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Archaeometric Investigation of Roman Glass Finds from Bulgaria Introduction Experimental Berliner Beiträge zur Archäometrie Seite 183-198 1999 Archaeometric investigation of roman glass finds from Bulgaria I. KULEFF, R. DJINGOVA Faculty of Chemistry, University of Sofia 1126-Sofia, B ulgaria Introduction Glass finds discovered in the European part of the Roman Empaire are usually referred to as Romanglasses while the glass from the Near East and Egypt is considered separately although it has been produced in the same period of time. One of the reasons for this classification isthat glass production in Egypt and the Near East has had a long tradition while the knowledge of glassmaking has been introduced in the Roman Empire from Mesopotamia and Egypt and is considered as new for the territories of Italy and the Eastern provinces. The territory of present Bulgaria belongs to these regions. The Iack of enough chemico-thechnological investigations of Roman glass excavated in Italy was recognized in the Iiterature in the early 80-ies (e.g. Goffer, 1980) and it was recently compensated by the investigations carred out by Casoli&Mirti (1992) and Verita&Toninaga (1990). This Iack is stillmorevalid for the glass, excavated on Bulgarian territory where only a sporadic information exists which does not provide an answer to the questions concerning the technology of glassmaking. It is worth mentioning that the finds from that period are numerous (see e.g. Kabakhcieva, 1987; 1996; 1997; 1997a; Mincev, 1986; 1988; 1989; 1990; 1992) and there are direct evidences for glass production in Bulgaria in the period 1' '- S'h century AD (Kabakhcieva, 1987; 1996; 1997; 1997a;). Therefore the aim ofthe present study is to investigate glass finds from the Romanperiod in Bulgaria using Instrumental Neu­ tron Activation Analysis (INAA). The method for analysis is described in Kuleff et al., (1984; 1988) and Kuleff&Djingova (1990). Thus data for the chemical composition of glasses from the Romanperiod in Bulgaria will be obtained for the firsttime and the results might be used for initial conclusions about the technology of glass production. Experimental 1. Material. Twenty six glass finds, referred to the Roman period, were subjected to analysis. Nine from the finds were excavated in the glass-workshop in the Roman town Oescus (the workshop is dated to the firsthalf of yct- firsthalf of 4'h century AD). Three of them represent glass from glassmelting tubs excavated in the workshop. The I 0 finds from Varna and the 5 finds from the Romanvilla Arrnira belong to the 2"ct - 4'h century AD, while the two finds from Kaliakra are dated to the 4'h- 6'h century AD. A short description of the finds is given in Table 1 and the investigated sites are presented in Fig.1. 183 a- 0 E s c U s b- V A R N A c-KALIAKRA d-ARMIRA Fig. 1: Map of Bulgaria showing the iocation of the samfing piaces. 2. Method of analysis. To remove surface contamination the g1ass sampies are carefully washed with tap water, detergent and brush and rinsed with deionized water. Thus the thin iridescent weathering iayer (if present) is removed. The samples are piaced between poiyetheiene plates, crushed and homogenized in an agate mortar. INAA (Kuieff et al., 1984; 1988; Kuieff&Djingova, 1990) and energy dispersive X-ray tluorecsence analysis (ED XRFA) have been used for the analysis ofthe investigated giass finds. INAA was used to determine the content of Al, As, Ba, Ca, Ce, Cl, Co, Cr, Cs, Cu, Dy, Eu, Fe, Hf, La, Mg, Mn, Na, Rb, Sb, Sc, Sm, Ta, Th, Ti, V, and Yb in the sampies after two irradiations with piie and one with epithermal neutrons and six measurements (twice after each irradiation) (Kuleff et al., 1984; Kuleff&Djingova, 1990). The gamma-spectra were measured with a HP Ge detector (energy resolution 1.9 keV and efficiency 15 % for i332.5 keY gamma line of 6°Co) connected to a 4096 channei pulse height anaiyser (Canbena 35 +). ED XRFA was used for determination of the content of Iead and sodium in some of the investigated samples. Excitation was done by X-rays produced by a tube: voltage 30 kV; current 0.15 mA, Ag anode and filter rhodium. The obtained anaiytical data (Tabie 2) were subjected to duster analysis using the program package of Brookhaven National Labaratory (Sayre, 1988). The fo ii owing subprograms were used: - CONDIST = for caiculation of distance coefficient matrix using squared mean Eudedean distance; -AGCLUS = for aggregative hierarchical dustering using " nature's group" as dustering method. The duster size is defined as the mean of the distances between all pairs of points within the duster, notjust pairs of distinct items, i.e. the "diagonal" entities ofthe di ss imiiarities matrix are induded in the mean and the size is multiplied by the number of specimens within the duster. Clustering proceeds by joining in sequence those dusters for which the new duster would have a minimum net increase in size over the combined sizes to the clusters tobe merged. 184 Table 1: Description ofthe investigated glass samples. Lab.code Description Colour Date Excavation c. AD site 52 .0ES Fragment, disc form, thick folded rim deep green IV-VI Oescus 53.0ES Glass from glassmelting tub green 111-IV Oescus 54 .0ES Fragment of bracelet colourless slight yellow 11-IV Oescus 56.0ES Fragment of window glass colourless slight yellow 111-IV Oescus 57.0ES Fragment of vessel (cup ?) colourless slight yellow 111-IV Oescus 58 .0ES Fragment of window glass colourless 111-IV Oescus 59.0ES Fragment of window glass colourless slight green 111-IV Oescus 60.0ES Glass from glassmelting tub colourless slight yellow 11-IV Oescus 61.0ES Glass from glassmelting tub slight blue-greenish 11-IV Oescus 62.VAR Fragment of unguentarium colourless 11-111 Varna in the form of a bell 63.VAR Fragment of vessel (cup ?) colourless 11-111 Varna 64.VAR Fragment of unguentarium green 1-11 Varna 65.VAR Fragment of unguentarium colourless slight yellow 11-111 nearVarna 66.VAR Fragment of bottle-flask colourless slight yellow 111-IV Varna 67.VAR Fragment of unguentarium colourless III Varna 68.VAR Fragment of unguentarium colourless III Varna in the form of a ball 69.VAR Fragment of jug (ionohoe) colourless slight greenish III Varna 70.VAR Fragment of unguentarium colourless IV-VI Varna 71.VAR Fragment of unguentarium colourless 11-111 Varna in the form of a bell 72 .KAL Fragment of wheel beaker slight greenish IV-VI Kaliakra 73 .KAL Fragment of window glass slight yellowish IV-VI Kaliakra 74.ARM Fragment of window glass colourless slight yellowish 11-IV Armira 75 .ARM Fragment of window glass colourless slight yellowish 11 -IV Armira 76.ARM Fragment of window glass colourless 11-IV Armira 77.ARM Fragment of window glass colourless blueish 11-IV Armira 78.ARM Fragment of the botom of bottle colourless greenish 11-IV Armira 185 Table 2: Concentration of determined elements (Jlg/g) in investigated samples of Roman glasses Element 52.0ES 53.0ES 54.0ES 56.0ES 57 .0ES Al 203 (%) 2.61 ±0.08 2.15±0.25 2.06±0.34 2.31 ±0.06 2.32±0.08 As 242±5 <4 14±2 5±1 <4 Ba 67±3 660±50 417±40 390±80 240±180 Br 9.3±1 .9 1.9±0.5 2.4±0.4 2.1 ±0.3 3.9±0.8 CaO (%) 5.81 ±0.32 7.22±0.84 6.41 ±0.50 8.27±0.50 7.56±0.75 Ce 16.6±1 .6 15.5±1 .6 95.0±1.5 11 .6±1.1 13.2±1.7 Cl(%) 0.87±0.09 1.93±0.23 0.20±0.19 2.60±0.45 2.51 ±0.43 Co 11 .5±1 .8 4.0±0.5 16.6±0.8 3.0±0.5 6.0±0.3 Cr 16±5 19±3 81 ±4 11 ±4 12±3 Cs 0.26±0.06 < 0.1 0.70±0.09 0.25±0.09 0.55±0.08 Cu 6410±520 130±20 330±50 220±30 215±30 Dy <3 4.0±1.0 3.0±1 .0 2.0±1 .5 2.3± 1.1 Eu 0.13±0.02 0.66±0.08 1.43±0.18 0.58±0.06 0.46±0.09 Fe 203 (%) 0.99±0.03 0.59±0.03 5.58±0.13 0.41 ±0.03 0.46±0.03 Hf 2.1±0.2 1.3±0.2 5.9±0.2 1.3±0.1 1.3±0.2 K20 (%) 0.9±0.1 0.8±0.1 0.9±0.1 0.5±0.1 0.9±0.1 La 13.8±1.5 8.7±0.4 41 .3±1.9 6.2±0.6 5.9±0.6 Lu 0.11 ±0.03 0.46±0.04 0.23±0.04 0.08±0.02 Mgü (%) 0.44±0.03 0.52±0.03 1.93±0.03 0.79±0.03 0.54±0.03 Mn 2730±40 1480±140 11520±440 2160±30 4250±130 Na20 (%) 23.6±0.5 21 .5±0.3 21 .5±0.4 22.6±0.3 21 .6±0.8 Nd 7±2 4±1 41 ±2 30±2 34±3 Rb < 20 45±6 125±9 18±4 35±5 Sb 122±8 2500±40 3.2±0.1 2960±50 2000±30 Sc 1.7±0.3 1.5±0.1 15.0±0.5 1.1 ±0.1 1.2±0.1 Sm 2.1 ±0.1 1.5±0.1 8.3±0.2 1.2±0.2 1.3±0.1 Ta 0.11±0.03 0.11±0.03 0.09±0.04 1.10±0.08 1.14±0.09 Th 1.6±0.1 1.4±0.3 14.4±0.4 0.6±0.2 0.5±0.2 Ti 840±120 660±140 4020±420 480± 160 410±160 V 26 .1 ±4.6 15 .2±1.7 120±5 13.6±2.9 25 .1±1.4 Yb 0.9±0.1 0.6±0.1 3.3±0.2 < 0.6 <0.5 186 Table 2: (continuation) Element 58 .0ES 59.0ES 60 .0ES 61.0ES 62.VAR Al 203 (%) 2.02±0.17 2.15±0.06 2.26±0.11 2.31 ±0.06 1.93±0.06 As <4 <4 <3 <3 <6 Ba 350±40 640±50 280±90 480± 70 760±60 Br 1.7±0.6 3.3±0.5 3.3 ±0.6 3.8±0.5 1.5 ±0.5 CaO (%) 7.48±0.55 7.36±0.53 7.52±0.54 7.98±0.54 5.73±0.36 Ce 10.5±1 .1 13.3±0.7 14.7±0.5 16.0±0.6 5.3±1 .3 Cl(%) 1.83±0.38 2.39±0.40 2.63±0.44 2.47±0.42 2.80±0.19 Co 2.2±0.5 4.2±0.1 5.4±0.2 4.8±0.2 2.2±0.3 Cr 8±1 9±1 13±1 12±1 14±1 Cs 0.25±0.08 0.52±0.05 0.86±0.07 0.91 ±0.09 0.53±0.07 Cu 162±45 150±50 200± 70 200±60 400±90 Dy 2.3±0.4 2.3±0.4 2.0±0.4 1.9±0.4 2.0±0.4 Eu 0.57±0.05 0.50±0.06 0.82±0.12 0.93±0.12 0.59±0.09 Fe203 (%) 0.36±0.04 0.50±0.03 0.44±0.04 0.49±0.03 0.23±0.02 Hf 1.6±0.1 0.9±0.3 1.6±0.2 1.7±0.2 1.4±0.2 K20 (%) 0.6±0.1 0.7±0.1 0.6±0.1 0.5±0.1 <0.5 La 6.6±0.4 6.0±0.6 6.9±0.5 4.4±0.4 6.4±0.4 Lu 0.11±0.04 0.45±0.05 0.23±0.04 0.08±0.02 MgO (%) 0.41 ±0.03 0.58±0.02 0.53±0.03 0.44±0.06 0.36±0.02 Mn 174±20 1950±50 2020±40 2080±40 105±20 Na20 (%) 22 .9±0.4 21.6±0.8 22.2±0.5 21 .3±0.8 23 .7±0.9 Nd 10±2 9±1 12±1 6±2 8±1 Rb 70±8 <5 33±5 12±1 40±5 Sb 4420±50 2470± 70 3110±90 2400±80 5300±80 Sc 1.0±0.1 1.2±0.1 1.2±0.1 1.2±0.1 0.6±0.1 Sm 1.3±0.1 1.1 ±0.1 1.4±0.2 0.7±0.1 1.2±0.1 Ta 0.07±0.01 <0.04 0.14±0.01 0.25±0.03 <0.05
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