Computers & Geosciences 27 (2001) 939957

A geostatistical investigation of the spatial variation of radon in soil

M.A. Olivera,*, A.L. Khayratb
a

Department of Soil Science, The University of Reading, P.O. Box 233, Whiteknights, Reading RG6 6DW, UK b Department of Physics, College of Science, Taiz University, Republic of Yemen, Yemen Received 1 January 1999; accepted 31 January 2000

Abstract Concern about possible links between emissions of radon (Rn) and certain types of malignant disease has led to surveys to measure Rn concentrations in the soil and in dwellings. There is little information about the spatial scales of Rn variation in bedrock and soil. Such information on Rn is needed to eectively sample it in order to measure for spatial prediction. To explore the spatial variation of Rn concentration in soil gas, it was measured using solid-state nuclear track detection in a Rn aected area in the English Midlands. Three surveys are described which show dierent sampling approaches for exploring spatial variation. The rst was a nested survey with seven stages conducted near Buxton in Derbyshire (UK), in an area comprising three principal lithologies (two limestones and a sandstone). The other surveys were south of Buxton on the Monsal Dale limestone. One was an irregularly distributed sample in two dimensions in which Rn concentration, particle size distribution, and elevation were recorded. The other was along a transect 2 km long. In addition to Rn concentration, ground conductivity and slope angle were measured at 20 m intervals. The results of the nested survey suggest that geology exerts a strong control on Rn variation, and those of the other two surveys that other factors are also involved, such as elevation, soil depth, and soil particle size distribution. # 2001 Elsevier Science Ltd. All rights reserved.
Keywords: Geostatistics; Kriging; Nested survey; Radon; Spatial variation; Variogram

1. Introduction Radon (Rn) is a ubiquitous naturally occurring radioactive gas that may be emitted from any rocks that contain radium. The Rn potential for a given region is likely to be the result of a combination of properties of the underlying bedrock and of the soil, such as the distribution of uranium (U) and radium (Ra), porosity, permeability, and moisture content, as well as weather conditions. Exposure to natural sources of radiation has become an important issue in terms of radiological protection. Most exposure comes from 222Rn and its solid, short-lived daughter products, 218Po, 214Pb and
*Corresponding author. Tel.: +44-1734-316557; fax: +441734-316660. E-mail address: m.a.oliver@rdg.ac.uk (M.A. Oliver).

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Bi. The National Radiological Protection Board (NRPB, 1992) estimates that Rn possibly accounts for approximately 50% of a persons annual dose of radiation from all sources in the United Kingdom. There is interest in the spatial distribution of Rn because of putative links with malignant disease. Elevated levels of Rn in houses are thought to lead to increased malignancy, in particular lung cancer (Clarke and Southwood, 1989; Green et al., 1992). Furthermore, other epidemiological studies have suggested that exposure to Rn might be a cause of several forms of cancer, including certain childhood cancers (Henshaw et al., 1990; Lucie, 1989). To substantiate these correlations, and to relate Rn values to estimates of the risk of malignancy (Oliver et al., 1992), information is required about the spatial variation of Rn concentration. Bowie and Bowie (1991), for example, have

0098-3004/01/$ - see front matter # 2001 Elsevier Science Ltd. All rights reserved. PII: S 0 0 9 8 - 3 0 0 4 ( 0 0 ) 0 0 1 3 3 - 3

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commented on the lack of substantive data on the localized exhalation rates of Rn. To describe Rn emanation in a given area reliably there is a need to determine what kinds of estimates can be made. It has already been accepted generally that Rn emission is aected by geology (Gundersen et al., 1988; Schumann and Owen, 1988), and this led Ball et al. (1991) to suggest that a few well-sited measurements could be used to predict its values over a larger area. Essentially, such estimates represent the mean concentrations of Rn for a given spatial class related to the underlying geology. In some areas, however, there could be considerable local variation in Rn concentration within geological units because its distribution depends on factors other than lithology, such as geologic structure, atmospheric pressure, temperature, soil moisture, CO2 concentration in the soil, soil porosity, and so on. If factors other than lithology aect the variation, then estimates based on classication would result in considerable loss of information, especially for comparing Rn concentration with the incidence of disease. If geology were to account for all of the spatially correlated variation, then it would be sensible to use the within-stratum means as predictors. If not, then some method of local estimation, such as kriging (Matheron, 1965, 1971), should be considered. The choice of the method of prediction depends on knowing something about the structure of the propertys spatial variation, and this in turn has implications for sampling. The body of techniques embodied in geostatistics (Matheron, 1965, 1971) can describe the spatial variation and, thereby, indicate an appropriate method of prediction, and aid the design of optimal sampling schemes for estimation by kriging. To gain insight into the nature of the variation of Rn in soil, gas concentrations were measured in a Rn aected area in Derbyshire (the English Midlands) using three dierent approaches to sampling. A nested survey and analysis with seven stages was used to determine the structure of Rn spatial variation on three lithologies. With this information, two further surveys were designed for a single lithology: the rst was an irregularly distributed sampling in two dimensions and the other was a regular sampling along a transect. In addition to Rn concentration, soil particle size distribution and elevation were recorded for the 2-D survey, and ground electrical conductivity and slope angle were measured for the transect.

2. Radon in soil gas Radon forms in rocks and soil that contain U or Ra. This radioactive element has three important isotopes (Evans, 1955): 222Rn, with a half-life of 3.82 days (a decay product of the iosotope 226Ra in the 238U decay

series); 220Rn, with a half-life of 55 s (a decay product of Ra in the 232Th series); and 219Rn, with a half-life of 4 s (a combined decay product of 223Ra and 219At in the 235 U series). Of these only 222Rn is generally considered a health hazard because it accounts for 47% of the average dose of radiation to the population of the United Kingdom, whereas 220Rn accounts for only 4%, and 219Rn is less than 1% (NRPB, 1990). The isotopes 222 Rn and 220Rn are usually produced in approximately equal quantities, but since the contribution of the latter to the overall dose of radiation is relatively small it is often ignored In general, rocks rather than soil have been thought to be the major source of Rn, for example the granites of Devon and Cornwall (UK) are important sources. The amount of Rn emitted in those counties is among the largest in the United Kingdom (NRPB, 1992). However, Peake and Hess (1987) suggest that the soil itself may also be an important source of Rn. This is supported further by the ndings of Jones (1995) who described the Rn source in soil as either dispersed, i.e. occurring as single particles of U disseminated randomly throughout the soil mass, or as U concentrated in minerals such as zircon, sphene and apatite. By examining the ssion tracks on detectors Jones (1995) concluded that U disseminated throughout the soil is more likely to be a source of mobile Rn than that trapped within minerals. He also found that the Rn concentration in the air in basements in Illinois (USA), was related to U dispersed in soil and not to its total U content. The half-life of 222Rn is 3.82 days, which is another factor suggesting that the Rn in houses is more likely to have formed in the soil than in the underlying rock. This is corroborated by Nero et al. (1990), who estimated that soil contributes more than 90% of Rn in houses, and by Akerblom et al. (1984) and Swedjemark (1986), who also reported that large concentrations of Rn in soil gas were associated with large concentrations indoors. Radon moves into buildings because of a negative pressure dierential, and because of a large concentration gradient between the building and bedrock or soil. Reimer (1991) says that the rate of migration of Rn in soil can inuence greatly indoor Rn concentration. Ball et al. (1991) suggested that the concentration of Rn in houses is likely to relate fairly closely to that in the soil, although there is no well established method of estimating Rn levels in individual dwellings based on soil Rn data. Reimer et al. (1991) also suggested that geology and soil gas Rn are useful indicators of indoor Rn concentration. Agard and Gundersen (1991) went further in suggesting that there are direct correlations between U, Ra, and Rn in the soil and indoor Rn concentrations. Surveys have tended to measure Rn concentration either in the soil or in homes. The relation between Rn concentration in homes and soil is unlikely to be straightforward, however, because of additional
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eects associated with the characteristics of the buildings. There is much scope for further investigation into this relation. For both the soil and buildings there are many other factors, in addition to the spatial variation in the source elements, that complicate the spatial variation of Rn emanation. For example, the spatial variation in soil permeability, porosity, CO2 concentration in the soil gas, moisture content, and atmospheric pressure all aect its emanation. At large soil moisture contents the soil pores become saturated with water which inhibits Rn emission. Carbon dioxide, on the other hand, acts as a carrier gas for Rn in soil which can enhance its concentration in the soil atmosphere near to the surface (Ball et al., 1991). The concentration of Rn inside buildings depends on structural characteristics, ventilation rates, aerosol concentration, central heating, building materials, and the life style of the inhabitants. To avoid the complications associated with buildings, Rn concentrations were measured in the soil using solidstate nuclear track detection (SSNTD)

tary information are classication and interpolation. The choice of approach should depend on the kind of estimates required, the structure of the spatial variation, and whether the data are suitable for interpolation. 4.1. Classication Classication is the classical approach to prediction; it gives an estimate of the mean concentration for each spatial class or stratum, and the estimated value at each location in the class is the mean. Any spatial correlation is assumed to be accounted for by the classes and any residual variation within them is regarded as wholly random. The model for classication is zij m aj eij ; 1

where zij is the value of property Z at any point i in class j, m is the general mean of Z, aj is the dierence between m and the mean of class j, and eij is a random component with zero mean and variance, s2 w , i.e. the within class variance. The estimate of zij is the mean of the observations in class j: zij
j 1X zij ; nj i1

3. Measuring radon in soil Cylindrical cans, each containing a 2 2 cm piece of CR-39 plastic detector, were placed in the ground at a depth of 50 cm. The hole at each sampling location was lined with a 70 cm length of PVC tubing covered at the top so that the detector measured only the Rn being emitted below 50 cm. Full details of this technique are given in Durrani et al. (1990). The detectors were left in situ for approximately three weeks } long enough for the 222Rn (T1/2=3.82 d) to reach equilibrium with its long-lived parent, 226Rn, and for a signicant number of tracks resulting from its a-decay to be registered on the plastic. A lter paper was placed at the base of the can to inhibit the diusion of 220Rn suciently for it to decay before entering the can and so prevent it from aecting the detectors. The detectors were calibrated in a purpose-built drum containing a source of Rn with known activity (Khayrat, 1997). In each case, the detectors were etched electrochemically in the laboratory (Durrani and Bull, 1987) under standard conditions to enlarge the tracks for counting with an optical microscope.

where nj is the number of observations in class j. The estimator, zij , is the weighted average of the observations in the class, with weights equal to nj . If the classication accounts for all of the spatially dependent variation, then the class mean is the best estimate of the property and one can do no better. However, if there is spatially dependent variation remaining within the classes then local detail is lost. 4.2. Geostatistics If a property 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 using a geostatistical approach. However, if the variation comprises marked boundaries that delimit areas of more or less continuous variation then Voltz and Webster (1990) showed that a combination of classication and kriging provides the best estimates. Estimation by some form of interpolation, such as kriging, provides more local detail about the spatial variation of a property. Interpolation, however, is appropriate only if the property varies continuously and the sample data are spatially dependent or correlated. A model of spatial variation for geostatistical estimation is Z x mv ex; 3

4. Estimating radon spatially The sampling design and separation between sampling sites to measure Rn concentration for a spatial investigation will depend on the kind of estimates required and on the nature of the spatial variation of Rn. Two of the main approaches for estimating the values of properties at unsampled sites from fragmen-

where Z(x) is the random variable at x, mv is the local mean of Z in the neighbourhood of x, and ex is a

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random term with an expectation of zero and a variance such that for any two places, x and x h, separated by a lag (a vector in both distance and direction) h is given by varex ex h Eex ex h2 2gh; 4

semivariance between the block and the ith sampling point, and  gB; B is the average variance within the block (i.e. the within-block variance). Subject to the above constraint on the weights, the estimation variance s2 B is least when
N X i1

where g is the semivariance between two places a distance and direction h apart. If mv is constant locally then Eq. (4) is equivalent to
2 1 gh 1 2 varZ x Z x h 2EZ x Z x h ;

li gxi ; xj c  gxj ; B for all j

and
N X i1

5 which denes the variogram of Z. The variogram provides an unbiased description of the scale and pattern of spatial variation, the spatial model needed for kriging, and a basis for designing optimal sampling schemes (McBratney et al., 1981). The variogram is scale dependent, therefore, one needs to have some idea of the order of magnitude of the spatial variation to sample adequately for its precise estimation. Clues to the approximate scale of the variation are often elusive because spatial variation is complex, and variation can occur on multiple scales which may dier by several orders of magnitude simultaneously (i.e. nested variation). An ecient means of exploring the spatial structure of the variation at the outset is by a nested sampling scheme and hierarchical analysis of variance (Oliver and Webster, 1987; Badr et al., 1993; Oliver and Badr, 1995). The reconnaissance variogram from a nested survey and the variogram of regionalized variable theory can indicate which approach to prediction would be suitable. Values can be estimated for points or blocks by kriging, which is essentially a method of weighted moving averages of the observed values of a property in a given neighbourhood, N. For a regionalized variable, Z, with measured values zxi at points xi , i 1; 2; . . . ; n, the equation for ordinary kriging is ^ B Z
N X i1

li 1:

The Lagrange multiplier, c, is introduced to achieve minimization. Eq. (8) are the kriging equations which are solved to determine the weights, which are then substituted in Eq. (6) for estimating ZB. They also enable the kriging variance to be estimated by ^ 2 B s
N X i1

li  gB; B: gxi ; B c 

The estimation variances can be mapped in the same way as the estimated values and they provide a guide to the reliability of the estimates. The application of geostatistics to explore spatial structure in soil Rn is illustrated using the data from three surveys undertaken near to the places in Fig. 1. The surveys were done in July and August in 1992, 1994 and 1995 during periods of dry and settled weather.

li zxi ;

where Z(B) is the value estimated for a block B, and li are the weights assigned to the sampling points in the search neighbourhood, and N is usually 1625. The kriging weights sum to one to ensure that the estimates are unbiased. The method is also optimal in the sense that the weights are chosen to minimize the estimation or kriging variances, given by ^B EfZ ^B ZB2 g 2 varZ
N X N X i1 j 1 N X i1

li  gxi ; B 7

li lj gxi ; xj  gB; B;

where gxi ; xj is the semivariance of Z between the ith and the jth sampling points,  gxi ; B is the average

Fig. 1. Map showing location of case study sites in England.

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5. Derbyshire: nested survey The nested survey in Derbyshire followed a similar survey near Hereford in the English Midlands on a single geological formation, the Old Red Sandstone of Devonian age (Oliver and Badr, 1995). Although the latter covered a wide range of sampling distances, from 10 m to 7.5 km, all of the variation appeared to occur over distances less than 10 m. The results suggested that there was no spatial structure in the variation, and that the Rn measurements were uctuating randomly about the mean. Since the survey was on a single geological formation, it seemed that lithology was exerting the major control on soil Rn concentration. Therefore, mean Rn concentration for that lithology was a suitable predictor. Furthermore, methods of interpolation including kriging could not be used for prediction with

these data because they were not spatially dependent. Another survey in the English Midlands with samples every 20 m along a transect near Nottingham (Oliver and Badr, 1995) also suggested that lithology accounted for all of the spatially dependent variation. A conventional variogram was computed from the Rn concentrations and this showed some spatial structure. However, when the eect of the dierent lithologies was taken into account, the variogram computed on the residuals from the class means was pure nugget. This indicated that there was no spatially dependent variation remaining within the lithological units. Again, in this example, estimates based on the within-stratum mean would be the best possible. To determine whether the mean Rn value for a given geological formation was the best predictor in general, another area with two primary rock types was surveyed

Fig. 2. Map showing location of nine main centres (IIX) of nested survey to measure soil radon near Buxton (Derbyshire, England), and solid geology of region.

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to the southeast of Buxton. This area has been declared a Radon Aected Area by the NRPB (1992) because >1% of homes have Rn levels greater than the British Governments recommended Action Level of 200 Bq m3. The predominant lithologies (Fig. 2) are both marine limestones of Carboniferous age, the Bee Low formation and the Monsal Dale limestone (Aitkenhead et al., 1985). The Bee Low limestone is fairly homogeneous and has limited faulting, whereas the Monsal Dale limestone is much more variable, fossiliferous, and more intensively faulted. There is also a small area of the Longnor sandstone in the southwest of the region (Fig. 2). The igneous outcrop did not fall within the nested sampling scheme.

total variance
2 2 2 s2 s2 1 s2 s3 sm :

11

A further advantage of the nested approach became clear when Miesch (1975) showed that, if the components of variance are accumulated, starting with the smallest spacing, they were equivalent over the same range of distances to the semivariances of regionalized variable theory, Eq. (5). For m stages of subdivision and distances d1, d2, . . . , dm, where d1 is the shortest distance at the mth stage and dm the largest distance at the rst stage, the equivalence is given by s2 m gd1 ;
2 s2 m1 sm gd2 ;

5.1. Theory of nested sampling Youden and Mehlich (1937) devised a means of determining the spatial scale of variation over several orders of magnitude simultaneously by adapting classical multi-stage sampling. They showed that dierent distances between sampling points could represent the stages in the hierarchy for a spatial property. The underlying theory is that a single-observation embodies variation contributed by each of the distances, including an unresolved variance for the smallest spacing. The contributions of each stage or sampling distance to the total variance can be determined by a hierarchical analysis of variance. The components of variance for each spacing from this analysis reveal over what part of the spatial scale most of the variation occurs. The advantage of this method is that several orders of magnitude of spatial scale can be covered in a single analysis. Since the eects of distance are assumed to be random, the appropriate model of the analysis of variance is Model II of Marcuse (1949). For a design with m stages the model of variation is zijk...m m Ai Bij eijk...m ; 10

2 2 s2 m2 sm1 sm gd3 ;

12

and so on. The values g(di) are the equivalent semivariances. In practice, the components are only rough estimates of the true semivariances because there are too few degrees of freedom from which to estimate each component. Nevertheless, the set of values provides a rst approximation to the variogram, and a rough description of the way a property varies with increasing separation in a given region. It can indicate the range of spatial scales over which most of the variation is occurring, and therefore, is an ideal reconnaissance tool for discovering the approximate spatial scale before designing a more detailed survey to estimate the experimental variogram precisely (Oliver and Webster, 1986, 1987) or to plan a routine survey for mapping. 5.2. Unbalanced nested sampling scheme in Derbyshire The area surveyed was to the southeast of Buxton in the county of Derbyshire: the northwestern corner of the grid was at SK 408373 (National Grid reference). The original sampling design of Youden and Mehlich (1937) was fully balanced, which results in a doubling of the sample size for each stage. For a design with many stages, the number of samples soon becomes prohibitively large for a reconnaissance survey. Therefore, an unbalanced nested scheme was adopted, following Oliver and Webster (1986) and Webster and Boag (1992), to achieve greater spatial resolution without increasing sampling excessively. Full replication at each stage is unnecessary because the mean squares for the lower stages are estimated much more precisely than those for the higher stages. Therefore, economy can be achieved by replicating at only a proportion of the sampling sites. Sacricing the balance, however, means that estimation of the components is somewhat more complex. Gower (1962) and Gates and Shiue (1962) have provided computational procedures for calculating the

where zijk...m is the value of the mth unit in . . ., in the kth class at stage 3, in the jth class at stage 2, and in the ith class at stage 1. The general mean is m; Ai is the dierence between m and the mean of class i at the rst stage; Bij is the dierence between the mean of the jth subclass in class i and the mean of class i; and so on. The nal quantity eijk...m represents the deviation of the observed value from its class mean at the last stage of subdivision. The quantities Aij , Bij , Cij ; . . . ; eijk:::m are assumed to be independent random variables associated with stages 1, 2, 3, . . . , m, respectively, having means of 2 2 2 zero and variances s2 1, s2, s3, . . . , sm. The latter are the components of variance for each stage. The individual component for a given stage measures the variation attributable to that stage, and together they sum to the

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coecients for an unbalanced design (see Webster and Oliver, 1990 for more detail). The unbalanced nested sampling design used had seven stages, and covered an area of 56.25 km2. Nine main centres (IIX in Fig. 2), 3.75 km apart, formed the nodes of a square grid, aligned with the National Grid. Three of the main centres were on the Bee Low limestone, ve were on the Monsal Dale limestone, and one was on the Longnor Sandstone (Fig. 2). The 12 samples associated with each centre were on one of the main lithologies, so that the eect of lithology on Rn concentration could be assessed. The sampling intervals were in a four-fold geometric progression at intervals of 3750, 950, 240, 60, 15, 4 and 1 m. From the nine main centres all of the other points in the scheme were then located on random orientations as follows. A second site was placed 950 m away to provide the second stage. From each of these 18 sites another point was located 240 m away (stage 3). At stage 4 a sample was placed 60 m away from just half of stage 3 sites. This procedure of replicating just half of the sampling points was repeated for stages 5, 6, and 7 at distances of 15, 4, and 1 m, respectively. Fig. 3 shows a plan of the sampling points for one of the main centres. There were 108 sampling sites in total, whereas a fully replicated nested survey would have resulted in 576 sampling points.

5.3. Analysis and results Considerable dierences in Rn concentrations were observed for each centre. For example, for Centre I the smallest value measured was 2.3 kBq m3 and the largest was 40.0 kBq m3. The overall minimum and maximum were 1.3 and 50.3 kBq m3, respectively, which is a dierence of almost two orders of magnitude (Table 1). Clear dierences were also observed between the mean Rn concentration for the Bee Low limestone of 10.1 and of 22.9 kBq m3 for the Monsal Dale limestone. The centre on the Longnor sandstone had the smallest mean concentration of 5.4 kBq m3. However, Rn values for this centre were similar to those of the centres on the Bee Low limestone. The overall average Rn concentration for this survey was 17.4 kBq m3 (Table 1) which is considerably greater than the national average of approximately 10 kBq m3. A study by OConnor et al. (1992) in Ireland has also shown large Rn concentrations over Carboniferous limestone. Although carbonate rocks generally contain small concentrations of U and Ra (of the order of a few parts per million) they are prone to dissolution (karstication) by circulating ground waters which enhances the permeability of the rock and enables Rn to move through it readily. The histogram of the Rn concentration for the Buxton survey was bimodal, which suggested that it was reasonable to combine the Longnor sandstone samples with those of the Bee Low limestone. The components of variance for Rn were determined by a hierarchical analysis of variance (see Webster and Oliver, 1990). An extra stage was incorporated in the analysis to represent the two main lithologies. Table 2 gives the sampling intervals for each stage in the survey, the components of variance, and the percentage variance explained. The components of variance were accumulated starting at the lowest stage, and plotted against distance on a logarithmic scale to give the reconnaissance variogram, the solid line in Fig. 4. There is virtually no residual variance, which suggests that samples separated by 1 m are very similar. From this it was also reasonable to assume that little of the variance is attributable to measurement error. Spatial dependence is evident in the
Table 1 Summary statistics for nested survey in Derbyshire, England Statistic Number of observations Mean Median Minimum Maximum Variance Standard deviation Skewness Radon (kBq m3) 106 17.36 16.75 1.30 50.30 124.08 11.14 0.634

Fig. 3. Spatial conguration of twelve sampling points for one of nine centres of nested survey, Buxton (Derbyshire, England).

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Table 2 Components of variance and percentage variance contributed by each stage from nested survey of soil radon near to Buxton (Derbyshire, England) Stage in hierarchy 1 2 3 4 5 6 7 8 Sampling distance (m) lithology 3750 950 240 60 15 4 1 Degrees of freedom 1 7 9 17 17 18 18 18 Components of variance 97.28 12.76 4.08 50.03 19.18 15.43 35.53 4.11 Accumulated components 173.9 75.60 89.35 93.43 43.40 24.22 39.64 4.11 Percentage variance explained 46.27 0 0 28.77 2.16 0 20.43 2.36

The nested survey suggests that, although geology exerts a major control on the spatial variation of soil Rn concentration, there is spatially dependent variation remaining within the lithological units. This residual variation was explored in more detail by sampling only the Monsal Dale limestone to estimate Rn concentration by kriging, as suggested by Voltz and Webster (1990).

6. Derbyshire: the two-dimensional survey The 2-D survey to measure soil Rn concentration covered an area of 4 km2 near Biggin (National Grid reference SK 415535945, see Fig. 5), south of the area of the nested survey. The spatial information from the nested analysis was used to choose an appropriate sampling scheme. Ideally, sampling on a grid is preferred for local estimation, but in this survey it was irregular to provide some closely spaced samples for computing the variogram as precisely as possible at the shorter separating distances and to comply with the farmers needs. The sampling interval varied from 50 to 250 m, which was well within the extent of spatial dependence indicated by the reconnaissance variogram (Fig. 4). Fig. 5 shows the locations of the 93 sampling points, the relief, roads, mineral deposits and main faults. The sampling points are fairly evenly spread over the area while ensuring that there would be enough pairs of comparisons at the shorter lags. The eld and laboratory procedures were the same as for the nested survey for determining the Rn concentrations. The particle size distribution (psd), which aects porosity and therefore the diusion of Rn through the soil, was determined in the laboratory from a sample of soil taken at a depth of 50 cm at each location. The soil was sieved and the ne fraction (52 mm) was dispersed in water containing Calgon. The proportions of sand silt and clay were then determined by settling (Klute, 1986). Elevation was also recorded at the sites where Rn was measured.

Fig. 4. Accumulated components of variance plotted against distance on logarithmic scale for soil radon concentration near to Buxton (England): solid line is for raw data and dotted one is for residuals computed from means of lithologic units.

variation of soil Rn concentration between 1 and 4 m, this stage accounts for 20% of the variance. Almost 29% of the variance is accounted for by variation over distances of 60 and 240 m, but just over 46% is accounted for by dierences in lithology. This analysis shows that the underlying geology exerts a strong control on concentrations of Rn in soil gas. However, the reconnaissance variogram also suggests that there is spatial dependence within the lithological units. To determine whether this relates entirely to the underlying geology, the components of variance were also computed from the residuals from the means of the two main lithologies. The reconnaissance variogram of the residuals is the dashed line in Fig. 3. It shows that there is still strong spatial dependence over distances less than 4 m and between 60 and 950 m, but that there is now no contribution to the variance by the stage representing the lithologies.

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Fig. 5. Map showing locations of sampling points for survey in two dimensions near to Biggin, Derbyshire (England), together with relief, roads, faults and geology.

6.1. Variogram analysis and results The summary statistics of the properties for the 2-D survey and their correlations are given in Tables 3 and 4, respectively. The observed correlations are generally fairly weak: the largest are between silt and clay, sand and silt, and Rn and elevation. Radon concentration was slightly skewed and the experimental variogram was computed conventionally from the raw data and the logarithmically transformed values using the standard formula: ^ gh 1 X zxi zxi h2 ; 2M h i1
M h

13

the lag by both distance and direction so that there was a range in each which was applied to a nominal lag at the centre of the range (Webster and Oliver, 1990). The experimental variograms from the raw and transformed values were similar and so the raw data were used for further analyses. Fig. 5 shows the experimental semivariances as discrete points. A mathematical model was tted to these values by weighted least-squares approximation using Genstat (Genstat 5 Committee, 1993). A power function, shown as the solid line in Fig. 5, provided the best t and its parameters are given in Table 4. The equation for the isotropic power function is gh c0 wha ; 14

where M(h) is the number of comparisons made at lag h. Since the data were irregularly distributed in two dimensions, the lag interval was determined by grouping

where w is the slope of the line, h is the lag, a is the exponent, and c0 is the nugget variance (i.e. the spatially uncorrelated variation at the scale of the investigation).

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Table 3 Summary statistics for survey on single lithology in two dimensions in Derbyshire Statistic Number of observations Mean Median Minimum Maximum Variance Standard deviation Skewness Radon (kBq m3) 93 13.03 11.27 2.78 35.11 57.67 7.59 1.11 Elevation (m) 93 327.7 328.0 293.0 379.0 657.4 25.64 0.272 Clay (%) 87 19.64 18.80 2.10 39.67 64.34 8.02 0.232 Silt (%) 87 66.68 68.98 11.40 95.90 129.4 11.38 1.58 Sand (%) 87 13.49 11.72 0.62 54.99 81.33 9.02 2.25

Table 4 Correlation matrix computed from data values of properties measured in two-dimensional survey in Derbyshire Variable Radon Elevation Sand Silt Clay 1.000 0.299 0.034 0.118 0.139 Radon 1.000 0.062 0.167 0.319 Elevation Correlations

1.000 0.670 0.107 Sand

1.000 0.639 Silt

1.000 Clay

The nugget variance encompasses spatially dependent variation over distances less than the shortest lag, measurement error, and any purely random variation. The nugget variance for this survey accounts for about 70% of the total variance encountered, which indicates that there is a large locally erratic component in the variation. The monotonically increasing section of the variogram represents the continuous component of the variation. The variogram is unbounded as might be expected for a single lithology. Variograms were also computed for elevation, and the particle size fractions. The former showed evidence of trend, which was removed by a linear function of the coordinates. The variogram was then computed from the residuals and tted by an exponential model; its parameters are given in Table 4. The equation for the exponential function is gh cf1 exph=d g; 15

parameters of these models. The variogram for sand could not be modelled satisfactorily.

6.2. Kriging results Radon concentration was estimated at the nodes of a 50 m grid and over blocks of 50 m 50 m using the variogram model and the data. The grid size for interpolation was based on the suggestion by Webster and Oliver (1990) that the grid should represent a mesh of about 2 mm on the nished map. The block size was chosen so that the eect of the large nugget variance was removed from the estimates which ensured that the regional pattern in the variation would be evident. The block kriged estimates were contoured to produce the map in Fig. 7a. Fig. 7b is the map of the standard errors which reects the distribution of the sampling points: the errors are smallest in three patches where there were small clusters of points and largest near to the edges of the region. Fig. 7a shows that there is fairly continuous change in the values over the area as one should expect with an unbounded variogram. It might also be a reection of the eect of sampling on a single lithology. The Rn 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 variation is particularly distinctive because the Rn concentration appears to be inversely related with the relief (Fig. 5).

where c is the spatially dependent component and d is the distance parameter. The exponential model reaches its sill asymptotically, therefore there is no absolute range or limit of spatial dependence. A working range, a, can be obtained as 3d, which is just over 1 km. Fig. 6b shows the experimental variogram with the tted model. The experimental variograms for the particle size fractions are erratic, possibly because there are too few sample locations. The variograms for clay and silt, Figs. 6c and d, respectively, were tted by power functions as for Rn concentration. Table 4 gives the

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Fig. 6. Variograms for Biggin, Derbyshire: (a) radon concentration; (b) residuals from trend for elevation; (c) percentage clay; (d) percentage silt. Symbols are experimental semivariances and solid line is tted model in each case.

Elevation was kriged using the variogram of the residuals from a linear trend and the residuals themselves. The linear trend function was then added back to the estimates of the residuals for mapping. Fig. 8 shows that there is a general decrease in the height of the land from east to west. There is a spur in the central part of the map anked by two small dry valleys. The inverse relation between elevation and Rn concentration is striking visually, yet the correlation coecient between the raw values is weak (Table 4). To assess this relation further, the kriged estimates of Rn were plotted against those of elevation (Fig. 9a). A negative relation is evident, but it appears to be non-linear. The correlation coecient between the kriged estimates of Rn and elevation is larger (Table 5). The dierence between the correlation coecients in Tables 4 and 5 probably arose because of the locally erratic variation in Rn concentration. Block kriging removed these local sampling eects in the estimates, and the correlation is more apparent for these than for the raw data.

Figs. 10a and b show the contour maps of the kriged estimates of clay and silt contents for the area. There also appears to be a relation between clay content, Rn concentration, and elevation: clay content is least in the west and northwest of the study area and greatest on the plateau and spur in the east. This observation is supported by the correlations between elevation and clay content for both the raw data (Table 4) and the kriged estimates (Table 5), which show a stronger relation. The scatter diagram of the kriged estimates of clay against elevation (Fig. 9b) shows a weak negative relation. The correlations between silt and elevation (Tables 4 and 5) and the scatter diagram of the kriged estimates (Fig. 9c) suggest little relation between silt content and elevation. Nevertheless, silt content in the soil is also least in the west and northwest, but it is greatest at the foot of the slope from the plateau and along the dry valleys. The relations between Rn and the particle size fractions need to be examined further, as does the mineralogy of the soil.

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Fig. 7. (a) Map of kriged estimates of radon concentration near to Biggin, Derbyshire (England), and (b) map of standard errors for kriging.

7. Derbyshire: the transect survey The map of Rn concentration (Fig. 7a) shows that there are factors other than the underlying geology that

account for its spatial variation since this survey was on a single lithology. A transect survey was carried out to gain further insight into the relation between elevation, soil depth, and Rn concentration. Since supercial

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Fig. 8. Map of kriged estimates of elevation, near to Biggin, Derbyshire (England).

materials move down slope, it is possible that there might be a relation between elevation and depth to the limestone bedrock. Such a relation would support Jones (1995) hypothesis that Rn emanation is primarily a function of nely disseminated U in the soil. Therefore, one might expect that thicker soil would contain more U resulting in greater Rn emanation. The transect extended for 2 km from east to west at grid reference SK 160587 (Fig. 5), with Rn measurements made at an interval of 20 m. Slope angle was also measured between the mid-sample positions on either side of the sampling point, and soil depth was measured electromagnetically. 7.1. Ground conductivity measurement Electromagnetic techniques can be used for geological mapping and groundwater surveys (McNeill, 1980). The continuous wave technique was used which measures the resultant of the primary and secondary elds using a continuous time-varying magnetic eld. The ratio of the secondary eld (Hs) to the primary eld (Hp) is linearly proportional to the terrain conductivity, which can be determined by direct measurement. The apparent conductivity (sa) is given by the relation sa 4=$mo s2 Hs =Hp ; 16

intervals by a continuous electromagnetic wave using the Geonics EM31 equipment. 7.2. Results of transect survey Radon concentration is plotted against sample spacing in Fig. 11a. The plot shows that the values are very irregular, but it is possible to identify a weak trend of decreasing values from west to east. Table 7 gives the summary statistics for Rn concentration along the transect. These data are skewed, so they were transformed to logarithms before computing the variogram. The experimental variogram, shown by the symbols in Fig. 11b, has a sinusoidal form. A combined periodic model with power function was tted. The parameters of the best-tting model are given in Table 8, and its equation is gh c0 a sin2ph=l b cos2ph=l wha 17

where $=2pf, and f is the frequency (Hz), mo is the permeability of the free space, and s is the intercoil spacing (m). Ground conductivity was measured at 20 m

in which the parameters a and b determine the amplitude and the phase of the wave, and l is its wavelength. Ground conductivity measurements were also plotted against sampling position (Fig. 12a). There is a weak trend from west to east with conductivity values decreasing. This suggests that the soil is deeper in the west than in the east. The peaks in the conductivity values along the transect can be explained in several ways. Conductivity can vary because the soil and supercial materials are not homogeneous. Highly conductive man-made objects, such as pipes, might be

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Fig. 9. Scatter plots of (a) radon concentration against elevation; (b) radon concentration against percentage clay in soil; (c) radon concentration against percentage silt in soil; (d) percentage clay content in soil against percentage silt.

Table 5 Correlation matrix computed from kriged estimates for radon, elevation, silt and clay from two-dimensional survey in Derbyshire Variable Radon Elevation Silt Clay 1.000 0.776 0.338 0.630 Radon Correlations 1.000 0.236 0.636 Elevation

1.000 0.740 Silt

1.000 Clay

present, but this seems unlikely in elds. Another possibility is that the peaks might reect the underlying karst topography of the Carboniferous limestone. The joints of this rock have been widened and deepened by solution, and have been lled subsequently with soil or sediments, which have a greater conductivity than the rock. This last explanation is favoured. Table 5 gives the summary statistics of the conductivity measurements, which were transformed to logarithms before computing the variogram because of the

large skewness value. The experimental variogram of the transformed conductivity measurements (Fig. 13) suggests that the variation is periodic, as was the case for the Rn concentration. It was tted best by a combined periodic and power function (Eq. (17)). The wavelength of the model is 182.6 m, which is shorter than that of the model tted to the variogram of Rn (Table 6). The experimental variogram of slope angle (Fig. 13) was also tted by a combined periodic and power function. It has a wavelength of 171.4 m which is close to that of conductivity (Table 6). The slope angle possibly reects weak terracing along the transect that might be associated with the major joint pattern in the Carboniferous limestone. The relation between the wavelengths of the variograms and features of the Carboniferous limestone, such as dolines, needs to be explored further.

8. Discussion and conclusion The results described here suggest that geology is the major factor controlling the spatially dependent component of the variation in soil Rn concentration. This

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Fig. 10. Map of kriged estimates of (a) percentage clay, (b) percentage silt near to Biggin, Derbyshire (England).

has been suggested by others such as Ball et al. (1991), but we have been able to quantify and illustrate this eect. The results also suggest that, in some areas, factors other than geology can account for a substantial proportion of the spatial variation in Rn. When the eects of geology were removed for the nested survey,

there was still evidence of spatially dependent variation. This situation is likely to result in a spatially correlated component of variation as well as a locally erratic one within lithological units. Radon varies considerably and unpredictably over distances of a few metres, which results in the large nugget variances of the

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Table 6 Variogram model parameters for properties measured in two-dimensional survey in Derbyshire Variable Radon Elevation (residuals) Clay (%) Silt (%) Sand Model type Power Exponential Power Power No suitable model tted Nugget variance 46.21 0.0 55.54 326.9 Structured component c 59.52 0.0055 0.0615 1.6219 1.6467 Slope w 0.2604 Exponent a 0.8108 358.68 Distance parameter d

Table 7 Summary statistics for transect survey on single lithology in Derbyshire Statistic Number of observations Mean Median Minimum Maximum Variance Standard deviation Skewness Radon (kBq m3) 86 10.55 10.55 1.780 36.80 29.82 5.461 1.532 Slope angle 86 1.961 2.000 3.000 6.500 3.789 1.947 0.436 Conductivity (mmhos) 86 4.382 4.000 3.000 10.00 1.556 1.248 1.770

Table 8 Variogram model parameters for properties measured along transect in Derbyshire Variable Radon Conductivity Slope angle Model Periodic with power } } Nugget variance 0 0 0 Amplitude 0.0241 0.1738 0.3499 Phase 0.0046 0.0450 0.0455 Wavelength 269.6 182.6 171.4 Slope 0.1607 0.5339 0.3322 Exponent 0.0438 0.0702 0.3749

experimental variograms of the 2-D and transect surveys. This supports the ndings of Reimer and Gundersen (1989) that homes only 100 m apart had Rn values that diered by two orders of magnitude. The 2-D survey near Biggin on the Monsal Dale limestone showed that it was feasible to estimate Rn values by kriging within the lithological units, as Voltz and Webster (1990) suggested. The results of estimating and mapping Rn concentration led to an examination of the variation in elevation and particle size distribution, which appear to be related to Rn concentration and to each other. The results of the transect survey suggest that Rn concentration is also related to the variation in soil depth and this, in turn, might be associated with the underlying karst topography and fracture patterns of the limestone which allow supercial materials to accumulate. These might have been derived from overlying rocks, such as the black shales, that were

richer in U than the limestones. This requires further investigation. From this study the procedure recommended for estimating Rn is rst to stratify the area on the basis of lithology and then determine whether geology accounts for all of the spatially dependent variation using the variogram of the raw data and that of the residuals. If so, then sampling should be optimized to estimate the mean Rn concentration within the geological units. If there is spatial dependence remaining within the classes, then sampling should be optimized for kriging, which will provide reliable estimates of Rn concentration with known error within strata. Reliable estimates of Rn and of the risk of developing diseases are vital to establish meaningful correlations between Rn concentration and radiation-related illnesses in specied regions. They are also important for locating new houses, for building practices, and for

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Fig. 11. (a) Radon concentrations plotted against sampling position along transect (Fig. 4) near to Biggin, Derbyshire (England), and (b) variogram of radon concentration for transect: symbols are experimental semivariances and solid line is tted model.

Fig. 12. (a) Conductivities plotted against sampling position along transect (Fig. 4) near to Biggin, Derbyshire (England), and (b) variogram of ground conductivity for transect: symbols are experimental semivariances and solid line is tted model.

ameliorating the eects of Rn in existing properties. The information required can be obtained by choosing a suitable sampling scheme and an appropriate method of prediction. These considerations are vital when planning large-scale geochemical surveys because of the associated costs.

Acknowledgements We thank Professor R. Webster for the use of software, Dr S.A. Durrani for advice on Rn monitoring, and the referees for their helpful recommendations.

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