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Assessment of natural radioactivity and associated radiation indices in soil

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Nadu, India

Article · January 2017

DOI: 10.4103/rpe.RPE_31_16

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Original Article

Assessment of natural radioactivity and associated radiation

indices in soil samples from the high background radiation
area, Kanyakumari district, Tamil Nadu, India
A. K. Ajithra, B. Venkatraman1, M. T. Jose2, S. Chandrasekar3, G. Shanthi
Department of Physics and Research Centre, Women’s Christian College, Nagercoil, 1Radiological Safety Division,
Indira Gandhi Centre for Atomic Research, 2Radiological Safety Section, Indira Gandhi Centre for Atomic Research,
3
Indira Gandhi Centre for Atomic Research, Kalpakkam, Tamil Nadu, India

Abstract Assessment of natural radioactivity is very important from different points of view, especially for assessment of
radiation exposure to human. In the present study, natural radionuclide concentrations of 238U, 232Th, and 40K
were measured by gamma spectrometry using HPGe detector in soil samples collected from Southwest coast
of Kanyakumari district, Tamil Nadu. The radiological index parameters due to natural radionuclides such as
radium equivalent activity, absorbed dose rate, annual effective dose rate, external hazard index, internal hazard
index, and gamma index were calculated for the soil samples. All the calculated radiological index values are
higher than world average values and the recommended safety limits. Multivariate statistical techniques such
as Pearson correlation, principal component analysis, and cluster analysis were applied to know the relation
between radionuclides and radiological parameters and to study the spatial distribution of radionuclides.

Keywords: Gamma ray spectrometry, multivariate statistical techniques, natural radioactivity, soil

Address for correspondence: Prof. A. K. Ajithra, Department of Physics and Research Centre, Women’s Christian College, Nagercoil, Tamil Nadu, India.
E‑mail: ajithra.ak@gmail.com
Submission: 15-May-16 Revision: 11-Dec-16 Accepted: 20-Jan-17

INTRODUCTION reactors, and discharges of radioactive waste from the

Natural occurring radionuclides, also called terrestrial
or primordial radionuclides, are present in varying
amounts in the earth’s crust (soil sand rocks). Terrestrial
radionuclides includes the decay radionuclides in the series
of uranium (238U) and thorium (232Th) and a nonseries
decay natural radionuclides such as 40K, 87Rb, 138La, 147Sm,
and 176Lu. The main contribution to external exposure
in outdoor is from gamma radiation emitted by these
terrestrial radionuclides mainly 238U and 232Th series and
40
K.[1] Artificial radionuclides can also be present from the
testing of nuclear weapons and the accidents at nuclear
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nuclear installations.
There are few regions in the world known to be high
background radiation areas due to local geology and geo
chemical effects that cause enhanced levels of terrestrial
radiation.[2] In the high background areas of the countries
such as Austria, Brazil, China, France, India, and Iran, the
radiation levels were found to be high varying over an order
of magnitude depending on the site‑specific terrestrial
radioactivity.[3] In India, there are quite a few monazite sand
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How to cite this article: Ajithra AK, Venkatraman B, Jose MT, Chandrasekar S,
DOI: Shanthi G. Assessment of natural radioactivity and associated radiation
10.4103/rpe.RPE_31_16 indices in soil samples from the high background radiation area, Kanyakumari
district, Tamil Nadu, India. Radiat Prot Environ 2017;40:27-33.

© 2017 Radiation Protection and Environment | Published by Wolters Kluwer - Medknow 27

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Ajithra, et al.: Assessment of natural radioactivity and associated radiation indices in soil samples
bearing placer deposits causing high background radiation
along its long coastal line. Ullal in Karnataka, Kalpakkam in
Tamil Nadu, coastal parts of Tamil Nadu and Kerala state
and Southwestern coast of India are known to be high back
ground radiation areas.[4] Coastal region of Kanyakumari
district, Tamil Nadu was one of the areas in the Southwest
coast where high radiation level has been reported. Beach
sand in these areas contains heavy minerals such as ilmenite,
rutile, zircon, monazite, and sillimanite. 232Th and 238U are
reported from these regions, caused mainly due to the
monazite bearing black sands. Natural radiation levels
in this region are higher than normal which are believed
to be emitted from the rich deposits of the monazite
bearing beach sands. The mineral monazite contains radio
elements, which is the main cause for natural radiation in
the Southwest coastal belt. Natural radionuclides in soil
are responsible for the background radiation exposure to
the population.
Natural radio nuclides in soil generate a significant
component of the background radiation exposure
to the population and gamma‑radiation intensity in a
region depends on soil and geomorphology. Therefore,
measurements of natural radioactivity in soil are of an
interest for many researchers worldwide, which has led
to worldwide national surveys in the past two decades.
Figure 1: Location map
28 Radiation Protection and Environment | Volume 40 | Issue 1 | January-March 2017
This study has been undertaken to measure the activity
concentrations of 40K, 232Th, and 238U in high background
radiation area soil samples collected from Thoothoor to
Chettikulam of Southwest Coast Tamil Nadu, India and to
assess the radiological conditions with statistical approach.
MATERIALS AND METHODS
Description of study area
The area chosen for this study was Southwest coastal
stretch of Tamil Nadu Kanyakumari district. The sampling
locations are located between 77°8’ and 77°38’of East
of longitude and 8°16’ and 8°19’ North of latitude. The
district has 62 km of coast on the Western side (Arabian
Coast) and 6 km of coast on the Eastern side (Gulf of
Mannar/Bay of Bengal Coast). The investigated locations
are Thoothoor, Eramanthurai, Colachel, Mandaikadu,
Manavalakurichi, Pillaithoppu, Azhickal, Muttom,
Kootapuli, and Chettikulam beach areas of Southwest
coast of Tamil Nadu, India.
Sample collection
The soil samples collected at different locations of
Southwest coast of Tamil Nadu are shown in Figure 1.
The locations selected for sampling were uncultivated areas
and each soil sample collection an area of 1 m × 1 m was
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Ajithra, et al.: Assessment of natural radioactivity and associated radiation indices in soil samples

marked and carefully cleared of debris to a few centimeters 27.3–794.3 and 44.1–251.4  Bq/kg-1, respectively. The
depth. Sampling site was chosen away from field boundary, data set includes high background and also a few normal
a road, or other obstruction. The collected samples were background locations such as PHU, AKL, MTM, KPL
then placed in labeled polythene bags and transferred to and CKM.. Figure 2 shows the variation of activity
the laboratory for preparation and analysis. These samples concentration at different sampling locations.
were mixed together thoroughly, to obtain a representative
sample of that area. Approximately 2 kg of wet weight per 232
Th was higher than 238U in all samples. This could be
sample obtained at a depth of 5 cm from the top surface related to their difference in chemical speciation and
layer. After removing stones and vegetable matter, each solubility in a natural environment. 232Th is insoluble and also
soil sample was packed into a water‑tight bag to prevent preferentially accumulated on the particular phases relative
cross contamination and shifted to the laboratory. Sample to 238U.[5,6] The high value for 232Th activity concentration
preparation was carried out by placing each soil sample observed at Mandaikadu  (MDU), Colachel  (CLL) and
in an oven, drying at a temperature of 105°C to achieve Thoothoor (THR) in the study area could be explained
a constant weight and pulverizing the sample into a fine due to the presence of black sands, which are enriched in
powder to pass through a standard 1 mm meshsize. The the mineral monazite containing a significant amount of
homogenized samples were placed in 250 ml Marinelli 232
Th. The enrichment occurs because the specific gravity
beakers, sealed with a polyvinyl chloride tape and stored for of monazite allows its concentration along beaches where
at least 1 month prior to measurement to attain radioactive lighter materials are swept away[7] and anthropogenic
equilibrium between 226Ra and 228Ac and their short lived inputs can release the additional amounts of natural
progeny (>7 half‑lives of 222Rn and 220Rn). radionuclides into the environment. From the results, it
is clear that the activity of 238U and 40K are lower while
Radiometric analysis that of 232Th is higher when compared with worldwide
The soil samples collected from the locations indicated on average value  (UNSCEAR, 2000) for this selected high
the data acquisition were subjected to gamma spectroscopic background radiation area (HBRA) regions of this study
analysis. Measurements of the radionuclide activities in (MDU, CLL & THR).
the soil samples were under taken using a high resolution,
low background, hyper pure P‑type coaxial gamma ray To determine the radiation hazard index due to the
detector (ORTEC HPGe) coupled to an ORTEC analyzer natural radioactivity associated with the soil, different
and an 8 K multi‑channel analyzer. The system has relative radiological parameters are estimated and the obtained
efficiency of 50% and resolution of 1.85 at a 1332 keV values are compared with internationally recommended
gamma line of 60Co. The spectrometer is calibrated using safe limits.
standard samples 137Cs and 60Co supplied by International
Table 1: Geographical information of sampling points,
Atomic Energy Agency, Vienna. The minimum detectable
Kanyakumari, Tamil Nadu
activity for 232Th, 238U, and 40K are 1.0, 3.5 and 12.25 Bq/ Location ID Location name Latitude Longitude
kg at a back‑ground shielding factor of 95%. THR Thoothoor 8.260998 77.143094
EMI Erayumanthurai 8.244220 77.163435
The analysis of the gamma spectra obtained is performed CLL Colachel 8.178620 77.256097
MDU Mandaikadu 8.163112 77.278588
with dedicated software, and the choice of the reference
MVI Manavalakurichi 8.147144 77.302287
peak is made in such a way that they are sufficiently PHU Pillaithoppu 8.126836 77.336750
discriminated. Of the peaks that could be identified through AKL Azhickal 8.135666 77.341913
MTM Muttom 8.126215 77.319644
the software, reference is made to that at 1.764 MeV for KPL Kootapuli 8.151110 77.600624
214
Bi in the 238U decay chain, that at 2.614 MeV for 208Tl CKM Chettikulam 8.160556 77.615833
in the 232Th decay chain, and one at 1.460 MeV of 40K.
Each measurement is performed with a counting time of
10,000 s.

RESULTS AND DISCUSSIONS

Activity concentrations of 238U, 232Th and 40K in the soil

The activity concentrations of 238U, 232Th and 40K together
with their average values for the soil samples are shown in
Table 1. All values are given in Bq/kg of dry weight. The Figure 2: Locations versus activity concentrations and radium
range of activities for 238U, 232Th, and 40K are 5.1–158.2, equivalent activity (Bq/kg)

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Ajithra, et al.: Assessment of natural radioactivity and associated radiation indices in soil samples
Determination of radiological hazard indices
Radium equivalent activity
It is well known that natural radionuclides 226Ra, 232Th, and
40
K are not uniformly distributed in soil. The nonuniform
distribution of these naturally occurring radionuclides
is due to several reasons such as land use patterns. For
uniformity in exposure estimates, the concentrations
of radionuclides have been defined in terms of radium
equivalent activity (Raeq) having units Bq/kg.
Raeq = AU + 1.43 ATh + 0.07 AK(1)
Where AU, ATh and AK are the activity concentrations of
238
U, 232Th and 40K, respectively (in Bq/kg). The assumption
is that 370 Bq/kg of 226Ra or 238U, 256 Bq/kg of 232Th
and 480 Bq/kg of 40K produce the same gamma‑ray
dose rate. As can be seen from Table 1, the Raeq
values for the soil samples varied from 51.35 (MTM) to
1296.36 (MDU) Bq/kg with the average of 471 Bq/kg.
The mean value of the Raeq obtained for the soil sample
is 471 Bq kg-1,(when all locations are considered), which
is higher than the recommended safe value of 370 Bq kg-1
(OECD (1979). Figure 2 shows the locations and Raeq.
Absorbed dose rate
The absorbed dose rate (D R) enables estimation of
radiation exposure from natural gamma radiation on the
terrestrial mainland. To assess the exposure to natural
radiation and convert activity concentrations of natural
radionuclides into dose rates, the DR in the air at 1 meter
above ground surface was calculated. Therefore, DR was
estimated using dose conversion factors 0.462 nGy/h for
238
U series, 0.604 nGy/h for 232Th series and 0.042 nGy/h
for 40K (UNSCEAR 2000).
DR (nGy/h) =0.462 AU + 0.604 ATh + 0.042 AK(2)
Where, AU, ATh and AK represent the activity concentrations
of 238U, 232Th and 40K in Bq/kg, respectively in the
samples. Using the above formula DR had been evaluated
and tabulated in Table 1. The absorbed dose rate values
ranged between 42.2 (MTM) and 1022.9 (MDU). The
Global and Indian average dose rates are 84 nGy/h and
90 nGy/h respectively as reported by UNSCEAR (2000).
The higher absorbed dose rates in few locations are due
significant amount of 232Th in the study area. Figure 3
shows the variation of absorbed gamma dose rate in
different locations.
Annual effective dose rate
To estimate the annual effective dose (HR), one has to
take into account the conversion factor from absorbed
30 Radiation Protection and Environment | Volume 40 | Issue 1 | January-March 2017
Figure 3: Locations versus absorbed gamma dose rate (nGy/h)
dose in air to effective dose and the outdoor occupancy
factor. In the recent UNSCEAR (2000) reports, a value
of 0.7 Sv/Gy was used for the conversion factor from
absorbed dose in air to effective dose received by adults,
and 0.2 for the outdoor occupancy factor, implying that
20% of time is spent outdoors on average around the
world. The effective dose rate was calculated from the
formula:
HR = DR (nGy/h) × 8760 h × 0.2 × 0.7 Sv/Gy × 10−6(3)
Where DR (nGy/h) is given by the Equation 2. The estimate
result for HR is given in Table 1. The estimated HR values
for all the studied samples ranged from 0.052 to 1.255
mSv/year with a mean of 0.459 mSv/year. In areas with
the normal background radiation, the average annual
external effective dose from terrestrial radionuclides is
0.07 mSv/year.[9] Therefore, the obtained mean value from
this study area (0.459 mSv/year) is higher than the world
average value due to high 232Th concentration in soil, as it
is a known HBRA. Figure 4 shows the locations and HR
of soil samples.
External radiation hazard indices
The external hazard index (Hex) is an important parameter
to evaluate the radiation dose expected to be delivered
externally if these materials are used for construction of
buildings. This index value must be less than unity for the
radiation hazard to be negligible. This Hex was calculated
from the formula:[10]
AU ATh AK
H ex = + +  (4)
370 Bq /kg 258 Bq /kg 4810 Bq /kg
Where AU, ATh, and AK are the activity concentrations of
238
U, 232Th and 40K, respectively. The calculated external
hazard values are between 0.14 (MTM) and 3.53 (MDU).
Figure 5 shows the variation of Hex with sampling locations.
Internal radiation hazard indices
The internal hazard index (Hin) is used to reduce the
internal exposure to 222Rn and its radioactive progeny. For
safe use of soils for building constructions, it should be
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Ajithra, et al.: Assessment of natural radioactivity and associated radiation indices in soil samples

noted that Hin is ≤1. Hence, the Hin, was calculated using
the following formula:[10]
AU ATh AK
H in = + + (5)
185 Bq /kg 259 Bq /kg 4810 Bq /kg
The calculated radiation Hin of soil samples are given
in Table 2. This Hin values vary from 0.152 (MTM) to
3.900 (MDU) with an average of 1.442 which is higher
than the recommended value of unity. Figure 5 shows the
variation of Hin with sampling locations.
Multivariate statistical analysis
Multivariate statistical methods are successfully used
to interpret the relationships among variables in the
environmental studies (Liu et al., 2003).[11] Multivariate
analysis such as principle component analysis (PCA),
and cluster analysis  (CA) is used to explain the
correlation amongst a large number of variables in
terms of a small number of underlying factors without
losing much information. [12,13] This method can also
help to simplify and organize large data sets to provide
meaningful insight (Laaksoharju et al., 1999),[14] and can
help to indicate natural associations between samples
and/or variables. [15] The main  Statistical Software
Statistical Program for the Social Science  (SPSS/PC,
Chicago, Illinois, United States) was used for statistical
analysis.
Basic statistics
The average activity concentration with minimum,
maximum, and standard deviation, kurtosis, and skewness
are presented in Table 3. In general, if the standard
deviation is higher than the mean value then it indicates
that low degree of uniformity and vice versa. In the present
study, the standard deviation value of 232Th higher than the
mean value indicates that low degree of uniformity, whereas
238
U and 40K standard deviations lower than the mean value
indicates the that high degree of uniformity in the soils.
According to Adam and Eltayeb,[16] skewness data of
natural radionuclide describes the degree of asymmetry of
a distribution around its mean. Positive skewness [Table 3]
indicates a distribution with an asymmetric tail extending
toward values that are more positive. Negative skewness
indicates a distribution with an asymmetric tail extending
toward values that are more negative. Kurtosis is a measure
of the peakedness of the probability distribution of a
real‑valued random variable. It characterizes the relative
peakedness or flatness of a distribution compared with the
normal distribution. Positive kurtosis indicates a relatively
peaked distribution. Negative kurtosis indicates a relatively
flat distribution. From Table 3, kurtosis of 40K is positive

Figure 4: Locations versus internal hazard index and external hazard

index Figure 5: Clustering of radioactive variables

Table 2: Activity concentration and radiation indices in soils of Kanyakumari, Tamil Nadu
Sample ID Activity concentration (Bq/kg) Raeq (Bq/kg) DR (nGy/h) HR (mSv/year) Hin Hex
U±1σ
238 232
Th±1σ 40
K±1σ
THR 133.2±4.9 580.7±8.8 124.0±9.5 973.2 771.2 0.95 2.98 2.63
EMI 43.7±3.0 144.6±5.1 44.0±25.3 254.0 202.9 0.25 0.80 0.68
CLL 158.2±23.2 756.9±41.8 251.3±11.2 1260.0 998.3 1.23 3.83 3.41
MDU 147.8±5.4 794.2±10.6 165.0±11.3 1296.0 1022.9 1.25 3.90 3.51
MVI 56.8±3.7 232.0±6.7 66.5±11.0 393.7 312.8 0.38 1.21 1.06
PHU 22.6±2.4 58.8±4.3 75.8±11.3 112.6 91.6 0.11 0.36 0.30
AKL 24.6±2.6 61.3±4.5 49.7±12.0 116.1 94.0 0.11 0.38 0.31
MTM 5.0±1.5 27.3±3.9 93.5±10.7 51.3 42.2 0.05 0.15 0.13
KPL 19.4±2.2 61.0±4.0 110.1±14.3 115.2 93.8 0.11 0.36 0.31
CKM 17.4±2.9 78.0±3.0 103.1±9.5 136.9 110.1 0.13 0.41 0.37
CLL: Colachel, THR: Thoothoor, MDU: Mandaikadu, EMI: Erayumanthurai, MVI: Manavalakurichi, PHU: Pillaithoppu, AKL: Azhickal, MTM:
Muttom, KPL: Kootapuli, CKM: Chettikulam, Raeq: Radium equivalent activity, DR: Absorbed dose rate, HR: Annual effective dose rate, Hin: Internal
hazard index, Hex: External hazard index

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Ajithra, et al.: Assessment of natural radioactivity and associated radiation indices in soil samples

indicate its peaked distribution whereas kurtosis of 238U Table 3: Summary of basic statistics of natural radionuclides
and 232Th is negative shows that flat distribution in the (Bq/kg) in soils
Variables U
238
Th
232
K
40
soil samples.
Mean 62.90 279.53 108.35
Minimum 5.05 27.34 44.06
Pearson correlation analysis Maximum 158.25 794.29 251.38
Pearson correlation analysis has been carried out to SD 59.66 307.74 61.94
determine the mutual relationships and strength of Variance 3559.67 94,706.50 3837.59
Kurtosis –1.187 –0.851 2.507
association between radionuclides and radiological Skewness 0.868 1.021 1.481
parameters. The results of the Pearson correlation Frequency Log‑normal Log‑normal Normal
co‑efficient of variables are given in Table 4. A very strong distribution
SD: Standard deviation, 238U: Uranium, 232Th: Thorium
positive correlation (R = 0.991) was found between the
238
U and 232Th. This may indicate the strong relationship
Table 4: Pearson correlations between radionuclides and
between 238U decay series and 232Th decay series in soils and associated radiological hazards
occur together in nature.[16] 40K had moderate correlation Variables U
238 232
Th K
40
Raeq DR HR Hin Hex
with uranium/thorium indicates that origin of 40K occur in 238
U 1
different decay series in nature. The calculated radiological 232
Th 0.991 1
parameters Raeq, DR, Hin, Hex showed that very strong
40
K 0.770 0.800 1
Raeq 0.993 1.000 0.800 1
positive correlation with 238U and 232Th. This indicates DR 0.993 1.000 0.801 1.000 1
that all the radiological parameters strongly associated HR 0.993 1.000 0.801 1.000 1.000 1
Hin 0.994 1.000 0.798 1.000 1.000 1.000 1
with concentration of uranium and thorium in the soils Hex 0.993 1.000 0.800 1.000 1.000 1.000 1.000 1
and these radionuclides mainly contribute the emission of Raeq: Radium equivalent activity, DR: Absorbed dose rate, HR: Annual
gamma radiation in the study area. effective dose rate, Hex: External hazard index, Hin: Internal hazard index,
238
U: Uranium, 232Th: Thorium
Principal component analysis
PCA is the most common multivariate statistical Table 5: Rotated factor loadings of variables
method used in environmental studies. This is widely Variables Component 1 Component 2
used to reduce data and to extract a smaller number U 0.905 0.409
238

232
Th 0.893 0.450
of independent factors (principal components) for 40
K 0.444 0.896
analyzing relationships among observed variables.[17] In Raeq 0.893 0.450
the present study PCA was applied to identify variables by DR 0.892 0.451
HR 0.892 0.451
applying varimax rotation with Kaiser normalization. By Hin 0.895 0.446
extracting the Eigen values and Eigen vectors from the Hex 0.893 0.450
Percentage of variance 74.92 24.96
correlation matrix, the number of significant factors and explained
the percent of variance explained by each of them were Raeq: Radium equivalent activity, DR: Absorbed dose rate,
calculated. Table 5 gives the results of PCA with varimax HR: Annual effective dose rate, Hex: External hazard index,
rotation. The results show that these two factors could Hin: Internal hazard index, 238U: Uranium, 232Th: Thorium
explain over  99.88% of the total variance. Normally,
an ordination result was good if the value was 75% or Cluster analysis
better.[18,19] CA is one of the multivariate techniques used to identify
and classify groups with similar characters in a new group
Component 1 is the most widespread within the determined of observations. CA is often coupled with PCA to check
natural radionuclides and radiological parameters describing results and to group individual parameters and variables.
74.92% of the data variability. It is characterized by high The purpose of CA is to discover a system of organizing
positive loading of 238U and 232Th and strong positive observations where a number of groups/variables
loadings of all radiological parameters. share observed properties. A dendrogram is the most
commonly used method of summarizing hierarchical
This Component 1 shows that the concentration uranium clustering. CA carried out through axes was to identify
and thorium plays the main role in natural radioactivity. similar characteristics among natural radioisotopes and
Component 2 loaded due to high positive loading of 40K radiological parameters in the soils.[19] In CA, the average
with accounts for 24.96% of total variance. This shows linkage method along with correlation coefficient distance
that concentration of 40K not contribute in the total natural was applied and the derived dendrogram is shown in
radioactivity. Figure 5.

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Ajithra, et al.: Assessment of natural radioactivity and associated radiation indices in soil samples
In this dendrogram, all radiological parameters and three
radionuclides were grouped into three statistically significant
clusters. Cluster‑I consists of Hex, Hin, HR, 40K and 238U.
Cluster‑II consists of 232Th and main radiological parameters
such as DR and Raeq. This is due to the high activity
concentration of thorium in the soil samples. From this CA,
Hex and Hin in the study area are due to the concentration
of 238U and dose absorbed by the human beings are due to
high concentration of 232Th. This CA results are in good
agreement with PCA and correlation analysis.
CONCLUSIONS
The measured activity concentrations of 238U, 232Th, and
40
K in soil samples from the high HBRA region for a
few locations are higher than the world average value
reported by UNSCEAR  (2000). The estimated gamma
DR is higher than the recommended safe limit. Hence, it
is observed that the soil samples may not be suitable for
building materials. The radiological data were processed
using multivariate statistical methods, Pearson correlation
coefficient, cluster, and factor analyses determined the
similarities and correlation between the various samples
in more systematic way.
Financial support and sponsorship
Nil.
Conflicts of interest
There are no conflicts of interest.
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