Arrhaeomerty 40, 1 (1998). 177-185.

Printed in Great Britain

PALAEOCLIMATIC IDENTIFICATION BASED ON AN ISOTOPE

STUDY O F TRAVERTINE FROM THE COPPER AGE SITE AT
LOS MILLARES, SOUTH-EASTERN SPAIN”

J . CAPEL,’ E. REYES,2 A. DELGAD0,2 R. NUNEZ2 and F. MOLINA’

‘ Departamento de Prehisioria y Arqueologia, Facultad de Filosof ia y Letras, Campus de Cartuja, 18071 Granada,
Spain
2Laborairwiode Geoquimica de lsdtopes Esiables, Departamenr de Ciencias de la Tierra. Estacidn Experimental del
Zaidin CSIC. ProfessorAlbareda I , 18008 Granada, Spain

Remains of an aqueduct from the Copper Age settlement of Los Millares have been studied.
The isotope results (-7%o < 6”O - 5.3%0)show that the aqueduct was used to transport
fresh water at room temperature. The results are inconsistent with the aqueduct being used f o r
hot water transport or as a container f o r water exposed to evaporation processes. Both
isotopic and mineralogical results were useful in identifiing the origin and use of building
materials and also in determining climatic conditions during the time of the settlement
occupation.

KEYWORDS SPAIN, LOS MILLARES, COPPER AGE, STABLE ISOTOPES, TRAVERTINE,

PALAEOCLMATE

INTRODUCTION

The Los Millares site lies in the Santa FC de Mondujar area (Almeria, south-eastem Spain). The
results of a recent excavation (Arribas et al. 1987) showed that the earliest phase of this Copper
Age site, ‘Millares 1’, dates to the Old Copper Age (2700-2400 BC). The next phase of the
settlement, ‘Millares IIa’, marked the transition to the Copper Age proper. The subsequent
phase, ‘Millares IIb’, dates to the Recent Copper Age (2000-1900 BC). The final phase,
‘Millares III’, was a period of changes culminating in the appearance of the first ‘Argiiricas’
populations, which marked the beginning of the Bronze Age.
The first excavation at this site was carried out in 1891-2 by H. L. Siret, the results of which
were published in the Revue des Questions Scientifques. Siret (1893) described a construction
made of travertine inside the settlement. The author referred to this structure as an ‘aqueduct’,
the purpose of which was apparently to direct the water flow to a water cistern inside the
settlement (Fig. I). More recent excavation results (Arribas et al. 1987,245-62) have suggested
that Siret’s hypothesis was not totally accurate. Nevertheless, for the sake of convenience, in the
present study we use the term ‘aqueduct’ when referring to the study area, without wishing to
enter into the debate about whether this construction is actually a true aqueduct or not, as this
question is to be addressed by a number of other authors.
The widespread distribution of hot springs in the area surrounding the Los Millares
archaeological site could, however, suggest a different contextuaVfunctiona1 interpretation
for the aqueduct, according to the type of water that was transported. The use made of the

* Received 12 November 1997. accepted 4 March 1997

177
178 J. Capel, E. Reyes, A. Delgado, R. Nuiiez and F. Molina

Figure 1 Location of the aqueduct (arrowed). (a): Plan of Los Millares (afier Siret 1893,jg. 168); (b): schematic of the
Millares settlement, the fort$cation’s southern and central sector (Arribas et al. 1987, 251,jg. 4); (c): reconstruction of
the fortification lines (phases I and I la).

aqueduct by the Copper Age settlers at Los Millares could have served a socio-economic
purpose, with the ‘aqueduct’ being used to transport the settlement’s water supply, and as a
watering place for animals, external to the wall of the fortification which encloses the
inhabited area (Fig. 1 (c)). The data obtained will, therefore, provide the main basis for the
development of any hypothesis regarding the socio-economic nature of the creation and
development of the aqueduct.
The aim of the isotope study of travertine materials from the Los Millares archaeological
site was to determine the temperature of the water flowing along the aqueduct andor the
palaeoclimatic conditions that were prevalent when the first communities settled there. We also
wished to obtain complementary information on the type and origin of the materials used in the
construction of the aqueduct, as well as any evidence of rebuilding.

MATERIALS A N D METHODS

The samples were taken from both the archaeological remains of an ‘aqueduct’ and the
calcareous platform upon which the Copper Age settlement at Los Millares was built. On the
‘aqueduct’, surface samples (Fig. 2) were taken from the watercourse (Sl-3), together with a
vertical sample (TRl-5), a sample from the interior of a small lamination (T1/6), and a sample
from the stones embedded in the ‘aqueduct’ (Dl-7). A significant amount of the material used in
the construction of the settlement was composed of small boulders taken from the calcareous
crust. There is evidence to suggest that some of these boulders may also have been used in the
 Palaeoclimatic ident$cation based on an isotope study 179

05 ,,D1
1

D6

E
r
TR 5
TR4 1

Figure 2 Diugruni of sampling from the ‘aqueduct’. ( S ) : surface samples; (TR):verticul sequence; (T): laminated
sequence: (D): boulders.

construction of the ‘aqueduct’. Samples were, therefore, also taken of the different levels
comprising the soil crust (C) (Fig. 3).
The carbonate isotope analysis was carried out according to the method described by Walters
et al. (1972), which in t u n was based on that of McCrea (1950). This method consists of

f -l ‘L ALLUVIAL

C1a
Cl b
c2
c 3

Sub C

Figure 3 Diagram of sampling from the edaphic crust. (Cla): compact limestone; (C1b): microconglomerate with a
cornpact CarblJnUfemutrix (highly variable, from centimetric to decimetric in size); (C2): fine, compact conglomerate
with (millitnetric) pebbles; (C3): conglomerate with gneiss pebbles and boulders, earthy carbonate cement; (Sub C):
,stones and boulders (from centrimetric to decimetric in size). bonded by a finer carbonate conglomerate morrix.
180 J. Capel, E. Reyes, A. Delgado, R. Nuiiez and F. Molina

attacking the samples with ultrapure (100%) P04H3.The calcites were attacked at 25 "C for 2
hours. For the dolomites, the temperature was increased 50 "C and the exposure time to 24 hours.
Measurement of the isotope composition of the C 0 2 thus obtained was carried out with a
Finnigan-Mat 25 1 mass spectrometer. The mineralogical analysis was performed by X-ray
diffraction.

RESULTS AND DISCUSSION

The composition of the travertine samples from the 'aqueduct' was 100% calcite, presenting
& I 8 0 values ranging between -7%0 and -5.3%0 (PDB), with a mean value of -5.8%0 (PDB).
These values enable the water temperature to be calculated, and may also provide evidence of
any significant evaporation of still water. The formation temperatures were calculated from the
equation given by Anderson and Arthur (1983):

t " C = 16-4.14(6,-6,)+0.13(6,-6,)2
where 6, and 6, are, respectively, the 6 l 8 0 values of the carbonate and the water with which it
precipitated in equilibrium.
The isotopic composition of rainwater and, therefore, also that of meteoric waters, is affected
by the prevailing climatic conditions. Thus, Dansgaard (1964) reported global variations of
0.69%0/"C. However, in the Mediterranean region somewhat shallower slopes have been
reported for Sicily, Italy (0.39%0pC: Hauser et al. 1980) and Granada, Spain (0.34%0l"C:
Delgado et al. 1991). Since the end of the last Ice Age 10000 years ago, the earth has enjoyed
relatively constant climatic conditions (i.e., the 'climatic optimum'), which has characterized the
entire Holocene epoch (COHMAP 1988; Dansgaard et al. 1993; Thompson et al. 1995). The
isotopic composition of the rain and meteoric waters in the region during the Copper Age ought,
therefore, to have been similar to that found today. In the southern Iberian Peninsula values of
around -5%0 have been recorded at sea level in Gibraltar (IAEA 1981) and of -7.45%0 at an
altitude of 600m in Granada (Delgado et al. 1991). In areas which are located very near to the
study area the following equation can be used to relate altitude to the 6I8O (Benavente et al.
1992):
y = -1735.71 - 357.14~
This equation gives a 6 I 8 0 value of -5.6%0 for the Los Millares site. Since a climatic fluctuation
of 1 "C would have a corresponding effect of approximately ? 0.5%0(considering an inter-
mediate slope between the global and Mediterranean values), in order to calculate the
temperature we have considered the meteoric waters to have 6 l 8 0 values between -5.1 and
-6.l%0.
The temperatures obtained are shown in Table 1. For waters with 6l8O values of -5.1%0,
-5.6%0 and -6.l%0, mean temperatures of 19.2 "C, 17.1 "C and 15 "C are obtained, respectively.
The present-day mean temperatures in the region range between 15°C and 18"C, so the data
obtained are plausible. With regard to the extreme values shown in Table 1, maximum
temperatures of 24.4 "C and minimum temperatures of 12.9 "C correspond to seasonal changes.
The relatively negative 6I8O values of the travertine material seem to suggest that the occurrence
of significant evaporation processes which would be expected for still waters may be discounted.
This can be confirmed if we fix the temperature between 15"C and 20 "C, and calculate the
 Palaeoclimatic identijication based on an isotope study 181

Table I Isotopic (6"O and 6'jC) composition of the travertine contained in the 'aqueduct'. Tempera-
tures have been calculated for various types of meteoric waters

Sample 6" c 6l8O T "C T "C T "C

(PDB) (PDB) (6I8O,,, = -5.1) (6"O0,= -5.6) (6"0, = -6.1)

S1 -7.7 -7.0 24.4 22.1 19.9

s2 -6.2 -6.6 22.4 20.2 18.0
s3 -4.7 -5.9 19.5 17.3 15.3
TR I -4.2 -5.1 18.5 16.4 14.4
TR2 -3.8 -5.4 17 15.0 13
TR3 -4.2 -5.3 16.9 14.9 12.9
TR4 -3.9 -5.5 17.6 15.5 13.4
TR5 -4.1 -5.6 17.9 15.8 13.8
TI -4. I -5.5 17.8 15.7 13.6
T2 -4. I -5.9 19.4 17.3 15.2
T3 -6.4 -6.6 22.4 20.2 18.0
T4 -5.9 -6.2 20.5 18.4 16.3
T5 -5.1 -5.5 27.7 15.6 13.6
T6 -3.1 -5.3 16.9 14.9 12.9
Mean -4.8 -5.8 19.2 17.1 15.0

isotopic composition of the waters (see Fig. 4). The values obtained range between -4.4%0 and
-7.3%0 (SMOW), which are normal for the study area, and are not enriched with l8O as they
would be if tightly evaporated waters were involved.
The carbon isotope composition is somewhat more heterogeneous: -7.7 < 613C < -3.7. The
possible sources of carbon for these waters would be C 0 2 from the decay and respiration of
plants, atmospheric C02, and limestone (widely found in the region). (Edaphic carbonates that
developed in areas where the only plants present follow the C3 photosynthesis cycle present 6I3C
values which are very close to -12%0. However, carbonates originating in areas with a warm,
arid climate-where C4 plants predominate-have 613C values which are close to +2%0
(Deines 1980; Cerling 1984; Salomons and Mook 1986; Quade et al. 1989).) The sample with
the most negative value (6I3C = -7.7) coincides with the most negative oxygen value, so it
appears that little evaporation took place. This 6I3C value indicates a supply of C 0 2 that mainly
originated from C3 plants, with a smaller proportion of I3C-rich carbon from C4 plants and
atmospheric C02 and/or carbon from dissolved limestone. During drier periods, the meteoric
waters would be richer in I8O. A decrease in vegetation cover would also mean that atmospheric
13C-enrichedC 0 2 would play a greater role in the soils (Cerling 1991). Furthermore, the greater
water-rock interaction may lead to a higher proportion of carbon from the dissolution of
limestone. Thus, alternating cycles of dry and wet periods may explain the positive correlation
between 6 ' * 0 and 6I3Cfound in the travertine. However, this correlation could also be explained
by the preferential freeing of both I6O and 12Cduring evaporation (Gonfiantini et al. 1968; Turi
1986; Leslie et al. 1992).
The edaphic carbonates comprising the calcareous crust upon which the settlement was built
present completely different isotope values, according to their origin and age. There is also a
correlation between 6 I 8 0 and 613Cbut with a different slope from that of the travertine (Fig. 5 ) .
The enrichment in I8O within the palaeosols can be explained by evaporative precipitation of
182 J. Capel, E. Reyes, A. Delgado, R. Nuiiez and F. Molina

-10 -9 -8 -7 -6 -5 -4 -3 -2 -1 0 1 2
6"o %o(PDB) CALCITE
Figure 4 The curving lines represent theoretical water temperatures (isotopic Composition is indicared in circles) in
equilibrium with calcite (x-axis), calculated from the equation given by Anderson and Arthur (1983).The shaded area
indicates the temperature range obrained considering wafers with 6"O values ranging between -5.1%0 and -6.1%0
(SMOW). If the temperature range isfuced between 15 "Cand 20"C, the isotopic composition of the waters would range
between -7.3%0 and -4.4%0, indicating that no significant evaporation processes took place.

calcite during soil formation (Salomons et al. 1978; Videtich and Matthews 1980). The
relatively high 6 ' * 0 values indicate semi-arid conditions; similar values and tendencies have
previously been described for this area by Solomons et al. ( 1978) and Delgado (1 993).
As mentioned above, the 'aqueduct' includes small boulders of varying size and composition
(travertine and limestone). In order to determine their origin, their isotopic and mineral
compositions were analysed (Tables 2 and 3). The travertine boulders originate from the
'aqueduct' itself, as shown not only by their structure but also by their isotopic composition (see
Fig. 5 ) . However, the compact structure and reddish colour of the calcareous boulders would
suggest that they originated from the calcareous crust upon which the settlement was built. This
hypothesis may be confirmed by isotope analysis, as the composition of the boulders is identical
(6"O = -3.313.4) to that of the C1 level of the edaphic crust. Furthermore, these boulders
contain considerable quantities of quartz and mica, as does the calcareous crust. The fact that the
'aqueduct' has been strengthened in places by boulders from the 'aqueduct' itself and elsewhere
would indicate that maintenance work was subsequently carried out on the structure.

CONCLUSION

The travertine carbonates of the 'aqueduct' at Los Millares were formed by the circulation of
 Palaeoclimatic ident$cation based on an isotope study 183

-2 -

-
-4

-6-

-8-

1 , l , 1 1
-10‘ I
-8 -7 -6 -5 -4 -3 -2 -1 0

6”O %O (PDB)
Figure 5 Isotopic composition of the cements (lineA: 613C = 26“O +
7; r = 0.89, n = 14) and boulders of which the
‘aqueduct’ is composed. Relationship with the carbonate ofedaphic origin (line B: 6°C = 0.646’80 - 2.64; r = 0.74,
n = 6 ) present in the area.

meteoric waters at environmental temperatures and under variable local climatic conditions,
which were somewhat more humid than present-day conditions. We must, therefore, discount
hypotheses that suggest that the ‘aqueduct’ was used to redirect hot-spring waters or was used as
a container for still waters prone to evaporation processes.
Maintenance work was carried out on the ‘aqueduct’, using materials that had broken off from
the ‘aqueduct’ itself or the calcareous crust. The isotopic composition of the various components
has enabled these problems to be resolved.
The isotope values of the calcareous crust upon which the Los Millares settlement was built
correspond to those of an edaphic crust, formed in a semi-arid environment which was similar to
the present one.

Table 2 Mineralogical and isotopic cornposition of the boulders sampled

Sample Description Calcite Quartz. Mica d80(PDB) 6°C (PDB)

DI Calcrete 74 25 1 -1.9 -3.4

D2 Calcrete 74 25 I -3.3 -4.8
D3 Calcrete 14 25 I -1.8 -3.6
D4 Calcrete 73 21 6 -3.4 -4.3
D5 Travertine I00 - - -5.3 -2.2
D6 Travertine I00 - - -6.0 -5.9
D7 Travertine I00 - - -5.1 -3.8
184 J. Capel, E. Reyes, A. Delgado, R. Nuiiez and F. Molina

Table 3 Mineralogical and isotopic composition of the various levels of the edaphic crust. Ca: Calcite; Do: dolomite;
Q: quartz; Mi: mica; FtK: potassium feldspar: Ha: halite

Sample Ca Do Q Mi FtK Ha 6'80co 6"CCa 6"OD, 6I3CD,

Cla 70 T 24 6 T - -3.2 -4.0 - -

Clb 81 T 15 4 T - -3.7 -5.6 - -
c2 33 15 32 13 7 - -4.5 -6.0 -0.8 -4.3
c3 36 28 24 9 3 - -4.3 -5.0 -2.7 -3.9
SubC 40 20 26 8 3 3 -4.9 -4.5 -2.8 -4.1

ACKNOWLEDGEMENT
This work has been supported by the projects PB-910072 and PS-0077 of DGICYT.

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