Abstract
One of the most critical found objects from the site of Shahr-i Sokhta are lapis lazuli stones and beads, which were used as stone jewelry and ornaments. One of the site’s most significant archaeological and archaeometry topics is the way of manufacturing and types of stone structures into these objects. The Shahr-i Sokhta’s lapis lazuli beads manufactured with flint borers are in the forms of lens, lozenge, circle, etc., and were used as jewelry and ornaments such as bracelets, anklets, necklaces, etc. The main discussion in this research is recognizing the structure and studying the mineralogy of lapis lazuli beads discovered from Shahr-i Sokhta. Hence, by using laboratory-device methods such as petrography of thin sections, X-ray energy diffraction microanalysis, Raman Spectroscopy analysis, and gemology methods, this research studies the structures of three samples of lapis lazuli beads and stones of Shahr-i Sokhta. The results of laboratory studies show that Shahr-i Sokhta’s structure of lapis lazuli stone consists of lazurite minerals with a high percentage of calcite mineral impurities, which causes a reduction of transparency and purity of the lapis lazuli stones; also, elemental studies represent the presence of lazurite minerals. Raman structural and gemological studies show the structure, the amount of absorption coefficient, and its specific weight in the main structure of lapis lazuli stone. Chemical and structural studies indicate that the stones are similar in terms of composition.
Keywords: Stone Jewelries, Lapis Lazuli, Archeaometry, Shahr-i Sokhta in Sistan, South-east of the Iranian Plateau.
Introduction
Shahr-i Sokhta is one of the most important and key sites among Bronz-age sites in southeast Iran’s archaeology (Biscione et al., 1974; Tosi, 1968, 1969, 1973; 1976; Tosi and Piperno, 1975; Savatori & Vidale, 1997; Piperno & Salvatori, 2007). Through excavations during different years up to now, a vast majority of semiprecious Stones and jewelry have been discovered; some of them are healthy beads in the form of necklaces, bracelets, and anklets, while others are half-worked beads as well as raw stone and blocks (Foglini, 1998). The jewelry is lapis lazuli, agate, chlorite, turquoise, limestone, flint, jasper, marble (calcite and aragonite), quartz, green tuff, and chert; that one of the most significant of them is lapis lazuli which was brought to Shahr-i Sokhta as a result of the trade from other regions. lapis lazuli stone in various forms and shapes is the most discovered abundant cultural material in Shahr-i Sokhta (Sajjadi, 2005, 2007). The discovered lapis lazuli are healthy and semi-worked, as well as raw and discarded material. The archaeological studies have demonstrated that the raw lapis lazuli blocks were imported into Shahr-i Sokhta, and then they were changed into various artifacts by artisans (Farzin et al., 2019). Hence, recognizing the structure and method of manufacturing the discovered lapis lazuli beads from Shahr-i Sokhta could be one of the most important topics for archaeologists. The archaeo-gemological study is a field of archaeometry that investigates and recognizes the structure and method of manufacturing and polishing these semiprecious Stone ornaments and jewelry. Archaeo-gemological studies examine minerals, gem materials, and jewelry, which were used as ornaments, decorative objects, jewelry materials, etc., in particular eras and places of the ancient world (Hatipoglu & Guney, 2013; Rapp, 2009; Dominguez-Bella, 2012). Therefore, this research based on Archaeo-gemological studies investigates the preliminary lapis lazuli stone jewelry produced in Shahr-i Sokhta.
Material and Methods (Samples)
The selected samples in this research include three pieces of lapis lazuli discovered from the archaeological survey of Shahr-i Sokhta. One of the samples is a raw material with a small incision that had been discarded as waste (SH-L1). The other one is a rectangular object with grooves in its width, which was broken during use (SH-L2), and the last one is a tiny bead; all three are studied in this research (SH-L3).
Methods
Microscopic thin section petrography (OPM) is administered to examine the samples under a polarizing microscope. The device model used in this research is James Swift, made in England.
The elemental Micro-analysis EDX method is applied to recognize samples chemical combinations. This examination is conducted through EDX devise coupled with a field emission electron microscope (FESEM) manufactured by Tasken company, model MIRA3TESCAN-XMU.
For structural investigation of the samples, this research uses Raman spectroscopy examination through (Takram) P50C0R10 model device, Taskan company in Raman laboratory. This device has a laser wavelength of 532nm (Nd: YAG Laser), and the range of Raman shift RS is 100-4600.
Moreover, this study uses gemological methods such as specific weight and refractive index to identify the samples.
Results
Petrography
According to the petrographic studies of the lapis lazuli samples under a polarizing microscope, blue lazurite minerals are seen with white calcite.
Raman Spectroscopy
The obtained spectra from this chart are compared with the reference spectrum at http://www.rruff.info This comparison indicates the existing lazurite in the stone structure of Na3Ca(Si3Al3)O12S. There is a Raman spectrum in the range of 546 cm-1, 1092 cm-1, and 254 cm-1, and the intensified spectrum is high in the range of 546 cm-1, considered the main spectrum.
EDX
Micro-analysis (EDX) Obtained spectra in the formula of these stones represent the amount of silicon (19/61 and 19/11), aluminum (7/14 and 7/21), magnesium (7/98 and 6/73), calcium (4/98 and 4/94), and sodium (3/46 and 3/13) elements with the highest abundance.
Gemological Analysis
This part investigates these lapis lazuli’s mineralogical features through two refractometer methods and the determination of specific weight.
Refractometer
Among Shahr-i Sokhta’s studied samples, this research has selected three lapis lazuli samples to study. For investigating, first, one drop of special liquid (REFRACTOMETER LIQUID-Nd 1.81) is poured into the location of the samples; second, the flat sides of the gems locates on the oil. Then, by turning on the device lamp and closing the deflectometer cap, one could obtain each sample’s refractive coefficient measure by reading the refractive coefficient. The type of the studied sample has been identified by measuring the refractive coefficient of the samples and comparing obtained numbers with the standard table of gems (GIA- GEM PROPERTY CHART). The refractive coefficient of 1.50 is related to lapis lazuli stone.
Determination of Specific Weight
One of the quick identifying ways of the gems is the determination of their specific weight, which causes no damage to the gems. To obtain the particular weight of each mineral or gem, first, they are weighted in the air and then in the water. Next, by using a formula, the amount of specific weight is calculated. The particular weight of the discovered lapis lazuli samples of Shahr-i Sokhta is 2.1-3.3.
Conclusion
Microscopic investigations based on the thin section petrography show that the structure of studied lapis lazuli is lazurite mineral type with calcite minerals. In microscopic images, Lazurite minerals clearly are blue, calcite minerals in the stone texture are white, and pyrite minerals rarely can be seen in the studied stone texture. Identifying the existence of a significant amount of calcite and a poor amount of pyrite in the lapis lazuli structure represents the amount of impurities in these stones. Furthermore, elemental analysis of the three lapis lazuli indicates that there are other elements with the highest frequency; these elements are silicon (20/95 and 20/67), aluminum (7/80 and 7/63), magnesium (7/28 and 8/52), calcium (4/94 and 5/33), sodium (3/34 and 3/74) and sulfur (0/66 and 1/09). In fact, lapis lazurite is a blue stone whose chemical composition is variable, and its basic composition is mineral lazurite consisting of aluminum, calcium, and sodium silicates. Lapis lazuli consists of several different minerals, such as sodalite, hauynolith, calcite, pyrite, and lazurite, which are lapis lazuli’s main components. Fewer white calcite spots and more yellow pyrite in the lapis lazuli indicate the best quality of the lapis lazuli. In table 3, silicon element (29.87%) and calcium element (12.26%) are the most amounts of compounds in the Shahr-i Sokhta lapis lazuli structures. The identified chemical compositions of the lapis lazuli in Shahr-i Sokhta are a high amount of calcium and a low amount of iron, which indicates the lapis lazuli structure of this site has a high calcium impurity and low pyrite impurity; this issue could be confirmed through petrography studies. Finally, this analysis represents the correct recognition of the composition and type of used stones in manufacturing ornament objects of Shahr-i Sokhta.
The element percentage of obtained spectra is clearly determined, indicating the main composition of lapis lazuli. The elements represent the chemical structure of a lapis lazuli, a lazulite mineral type with a high calcite impurity percentage. In addition, this study examines the three pieces of lapis lazuli samples through Raman spectroscopy; two samples represent almost similar peaks in the range of 546 cm-1 and 1092 cm-1, and only one sample shows a peak in the range of 546 cm-1. The investigations represent that based on the lapis lazuli studies using the Raman, the lapis lazuli in the mentioned ranges shows an almost significant peak. The number of elements and obtained spectra in these two spectra are almost similar.
Acknowledgments
This work has been supported by the “Investigation and study of Shahr-i Sokhta semi-precious stones” project funded by the Research Center for Conservation of Cultural Relics (RCCCR). The authors are thankful to Center for Conservation of Cultural Relics. The authors want to National Museum of Iran, Southeast Regional Museum of Zahedan, and Shahr-i Sokhta World Heritage Site for their supporting.