Radiation Measurements 34 (2001) 365–371

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The e!ect of soil particle size on soil radon concentration

A.H. Khayrata , M.A. Oliverb; ∗ , S.A. Durranic
a TaizUniversity, Faculty of Science, Department of Physics, Taiz, Republic of Yemen
b Department of Soil Science, University of Reading, Whiteknights, Reading RG6 6DW, UK
c School of Physics & Astronomy, University of Birmingham, Birmingham B15 2TT, UK

Received 28 August 2000; received in revised form 15 January 2001; accepted 8 March 2001

Abstract
It has been suggested in the literature that the radon concentration in the soil gas is related to the particle size distribution
of the soil. This paper examines this relation. Radon concentration was measured in the soil on the Carboniferous limestone
south of Buxton in Derbyshire, England, using the can technique. At each site, a sample of soil was taken at the bottom of
the hole in which the dosimeter was placed to determine the particle size distribution.
The correlations between the raw values of radon concentration, soil particle size fractions and elevation were weak.
Nevertheless, the kriged maps of radon, silt, clay and elevation showed some spatial relation to one another. The kriged
estimates showed stronger correlations among these properties, especially between radon and elevation.  c 2001 Elsevier
Science Ltd. All rights reserved.

Keywords: Radon soil-gas; Kriging; Spatial variation; Soil particle size

1. Introduction true for radium distributed uniformly throughout the volume

The e!ect of soil particle or grain size on the concen-
tration of radon in soil gas was investigated. Jong et al.
(1993) suggested that the radioactivity of the soil depends
on grain size: the radioactivity decreases with sand content
in the soil and increases with clay content. Considering the
‘surface distribution model of radium atoms’ (Morawska
and Phillips, 1993), it is assumed that the radium atoms are
present only on the surface of the soil particles. It follows
that for all radium atoms, the distance between the radium
atom and surface is zero. Here, the surface : volume ratio
will be larger for smaller sized particles. In this case, the
radium concentration is inversely proportional to the radius
of the particles, and the emanating power (which is deAned
as the ratio between the number of radon atoms emanating
per unit time and the total number of radon atoms formed
per unit time) is independent of grain size. The opposite is
of the particle (volume model).
2. Exploring radon spatial variation
Spatial information is generally obtained at selected loca-
tions, sampling points. The sampling design and intensity of
sites at which to measure radon concentration will depend
on how radon varies spatially, and the method of estimation
that we would either like to use, or that is appropriate. Since
it seems likely that radon varies more or less continuously
in geographical space, it can be regarded as a regionalized
variable (Matheron, 1965; Badr et al., 1993) and can be
analysed geostatistically.
A model of spatial variation for geostatistical estimation
is (Webster and Oliver, 2001):
Z(x) =  + (x); (1)

∗ Corresponding author. Tel.: +44-1189-316557; fax: +44- where Z(x) is the random variable at x,  is the local mean
1189-316666. of Z in the neighbourhood of x, and (x) is a random term
E-mail address: m.a.oliver@reading.ac.uk (M.A. Oliver). with an expectation of zero and a variance such that for any

1350-4487/01/$ - see front matter
c 2001 Elsevier Science Ltd. All rights reserved.
PII: S 1 3 5 0 - 4 4 8 7 ( 0 1 ) 0 0 1 8 7 - 1
366 A.H. Khayrat et al. / Radiation Measurements 34 (2001) 365–371

two places x and x + h separated by a lag h is of the data z(x1 ); z(x2 ); : : : ; z(xn ) at the unknown block:
2
var[(x) − (x + h)] = E[{(x) − (x + h)} ] = 2(h);
n
z(B)
ˆ = i z(xi ); (6)
(2) i=1
where  is the semivariance between two places, a distance where n usually represents the data points within the local
and direction h apart. If  is constant locally, then Eq. (2) neighbourhood, V , which is much less than the total number
is equivalent to in the sample, and i are the weights. The weights are chosen
(h) = 12 E[{Z(x) − Z(x + h)}2 ]; (3) to sum to 1 to avoid bias and to minimize the estimation
variance.
where Z(x) and Z(x + h) are the observed values of z at xi
n
and xi + h, respectively, and E denotes the expectation. The i = 1:
function (h) that relates the variance to the lag is the var- i=1
iogram. The usual computing formula for the variogram is The estimation variance of Z(B) is
M (h)

n

n
n
1

(h)
ˆ = [z(xi ) − z(xi + h)]2 ; (4) 2 (B) = 2 i (x
J i ; B) − i j (xi ; xj ) − (B;
J B);
2M (h) i=1 i=1 i=1 j=1
(7)
where M (h) is the number of comparisons made at lag h,
and ˆ signiAes that the result is an estimate. The variogram where (xi ; xj ) is the semivariance between points xi and
provides an unbiased description of the scale and pattern of xj , (x
J i ; B) the average semivariance between data point
spatial variation, the spatial model needed for kriging, and a xi and the block B, and (B;J B) the within block variance.
basis for designing optimal sampling schemes (McBratney These semivariances are derived from the variogram model
et al., 1981). because the experimental semivariances are discrete and at
limited distances. The value of 2 (B) is least when

n

3. Estimating radon concentration i (xi ; xj ) + = (x

J i ; B) for all j;
i=1
There are two basic procedures for estimating the val-

n

ues of properties at unsampled sites from fragmentary in- i = 1: (8)

formation: classiAcation and interpolation. ClassiAcation is i=1

the classical approach, and any spatial autocorrelation is as-
sumed to be accounted for by the classes and any residual
variation within them is regarded as wholly random. The
estimate of zij is a mean of the observations in class j:
1

n
Ẑ ij = zij ; (5)
nj i=1
where n is the number of observation in class j. The esti-
mator, Ẑ ij is the weighted average of the observations in the
class, with weights equal to 1=nj .
If the classiAcation accounts for all of the spatially de-
pendent variation then the class mean is the best estimate
of the property and we can do no better. However, if there
is a spatial dependence remaining within the classes, then
interpolation by a method such as kriging can be used for
estimating values of properties at unsampled sites. Kriging
is essentially a method of weighted moving averages of the
observed values of a property in a given neighbourhood.
If sample data are spatially dependent, or autocorrelated,
or there is spatial dependence remaining within the classes,
then interpolation should provide more local detail on how
the property of interest varies spatially than does classiA-
cation. The method of geostatistical prediction is known
as kriging which is an optimal method of interpolation
(Webster and Oliver, 2001). Consider that radon concentra-
tion, Z, has been measured at sampling points, xi , i = 1;
: : : ; n, and we would like to use this information to estimate
its value at a block xB . The estimate is a weighted average
The Lagrange multiplier, , is introduced to achieve
minimization.
4. Study area
We surveyed an area of 4 km2 just to the South of Bux-
ton in the county of Derbyshire near Biggin (National Grid
reference SK 41553594). The sampling scheme was based
on the spatial information from a nested survey and analysis
(Badr et al., 1993). Ideally, sampling on a grid is preferred
for local estimation, but this was not feasible here because
we had to take the landowners’ convenience into account in
locating the detectors as they had to be left in situ for about
4 weeks. In addition, we wanted to compute the variogram
as precisely as possible at the short lag distances since this
is the part of the variogram that is most important for krig-
ing. The sampling interval was irregular, it varied from 50
to 250 m, which was well within the extent of spatial de-
pendence indicated by the reconnaissance variogram. Fig. 1
shows the location of the 93 sampling points; they are fairly
evenly spread over the area while ensuring that there would
be enough comparisons at the shorter lags.
5. The experimental procedure
Soil radon concentration was measured using solid state
nuclear track detectors, CR-39, and the ‘can technique’
 A.H. Khayrat et al. / Radiation Measurements 34 (2001) 365–371
Fig. 1. Map shows the locations of the sampling points for the survey in two dimensions near Biggin, Derbyshire (England), together with
the relief, roads, faults and geology.
(Durrani and Bull, 1987; Durrani et al., 1990). Ninety-three
dosimeters were placed at a depth of 50 cm in the soil over
the surveyed area. A sample of the soil was taken at the
bottom of each hole where a dosimeter was placed.
For soil particle size study, the soil samples were collected
from the holes created with a bucket auger. The soil was
sieved and the Ane fraction, ¡2 mm, was dispersed in water
containing Calgon. The proportions of sand, silt, and clay
were then determined by settling. Elevation was recorded
over the area at the same sites as were those at which radon
was measured.
6. Results and discussion
Radon concentration in the surveyed area varied between
2:78 and 35:11 kBq m−3 . The summary statistics of the
properties for the above survey are given in Table 1. Radon
367
concentration was marginally skewed; therefore, the values
were transformed to logarithms. Experimental variograms
were computed from the raw data and the transformed val-
ues. Since the variograms were similar, the raw values were
used to avoid back-transforming the kriged logarithmic esti-
mates. Fig. 2a shows the experimental semivariances plotted
as discrete points.
A mathematical model was Atted to these values
by weighted least-squares approximation using Genstat
(Genstat 5 Committee, 1993). A power function provided
the best At and this is shown as the solid line in Fig. 2a.
This is an unbounded variogram which we might expect for
a single lithology. The monotonically increasing section of
the variogram represents the continuous component of the
variation. There is a large nugget variance which represents
the considerable locally erratic component of the variation,
which Badr et al. (1993) also observed.
368 A.H. Khayrat et al. / Radiation Measurements 34 (2001) 365–371

Table 1
Summary statistics for the survey on a single lithology in two dimensions in Derbyshire

Statistic Radon (kBq m−3 ) Elevation (m) Clay % Silt % Sand %

Number of observations 93 93 87 87 87
Mean 13.03 327.7 19.64 66.68 13.49
Median 11.27 328.0 18.80 68.98 11.72
Minimum 2.78 293.0 2.10 11.40 0.62
Maximum 35.11 379.0 39.67 95.90 54.99
Variance 57.67 657.4 64.34 129.4 81.33
Standard deviation 7.59 25.64 8.02 11.38 9.02
Skewness 1.11 0.272 0.232 −1.58 2.25

Fig. 2. Variograms for Biggin, Derbyshire: (a) radon concentration; (b) the residuals from the trend for elevation; (c) percentage clay; and
(d) percentage silt. The symbols are the experimental semivariances and the solid line is the Atted model in each case.

Table 2
Variogram model parameters for properties measured in the two dimensional survey in Derbyshire

Variable Model type Nugget Structured Slope Exponent Distance

variance component c w  parameter d

Radon Power 46.21 0.2604 0.8108

Elevation Exponential
Residuals 0.0 59.52 358.68
Clay% Power 55.54 0.0055 1.6219
Silt% Power 326.9 0.0615 1.6467
Sand No suitable
model Atted
 A.H. Khayrat et al. / Radiation Measurements 34 (2001) 365–371 369

Fig. 3. Maps of kriged estimates of: (a) radon concentration in the soil gas (the units are kBq m−3 ), and (b) of elevation (the units are
metres) near Biggin, Derbyshire (England).

Variograms were also computed for elevation and the
particle size fractions. The variogram for elevation showed
evidence of trend, which we removed by a linear func-
tion of the coordinates. We computed the variogram from
the residuals and Atted an exponential model to them: its
parameters are given in Table 2. The exponential model
reaches its sill asymptotically; therefore, there is no abso-
lute range or limit of spatial dependence. Fig. 2b shows the
experimental variogram with the Atted model. The vari-
ograms for the particle size fractions are erratic and have
large nugget variances, possibly because there are few sam-
ples. Fig. 2c and d shows the variogram of percentage clay
and silt, respectively. They were modelled with power func-
tions as for the radon concentrations. Table 2 gives the pa-
rameters of these models. The variogram of sand content
was pure nugget, i.e. it shows no spatial structure.
370 A.H. Khayrat et al. / Radiation Measurements 34 (2001) 365–371

Fig. 4. Maps of kriged estimates of: (a) percentage clay, and (b) percentage silt near Biggin, Derbyshire (England).

The parameters of the variogram models for radon, and
silt and clay were then used together with their values for
estimating their concentrations over the area by block krig-
ing. Fig. 3a shows the kriged map of the estimates of radon
concentration. It shows that the values change in a fairly
continuous way, which is what we might expect on a sin-
gle lithology. The radon concentrations decrease from West
to East: they are largest in the low-lying area of the West
and smallest on the plateau and spur in the East. The pattern
of the variation is particularly distinctive because the radon
concentrations appear to have an inverse relation with the
relief, Fig. 3b. The small radon concentrations are associ-
ated with the highest elevations which are in the eastern part
of the area, and the largest values in the western part where
the elevation is low. The radon values mirror the relief in-
versely in a fairly close way as seen by the relation with the
valleys.
Fig. 4a and b shows the contour maps of the kriged es-
timates of clay and silt contents for the area. There also
appears to be a relation between clay content, radon con-
centration and elevation: clay content is the least in West
and North West and the greatest on the plateau and spur in
 A.H. Khayrat et al. / Radiation Measurements 34 (2001) 365–371
the East. Silt concentration is greatest between the plateau
and valley and also along the dry valleys. It seems that the
large particle size fraction is associated with the large radon
concentration in the soil. This relation needs to be examined
further.
7. Conclusion
This survey did not show a positive relation between clay
content and radon concentration in the soil as suggested
by Jong et al. (1993). However, there appeared to be a
weak relation between sand and silt contents and radon. The
strongest apparent relation is between radon concentration
and elevation. Oliver and Khayrat (2000) explored this rela-
tion further using a ground conductivity survey. This showed
that the thickness of superAcial materials over the limestone
in the West was greater than on the plateau in the East.
From this, we deduced that most of the radon was emitted
from soil or regolith particles rather than from the underly-
ing rock. The nature of the particles in the soil associated
with this emission needs further investigation.
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