Journal of Radioanalytical and Nuclear Chemistry

https://doi.org/10.1007/s10967-018-5863-8(0123456789().,-volV)(0123456789().,-volV)

Chemical characterization of large size archaeological clay bricks

for grouping study by internal mono-standard neutron activation
analysis
K. B. Dasari1,3 • R. Acharya2 • N. Lakshmana Das1

Received: 31 October 2017

Ó Akadémiai Kiadó, Budapest, Hungary 2018

Abstract
The k0-based internal mono-standard neutron activation analysis (IM-NAA) method was used to analyze large size
archaeological clay brick samples for grouping study. Elemental concentration ratios with respect to Sc were derived using
IM-NAA in conjunction with in situ relative detection efficiency. Preliminary grouping was carried out using bi-plot of Ce/
Sc and La/Sc ratios and the grouping was confirmed by statistical cluster analysis. Concentration results of a large size
sample were compared with analysis of small size replicates by both relative NAA and IM-NAA methods. The method
adopted here is a standard-less one for grouping combined with provenance study of archaeological artifacts.

Keywords Ancient clay bricks  IM-NAA  Concentration ratio  Non-standard geometry  Lanthanides  Grouping study

Introduction and monuments using modern technology [3–5]. Archae-

ological scientists and conservators are frequently con-
Buddhism was established in India during the 5th century cerned with the questions of the location, time, and method
BCE to 12th century CE. Buddhist stupas were built using of preparation of artifacts. These queries might be solved
burnt clay bricks by King Asoka (368–232 BCE) to honor with provenance study of archaeological artifacts using
the life of Lord Buddha (564–484 BCE). Stupa complexes chemical composition analysis [6, 7]. Provenance study is
of antiquity are the largest brick structures in the world used to identify whether the artifacts under investigation
[1, 2]. These ancient stupas and monuments are in ruins belong to the same or different origin, thus assisting in
due to changes in aerial, terrestrial, and under-water finding their specific sources.
weathering. Stupas and other archaeological remains are Favorable characteristics including physiochemical
important for the history and economy of cultural heritage. properties of ancient and modern materials are required to
Archaeologists and analytical scientists, and engineers forecast the composition of similar materials to be restored
have been increasingly interested in the replication and with substitution materials. Many scientific studies focused
restoration of the architectural heritage of ancient stupas on the physical, chemical and mechanical properties of
clay ceramics are used in architecture [7, 8]. Clay ceramics
such as potteries and bricks are frequently studied to obtain
& K. B. Dasari information on the sources from which they were prepared.
dkishore4u@gmail.com Chemical characterization of clay ceramics is a suit-
& R. Acharya able method for grouping or provenance studies using trace
racharya@barc.gov.in elements such as transition and/or rare earth elements. The
1 trace elemental concentration determination of clay
GITAM Institute of Science, GITAM University,
Visakhapatnam 530 045, India ceramics is a more suitable approach for provenance study
2 since they are strongly correlated to source clay compared
Radiochemistry Division, Bhabha Atomic Research Centre,
Trombay, Mumbai 400 085, India to major elements. These elemental concentration data are
3 statistically analyzed to find groups based on the similar
Present Address: Korea Research Institute of Standards and
Science, Daejeon 34113, Republic of Korea composition of artifacts [7, 9, 10]. The chemical analysis of

123

clay ceramics through a non-destructive analytical method
is preferred over a wet-chemical method. Analysis using
conventional radioanalytical techniques including X-ray
fluorescence [11], ion beam analysis [12], and neutron
activation analysis (NAA) are conducted using a small
sample size and similar/identical matrix matched standard
[9, 10]. Other non-destructive analytical techniques are
also applied to find the physical and chemical properties of
archaeological objects to achieve better restoration and
conservation [13]. In our previous work, numerous ancient
potteries and brick samples were analyzed using relative
and k0-based INAA methods for provenance studies
[10, 14, 15]. In our work, routinely used small size samples
are in the mass rage of 100–250 mg, whereas sample mass
above 10 g has been considered as large size sample. Large
size sample analysis is feasible in NAA because of high
penetration powers of neutrons and gamma rays. Compared
with the analysis of a small size sample (100 mg), the
analysis of a large sample is advantageous for enhanced
analytical representativeness of results. In the present
work, we adopted the k0-based internal mono-standard
NAA (IM-NAA) method to analyze the clay brick samples.
However, this method encounters problems of neutron self-
shielding and gamma-ray self-attenuation [16, 17]. These
problems can be easily addressed through the IM-NAA
method using in situ detection efficiency [18–21]. The IM-
NAA method was developed at Radiochemistry Division,
Bhabha Atomic Research Center (BARC), Mumbai for
large and small sample analyses by using reactor neutrons
and applied to various matrices of wheat, coal, and nuclear
material samples [14, 20–22]. Our laboratory participated
in the International Atomic Energy Agency (IAEA) coor-
dinated research project (CRP) for inter comparison exer-
cise of non-standard geometry size pottery replica analysis
using IM-NAA [21]. This method is simpler than the
conventional k0-based NAA method and provides ele-
mental concentration ratio with respect to one of the ele-
ments present in the sample called internal mono-standard.
A priori knowledge of the concentrations of the internal
mono-standard is required to convert relative to absolute
concentration [19]. In the present work, the IM-NAA
method using in situ relative detection efficiency was
applied to large and non-standard geometry clay brick
samples for their chemical composition in order to arrive at
the grouping or provenance through elemental concentra-
tion ratios with respect to Sc as the internal mono-standard.
Experimental
Ancient clay brick samples (4th BCE to 3rd CE) were
collected in India from historical Buddhist stupas. Four
samples were from Hyderabad region (Samples: 1–4) and
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Journal of Radioanalytical and Nuclear Chemistry
14 were from Visakhapatnam regions (Samples: 5–18) of
India. In our previous study, clay brick samples from
Visakhapatnam region were analyzed by relative INAA
method [10]. Sample collection locations are illustrated in
Fig. 1. Samples were analyzed directly without any
chemical treatment and destruction. For homogeneity study
as well as to compare the large size sample results obtained
by IM-NAA of one sample, three replicate small size
samples were analyzed by both relative INAA and IM-
NAA methods. Samples were dried at 100 °C in a hot air
oven for approximately 24 h to remove moisture content.
Based upon previous studies on large clay ceramics sam-
ples, the representative sample size has been found to be
1 g and above [14]. However to get higher counts (or lower
counting statistical error) in the peak of interest of corre-
sponding gamma-ray, about 10 g of sample is better choice
to be analyzed using relatively lower neutron flux
(107 cm-2 s-1). Thus large size samples (11–60 g) were
chosen and doubly sealed in polyethylene for irradiation.
Samples were irradiated for 4 h with highly thermalized
(99.97%) reactor neutrons with neutron flux of approxi-
mately 107 cm-2 s-1 at the graphite reflector position of
Advanced Heavy Water Reactor (AHWR) Critical Facility
(CF), BARC, Mumbai. Samples were transferred to the
laboratory after a cooling time of 2 h and then mounted on
standard Perspex plates for radioactive assay. In the present
method counting geometry/distance with respect to the
detector was flexible because this method uses in situ rel-
ative detection efficiency of each sample for calculating
elemental concentrations. Gamma ray measurement was
performed using a 40% relative efficiency HPGe detector
Fig. 1 Map of the sample collection sites and typical brick samples
Journal of Radioanalytical and Nuclear Chemistry

coupled to 4k multi-channel analyzer (MCA). The mx ðS  D  CÞy Np;x ey k0;Au ðyÞ

gamma-ray spectra were analyzed using peak-fit pulse ¼    ð1Þ
my ðS  D  CÞx Np;y ex k0;Au ðxÞ
height analysis software (PHAST) developed at BARC.
Each sample was counted at least twice, taking into where m, S, D, C, Np, ec and k0,Au are absolute elemental
consideration the half-lives of the activation products. In- concentration, saturation factor, decay factor, counting
situ relative detection efficiency was obtained from c-rays factor used for correcting the decay during the counting
of four activation products, namely 152mEu, 140La, 56Mn period, net peak area under the gamma ray peak of interest,
and 24Na covering a wide energy range of 122–2754 keV. absolute peak detection efficiency and literature k0,Au–
The in situ relative detection efficiency takes care of c-ray factors, respectively, for analyte (x) and internal mono-
self-attenuation and geometrical effects, thus making the standard Sc (y). Relevant nuclear data and literature k0,Au
method geometry independent. Figure 2 shows the rela- factors are given in Table 1 [23, 24]. The sub-cadmium to
tive detection efficiency curves obtained from two shapes epithermal neutron flux ratios (f) of their radiation position
and sizes of clay ceramic samples with varying masses was 860 ± 31 and this value was obtained from the cad-
(11 and 53 g). The IM-NAA method generates elemental mium ratio method using gold foil. The uncertainty on
concentration ratios with respect to internal mono-stan- f value was arrived from standard deviation of five replicate
dard (IM) [19, 20]. In the present study, Sc was selected analyses [14, 21]. The IM-NAA method has been validated
as an internal mono-standard geometry because of its using IAEA reference materials, small sample replicate
favorable geochemical properties and nuclear data [14]. It study, and comparison with other analytical methods pre-
is not enriched or depleted during weathering and firing sented in the literature [19–22]. Further details on in situ
process while making the bricks from raw clay. Elemental relative detection efficiency and elemental concentration
concentration ratios with respect to Sc of large size ratio calculation for small size samples are described in our
samples were calculated using the IM-NAA method using previous studies [19–21].
in situ relative detection efficiency according to simplified
Eq. 1 [19, 20].
Results and discussion

The concentration ratios of fifteen elements: Na, K, Cr,

Mn, Fe, Co, Zn, As, Cs, La, Ce, Eu, Lu, Hf, and Th with
(b) respect to Sc were calculated in all eighteen large size
1.4E-3 152m 140 56 24
Nuclides used : Eu, La, Mn, Na ancient clay bricks. Such elemental concentration ratios
obtained in two representatives clay brick samples (one
1.2E-3 (a) - 11 g each from Visakhapatnam and Hyderabad regions) are
(b) - 53 g given in Table 2. The combined uncertainties reported on
Insitu relative detection efficiency

the elemental concentration ratios determined at ± 1r

1.0E-3 confidence limit were in the range of 3.0–9.1%. The
combined uncertainties were calculated using error propa-
gation formula of individual uncertainty parameters (as per
8.0E-4 the Eq. 1) of counting statistics along with peak fitting
errors (0.8–8.6%), uncertainties on k0,Au (0.4–2.0%), and ec
(1.6–3.4%) of analyte and internal mono-standard Sc.
6.0E-4
For comparison of large size sample results as well as
homogeneity testing, one representative clay ceramic
4.0E-4
(a) sample was analyzed by IM-NAA and three small size
(100 mg each) samples and relative INAA using small size
samples (N = 3). The concentration ratios of elements Cr,
2.0E-4 Fe, Co, Cs, La, Ce, Zn, Eu, Lu, Hf, and Th with respect to
Sc were selected for comparison and the results are given
in Table 3. Relative and IM-NAA methods are suitable for
0.0 the analysis of small size samples with good precision and
0 500 1000 1500 2000 2500 accuracy. In the relative method, absolute concentrations
Energy (kev) were converted to ratios by dividing the Sc concentration.
Fig. 2 Relative in situ detection efficiency of two irregular clay
The elemental concentration ratios along with combined
ceramic samples uncertainty or % relative standard deviations (% RSD)

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 Journal of Radioanalytical and Nuclear Chemistry

Table 1 Nuclear data used for k0-based IM-NAA method calculations [23, 24]
Target element Nuclear reaction Product half life Main c-ray energies, keV (intensity, %) k0,Au (s, %)
23
Na Na(n, c)24Na 14.997 h 1368.63 (99.99), 2754.01 (99.86) 4.68E-02 (0.6), 4.62E-02 (0.9)
41
K K(n, c)42K 12.355 h 1524.6 (18.08) 9.46E-04 (0.6)
45
Sc Sc(n, c)46Sc 83.79 days 889.28 (99.98), 1120.54 (99.99) 1.22E?00 (0.4), 1.22E?00 (1.1)
50
Cr Cr(n, c)51Cr 27.704 days 320.08 (9.91) 2.62E-03 (0.5)
55
Mn Mn(n, c)56Mn 2.5789 h 846.76 (98.85), 1810.73 (26.9) 4.96E-01 (0.6), 1.35E-01 (0.4)
58
Fe Fe(n, c)59Fe 44.495 days 1099.24 (56.5), 1291.59 (43.2) 7.77E-05 (0.5), 5.93E-05 (0.4)
59
Co Co(n, c)60Co 1925.28 days 1173.23 (99.85), 1332.49 (99.98) 1.32E?00 (0.4), 1.32E?00 (0.5)
64
Zn Zn(n, c)65Zn 243.93 days 1115.54 (50.04) 5.72E-03 (0.4)
75
As As(n, c)76As 1.0942 days 559.10 (45.0) 4.83E-02 (1.6)
133 134
Cs Cs(n, c) Cs 2.0652 years 604.72 (97.62), 795.86 (85.46) 4.76E-01 (2.0), 4.15E-01 (2.0)
139
La La(n, c)140La 1.679 days 487.02 (45.5), 1596.21 (95.40) 6.37E-02 (0.9), 1.34E-01 (1.1)
140
Ce Ce(n, c)141Ce 32.511 days 145.44 (48.40) 3.66E-03 (0.9)
151
Eu Eu(n, c)152Eu 13.517 years 344.28 (26.59), 1408.01 (20.87) 1.19E?01 (0.9), 9.36E?00 (0.6)
176
Lu Lu(n, c)177Lu 6.647 days 208.36 (10.36) 7.14E-02
180
Hf Hf(n, c)181Hf 42.39 days 133.02 (43.3) 2.37E-02 (0.6)
232
Th Th(n, c)233Pa 26.975 days 311.90 (38.5) 2.52E-02 (0.5)

Table 2 Results of two representative brick samples of Visakhapat- size samples by IM-NAA, the uncertainties on concentra-
nam and Hyderabad regions by IM-NAA using Sc as internal mono- tion ratios were evaluated from the standard deviation of
standard replicate (N = 3) analyses and the % RSD are in the range
Element ratio x/Sc Ancient brick samples of 2.4–5.0%. In the case of relative INAA, the percentage
Visakhapatnam Hyderabad
combined uncertainties on elemental concentration ratios
with respect to Sc are in the range of 3.9–6.2% and these
Na 119 ± 4 1062 ± 35 values have been arrived from propagation of % RSD
K 1255 ± 42 2182 ± 100 values of replicate analyses and uncertainty on Sc con-
Cr 6.27 ± 0.21 3.62 ± 0.15 centration (3.2% at k = 1). The concentration ratios with
Mn 45.4 ± 2.6 40.3 ± 2.0 respect to Sc of the clay ceramic sample analyzed through
Fe 2943 ± 122 1776 ± 73 the three methods were found to be in good agreement
Co 1.37 ± 0.07 0.8 ± 0.02 (Table 3). The IM-NAA method does not require any
Zn 4.59 ± 0.34 2.84 ± 0.19 external or internal standards for obtaining elemental
As 0.18 ± 0.02 0.26 ± 0.02 concentration ratio. The analysis is more advantageous in
Cs 0.14 ± 0.01 0.15 ± 0.01 large size samples than in small samples by IM-NAA,
La 2.94 ± 0.09 3.83 ± 0.12 because uncertainties due to f, a and Q0 are not included to
Ce 6.21 ± 0.24 6.61 ± 0.23 the combined uncertainty.
Eu 0.071 ± 0.006 0.086 ± 0.007 The elemental concentration ratios (Table 2), including
Lu 0.034 ± 0.002 0.026 ± 0.002 La/Ce ratios, in both locations were found different. The
Hf 0.42 ± 0.01 1.07 ± 0.04 results showed that the origin of samples might be differ-
Th 0.82 ± 0.03 1.79 ± 0.06 ent. Further grouping confirmation was done through Ce/Sc
La/Ce 0.47 0.57 vs. La/Sc bi-plot and multivariate statistical cluster analysis
(CA) programs [26]. The preliminary grouping study was
performed based on bi-plot of Ce/Sc versus La/Sc con-
centration ratio values. La and Ce were selected because of
values are given in Table 3. IAEA RM SL-1 (sediment their similar geochemical properties. These results of the
matrix) was used as the comparator for mass fraction preliminary grouping of clay brick samples resulted in
determination in relative method of INAA [25]. The three broad grouping as demonstrated in Fig. 3. Samples of
uncertainty values for large size sample were obtained in bricks from the Hyderabad region fell in one group: Group
similar way to that given in Table 2 and the combined I (Samples 1-4), and samples from the Visakhapatnam
uncertainty values are in the range of 3.1–8.9%. For small region fell two groups: Groups II (Samples 5–13) and III

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Journal of Radioanalytical and Nuclear Chemistry

Table 3 Results of one representative brick sample analyzed by relative INAA and IM-NAA methods
Element (x/Sc) Small size sample by relative NAA (N = 3) Small size sample by IM-NAA (N = 3) Large size sample by IM-NAA

Cr 5.55 ± 0.35 5.72 ± 0.19 5.68 ± 0.27

Fe 3088 ± 191 2966 ± 76 3055 ± 96
Co 0.55 ± 0.03 0.54 ± 0.01 0.50 ± 0.02
Zn 4.38 ± 0.27 4.47 ± 0.22 3.91 ± 0.25
Cs 0.21 ± 0.01 0.200 ± 0.007 0.20 ± 0.01
La 2.91 ± 0.17 2.77 ± 0.07 2.90 ± 0.15
Ce 6.77 ± 0.41 6.79 ± 0.19 6.58 ± 0.40
Eu 0.112 ± 0.004 0.115 ± 0.003 0.106 ± 0.005
Lu 0.059 ± 0.003 0.060 ± 0.002 0.060 ± 0.003
Hf 0.53 ± 0.02 0.60 ± 0.02 0.40 ± 0.04
Th 1.35 ± 0.08 1.40 ± 0.05 1.37 ± 0.06

major and minor elements [7, 9]. The elemental concen-

7.0
trations of Na, K and As were not used for grouping study
6.8 [7, 14]. Among the determined elemental concentration
ratios, eleven selected trace elements, namely, Cr, Mn, Co,
6.6
G-I Zn, Cs, La, Ce, Eu, Hf, and Th along with major element
6.4 Fe were used for grouping analysis. The dendrogram of
brick samples obtained by CA is illustrated in Fig. 4. The
Ce/Sc

6.2 statistical cluster analysis dendrogram suggested that

6.0
G-III
5.8
G-II
5.6
5.4
1.6 2.0 2.4 2.8 3.2 3.6
La/Sc
Fig. 3 Biplot of Ce/Sc versus La/Sc for preliminary grouping
(Samples 14–18) without any outliers. The outliers repre-
sent the foreign or imported artifacts from other sources
whose chemical composition data are different than the
similar group of artifacts collected from a particular
location.
Statistical cluster analysis (CA) was used to confirm the
preliminary grouping study. The use of statistical treatment
through multivariate techniques is to divide the artifacts
into groups with similar compositional data obtained using
IM-NAA. Ward’s method of CA using square-mean
Euclidean distance procedure was used to obtain the sim-
ilarity or dissimilarity among the archaeological artifacts,
and it is a sensitive method to identify the outliers [26, 27].
Euclidean distance gives clues to identify the groups of the
samples. Cluster analysis using concentration ratios of
eleven selected elements with respect to Sc was conducted
using WINSAT Excel software. The elemental concentra-
tions at trace levels provide more reliable clues than at
samples fell into three broad groups, namely, Hyderabad
region Group I (Samples 1–4), and Visakhapatnam region
Groups II (Samples 5–13) and III (Samples 14–18) which
coincide well with the preliminary grouping study. The
data were tested using single linkage method of CA which
also confirmed the same groups. Group II has high Eucli-
4.0 4.4
dean distance compared to other two groups. The group II
samples source might be mixed with two or more locally
produced clay. These all three groups agreed well with the
collection history provided by the archaeologists. Thus, we
conclude that the sample sources originated from three
specific places. In our previous work on the same small
clay brick samples (57 samples), the samples from the
Visakhapatnam region were classified into two major
groups [10]. In the present work, the 14 samples (Samples
5–18) indicated two different source locations. The con-
centration ratios, instead of absolute concentrations, could
be helpful in grouping the artifacts, thereby making the
method standard-less and simple.
Conclusions
The analysis of large samples analysis through the IM-
NAA method provides reliable results like that of replicate
small sample analyses. The present work demonstrated that
the elemental concentration ratios, instead of absolute
concentrations, are useful for grouping study. The grouping

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Fig. 4 Dendrogram of brick
samples obtained by cluster
analysis using concentration
ratios of eleven selected
elements
study using concentration ratios of large size sample agreed
well with the collection history and exhibited favorable
correlation with small size sample analysis by relative
NAA method. Results indicated that one large size repre-
sentative sample analysis is sufficient compared to many
replicate small size sample analyses. Cluster analysis using
elemental concentration ratios of eleven elements con-
firmed the preliminary grouping arrived by Ce/Sc vs. La/Sc
values. Analysis of such ceramic sample with non-standard
geometries by IM-NAA along with in situ detection effi-
ciency is a very powerful approach for grouping combined
with provenance study.
Acknowledgements Authors from GITAM University thank Dr. P.K.
Pujari, Head, Radiochemistry Division, BARC for the support and
encouragement. Authors thankfully acknowledge University Grants
Commission-Department of Atomic Energy Council of Scientific
Research (UGC-DAE CSR), Mumbai Centre for the project and
financial assistance and Dr. P. Gayatri, Ex. Director, Department of
Archaeology and Museum, united Andhra Pradesh, Hyderabad for
providing authentic samples. Authors thank nuclear reactor crew
members of the AHWR CF and Dhruva reactor, BARC, Mumbai for
their help during sample irradiation.
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