region is dominated by undifferentiated Upper Cretaceous volcanic rocks (basalt, gabro, ultramafics/pyroclastics and flows) and by Albian, Cenomanian and Turonian sedimentary rocks, intercalating limestone with dolostone, marl, chalk and chert (Sneh et al., 1998). Pliocene gypsum, oolitic limestone, conglomerates and sandstone units are also present in the area. Over these units, quaternary alluvial sedimentation can appear, consisting of gravel, sand, silt and clay. This geological context indicates that the geology of Mount Carmel was formed in magnesium-rich, shallow marine environments and not in deep and benthic marine environments related to contact zones, where igneous emulsions with benthic clays or bentonites with high manganese content usually occur. 2.3. Sedimentology in Tabun Cave Sediment samples from the levels being studied have not been accessible, apart from the material adhering to some of the bones. This lack of potential information has been overcome by making use of the results of the sedimentological studies carried out in the
Fig. 1. Example of the colouration in each category. (Photos by Eduardo Palacio, IIIPC). (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)
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Fig. 2. Geographical location of Tabun Cave in Israel (a) and geological map of the Mount Carmel area (b).
past, initially during Garrod’s excavations and later during Jelinek’s work. Garrod describes Level B as red clay, Level C as dark brown loam and Level D as brown sandy loam (Garrod and Bate, 1937: 128). The permeability of the substrate would increase with depth. The organic matter content, determined by chemical analysis on bulk sediment (Jelinek et al., 1973), was low in the upper level (0.31%) and significant in the two lower levels (2.73% in Level C and 2.04% in Level D) (Fig. 3). Jelinek et al. (1973) attribute the origin of Level B to clay soils formed by the erosion of the limestone bedrock, which is abundant on the plateau beneath the cave location and which would have been washed down the shaft opening into the cave. For the same authors, Level C is a continuation of B, with the added peculiarity of the presence of fine intercalated dark red, white and black layers produced by repeated fires. The organic matter content in this stratum varies between 1 and 7%, which is clearly the highest percentage in the stratigraphic sequence. Finally, Level D, as the rest of the lower sequence, differs from the upper levels in its predominantly aeolian origin and its silty-sandy texture. Farrand (1979) defined Level C as a transition between the two main sedimentary processes in the cave: the inwashing of surface clays and the aeolian transport of sand and silt. The same author
also stressed the high mineral content in Levels B and C compared with the rest of the sequence. The previous stratigraphy would be coherent with the occurrence of ponding on the cave floor, which would have been less frequent in the older levels due to their greater permeability. 2.4. Environmental conditions The environmental conditions in which the strata of Tabun Cave were formed can be outlined through the 18O and 13C isotope record obtained by Bar-Matthews et al.’s (2003) from speleothems in the caves of Peqiin (northern Israel) and Soreq (central Israel). By applying the model of Frumkin et al. (1999), the climatic interpretation shown in Fig. 4 can be inferred. As can be seen, the three levels being studied here, attributed to the MIS 7 and MIS 5 interglacial periods, correspond to a temperate and relatively wet climate. 2.5. Geochemical tests The instruments and techniques used to analyse the samples and their justifications are listed below:
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Fig. 3. Stratigraphic section of Tabun Cave, showing levels B, C and D.
Scanning electron microscopy (SEM). This technique was applied in order to obtain the elemental composition of the samples (percentages of main chemical elements) by means of an energy-dispersive X-ray microanalysis probe (EDX). A HITACHI S-3000N device was used, equipped with a secondary electron detector (photomultiplier type e 3.5 nm resolution), a semiconductor backscattered electron detector (5 nm resolution), as well as an X-ray detector that was able to detect from Carbon to Uranium. X-ray micro-fluorescence spectrometry (mXRF). This technique of elemental analysis enables the examination of very specific parts of a sample. It is a non-destructive test that, in contrast with conventional X-ray fluorescence, makes use of X-ray optical elements to get a thinner X-ray beam that can focus on a small spot on the sample’s surface. An Orbis Micro-XRF Analyzer from EDAX, with fast and simultaneous multielemental detection from Sodium to Uranium, was used here. Data on the qualitative and quantitative spatial distribution of atomic elements were obtained. X-ray photoelectron spectroscopy (XPS). This technique, which provides binding energy values, allowed the analysis of the superficial coating of bone remains in order to identify the oxidation state of the existing chemical compounds. A VG Scientific, Microtech Multilab spectrometer with a MgKa X-ray source (1253.6 eV) operating at 15 keV and 300 W and applying a pass energy of 50 eV was used here. The pressure inside the analysis chamber was held below 5 108 Torr during the course of the analysis. Binding energies were referenced to the C1 s at 285.0 eV. Multicomponent C1 s photopeaks were curve-fitted using 30% Gaussian/Lorentzian function with a full-width at half-maximum (FWHM) of 1.80 eV. X-ray diffraction (XRD). This technique was used with small samples of soil attached to some bone remains. They were examined on a Bruker D8 Advance X-ray Diffractometer with CuKa radiation (40 kV, 40 mA). Each sample was scanned over the 2-theta range 4e80 with a step size of 0.05 and a count
Fig. 4. Climatic reconstruction of the Levant based on the oxygen-isotope and carbon-isotope profiles from Peqiin and Soreq caves, Israel.
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Fig. 5. Elemental composition of Sample M82679. Test 1.
time of 3 s per step. The diagnostic peaks used as reference and the degree in which reflection is produced were based on the intensities provided by the Joint Committee on Power Diffraction Standards.
Table 3 Manganese and iron content in the samples.
3. Results 3.1. Presence of diagenetic alteration within the sequence The absence of data about the exact position of the bone remains has not allowed the spatial distribution of the phenomenon to be determined precisely. However, it has been possible to appreciate colouring differences in the sequence. Table 2 gives, for each level, the percentages of bones classified in each of the established categories. The darkest colouring occurs in Level C, coinciding with the greatest content of organic matter in the sediment. The degree of staining in Level D is also significant. Table 2 Abundance of each type of colouring categories.
% Type 0 % Type 1 % Type 2 % Type 3 % Type 4 Colouring Index
sodium and magnesium) and large amounts of iron and manganese (see Table 3). The two samples with the darkest colouration (M82679 and S5) were the ones that bore the largest manganese content (see Table 4 and Fig. 5).
Level B
Level C
Level D
26.6 69.3 1.2 1.5 1.4 0.8
4.3 5.5 10.1 40.5 34.0 2.8
22.9 22.9 16.7 30.2 7.3 1.8
3.2. Geochemical tests Firstly, using the Scanning Electron Microscope (SEM-EDX) the elementary composition of each of the samples was determined. Each bone was tested twice in two different areas of its surface. In addition to the components of the bones themselves (calcium, phosphorus and oxygen from apatite and hydroxyapatite), typical clay elements were identified (silicon, aluminium, potassium,
N NHM
Level
% Mn
M82676 M82677 M82678 M82679 M82680 M82681 M82682 M82683 M82684 S1 S2 S3 S4 S5
C C C C C C D D D C C C D D
e e e 1e17% e 0e1% 1e3% 1% 0e2% 0.6% 0.5e1% 1% 0 0.6e9%
% Fe
5e7% 0.3e1% 2e6% 1% 1e2% 3% 1e3% 4% >6% 3e5%
Table 4 Elemental composition (%) of the SEM-EDX analysis of the samples M82679 and S5. Element
C Na Mg Al Si P Cl K Ca Ti Mn Fe O
Sample M82679
Sample S5
Analysis 1
Analysis 2
Analysis 1
Analysis 2
3.51 0.47 0.26 2.92 7.05 6.98 0.47 0.78 19.54 1.26 16.87 5.53 34.36
1.86 0.03 0.35 5.05 11.90 6.46 0.10 0.81 23.06 0.69 0.62 7.26 41.81
2.27 0.66 0.40 2.95 6.41 9.58 0.52 0.40 23.47 e 3.10 3.04 47.20
3.35 0.29 0.11 3.88 7.88 4.29 0.39 0.70 16.99 0.67 8.90 4.83 47.72
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These results were confirmed by the X-ray micro-fluorescence spectrometry (mXRF) analysis. As in the case of the SEM-EDX tests, the samples exhibiting the largest manganese content were M82679 and S5. Both samples also yielded large percentages of calcium and phosphorus from the bone matrix, and small amounts of other elements (iron, silicon, aluminium, potassium and titanium) originating from the sediment. To avoid the interference caused by the main chemical elements of bones (calcium and phosphorus), a small sample of the surface patina of Sample S5 was taken and analysed by mXRF. In this case, the predominance of manganese was made clearer, with a percentage of 43%, followed by calcium, iron, titanium and
potassium, the latter two elements in smaller percentages (see Fig. 6). Sample 5 was also analysed by X-ray photoelectron spectroscopy (see Table 5 and Fig. 7) In this way, the manganese could be assigned to a IV valence, probably corresponding to manganese oxides/hydroxides (transition of manganese 2p3/2, 642.0 eV) (Moulder et al., 1992). In this state, the manganese, which is black in colour, is insoluble in water. Finally, the mineralogy determined by the XRD analysis of the sediment taken from bone M82678 (Fig. 8) displays a composition of igneous and sedimentary origin, in accordance with the geological surroundings of the site. Dahllite has also been identified
Fig. 6. X-ray micro-fluorescence spectrometry of the surface patina of Sample S5.
Please cite this article in press as: Marín-Arroyo, A.B., et al., Manganese coating of the Tabun faunal assemblage: Implications for modern human behaviour in the Levantine Middle Palaeolithic, Quaternary International (2013), http://dx.doi.org/10.1016/j.quaint.2013.07.016
A.B. Marín-Arroyo et al. / Quaternary International xxx (2013) 1e9 Table 5 Atomic and masic percentages of elements of Sample S5.
S S S S S S S
(C) (O) (Ca) (Al) (Si) (Mn) (Fe)
Area T
% Atomic
% Masic
32677,801 223435,8 37972,74 17535,078 11024,88 16393,34 9505,633
19,94288186 51,65161736 5,517695604 14,46142452 6,229959284 1,471274224 0,725147157
12,1370392 41,8729245 11,205497 19,7696369 8,8671207 4,09569827 2,05208336
in the sediment. This mineral compound is linked to the bone remains themselves and comes from the transformation of the apatite, as has previously been observed at the nearby cave of Hayonim (Weiner et al., 2002). In addition to these compounds, phyllosilicates are also present (peak 4.45e4.50 of the XRD). They are in an advanced state of lithification, consequently carbonation processes of clay.
4. Discussion The presence of large numbers of dark-coloured bone remains in Levels C and D at Tabun Cave might at first be attributed to the effect of fire, which would be in accordance with Jelinek et al.’s (1973) observations on the sedimentology of the deposit. However, the results of the geochemical tests performed here on several bone samples from these two levels reveal the existence of a large percentage of manganese IV, black in colour and insoluble in water. This suggests that a series of post-depositional biochemical processes within a certain sedimentary matrix were responsible for the staining of the bones. The source of the manganese should not be geological, as the surroundings of the site are dominated by reef coral calcareous formations intercalated with igneous and sedimentary soils, none of them associated with the presence of manganese. In this scenario, the hypothesis of an organic origin is more likely. In fact, the high proportion of organic matter observed in sedimentological studies and focused primarily on Level C, which contains clear evidence of residential human occupation, in combination with a fairly high degree of humidity, could have favoured the growth of saprophytic micro-organisms, above all within ponding conditions
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like the ones that may have occurred in Tabun Cave (Jelinek et al., 1973). These micro-organisms may have caused the decomposition and mineralisation of the animal and plant organic remains abandoned on the cave floor (Albert et al., 1999, 2000; MarínArroyo, 2013), in the process freeing the metallic ions present in them (Northup and Lavoie, 2001). For example, bacteria like Anthrobacter and Leptothrix are capable of oxidising Mn(II) to Mn(IV) by accumulating MnO2 in their structure (Paul and Clark, 1989; Tebo et al., 2005). During the process of decomposition of the organic matter, simpler substances would be produced, such as polysaccharides, proteins, sugars, amino-acids and humic substances (fulvic, and humic acids and humins) (Porta et al., 1996). The latter, in addition to favouring acidic conditions on the surface, are capable of interacting with Mn cations to create mixed organic-metallic compounds by the intervention of chelating agents in a process called biolixiviation (Brady and Weil, 1996; Vullo, 2003). With this, manganese would be mobilised and could migrate downwards through the sedimentary matrix (the smaller proportion of finer sediments in Levels C and D would permit this progressive infiltration). As the redox and pH conditions of the substrate varied with depth, the behaviour of the manganese compounds could be altered (Porta et al., 1996). The increase in pH, caused for example by the progressive percolation of carbonates from the bedrock or by the combustion in the hearths, in combination with more oxidising conditions associated with drier soils, would favour the transformation of soluble valence II manganese into insoluble forms with valence IV (Dorronsoro et al., 2006). As a result, the manganese would precipitate in the form of oxides and hydroxides (Hill, 1982), and the bone remains would become their main receptors due to their porosity. The staining process would therefore be similar to that identified at the nearby Hayonim Cave (ShahackGross et al., 1997) and at El Mirón Cave, in the north of the Iberian Peninsula (Marín-Arroyo et al., 2008). The verification of the occurrence of this process has implications for the interpretation of the deposit. The greater colouring intensity of bone remains in Level C in comparison with Level D is coherent with a more important human occupation in the former level, which would have resulted in the accumulation of a larger amount of organic matter on the cave floor and in more manganese being freed in the subsequent decomposition process. In a recent
Fig. 7. Manganese XPS spectrum of Sample S5.
Please cite this article in press as: Marín-Arroyo, A.B., et al., Manganese coating of the Tabun faunal assemblage: Implications for modern human behaviour in the Levantine Middle Palaeolithic, Quaternary International (2013), http://dx.doi.org/10.1016/j.quaint.2013.07.016
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A.B. Marín-Arroyo et al. / Quaternary International xxx (2013) 1e9
Fig. 8. X-ray diffraction pattern of the sediment attached to Bone M82678.
interpretation of the faunal record at Tabun Cave, Marín-Arroyo (2013a,b) studied the skeletal profiles recovered at the site, and their relationship with the topography of the surrounding area. It was suggested there that the site mainly acted as a residential settlement during MIS 5, which would imply that the anatomically modern humans who were responsible for Tabun Level C would have adopted a subsistence strategy based on greater logistic mobility around more permanent residential sites. This hypothesis is coherent with the results obtained by Wallace and Shea (2006) while studying the differences in lithic tool production, and with Lieberman’s (1998) research on the age of death of gazelle individuals to infer the seasonality of human occupations. The new data provided by the geochemical analysis of the staining on bone remains at Tabun Cave support this idea, which would mean that, despite sharing the same technology, modern humans would have occupied the territory in a different way than archaic populations. This particular mobility pattern could be explained by the anatomical differences between both human species. Thus, anatomically modern humans would be more slender and lighter, with longer lower limbs, which would reduce the energetic expenditure involved in travelling between base camps and hunting territories (Steudel-Numbers and Tilkens, 2004; Weaver and Steudel-Numbers, 2005; MacDonald et al., 2009). This would allow them to exploit resources, either located further away or larger in size, with greater efficiency (Cannon, 2003; Marín-Arroyo, 2009). This would therefore be one of the
earliest evidences of intensification in productivity among human species, which in the case of the Levant would also be reflected in the more frequent capture of adult individuals and high-ranked prey (Rabinovich and Tchernov, 1995; Stiner, 2005; Marín-Arroyo, 2013). Hence, the reduction in the amount of resources in the vicinity of the residential site, as a consequence of more persistent occupations, could have obliged these human groups to face economic decisions of greater importance, due to the need to maximise the productivity associated with the consumption of prey of different sizes and/or located at different distances. Acknowledgements The authors would personally like to thank the staff at the Natural History Museum in London for their help during the archaeozoological study of the material, especially Adrian Lister and Andy Currant. We would also like to acknowledge the collaboration of the X Ray and Microscopy Units of the Research Technical Services at the University of Alicante. In addition, we are also grateful to the organisers of the 2nd Taphonomy Working Group Meeting for giving us the opportunity to participate. This research was funded by the Vice-Rectorate at the University of Alicante and by the British Academy. ABMA is currently Ramon y Cajal Research Fellow (RYC-2011-00695) at the University of Cantabria. Finally, ABMA would like to thank David Ocio for his support during this research.
Please cite this article in press as: Marín-Arroyo, A.B., et al., Manganese coating of the Tabun faunal assemblage: Implications for modern human behaviour in the Levantine Middle Palaeolithic, Quaternary International (2013), http://dx.doi.org/10.1016/j.quaint.2013.07.016
A.B. Marín-Arroyo et al. / Quaternary International xxx (2013) 1e9
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Please cite this article in press as: Marín-Arroyo, A.B., et al., Manganese coating of the Tabun faunal assemblage: Implications for modern human behaviour in the Levantine Middle Palaeolithic, Quaternary International (2013), http://dx.doi.org/10.1016/j.quaint.2013.07.016