Environ Geol (2009) 56:15331549
DOI 10.1007/s00254-008-1252-x
ORIGINAL ARTICLE
Radon concentrations in soil gas, considering radioactive
equilibrium conditions with application to estimating
fault-zone geometry
Katsuaki Koike Tohru Yoshinaga
Hisafumi Asaue
Received: 12 November 2007 / Accepted: 11 February 2008 / Published online: 22 April 2008
Springer-Verlag 2008
Abstract A calculation method for determining the
amount of Rn isotopes and daughter products at the start of
measurement (CRAS) is proposed as a more accurate
means of estimating the initial Rn concentration in soil gas.
The CRAS utilizes the decay law between 222Rn and 220Rn
isotopes and the daughter products 218Po and 216Po, and is
applicable to a-scintillation counter measurements. As Rn
is both inert and chemically stable, it is useful for fault
investigation based on the soil gas geochemistry. However,
the total number of a particles emitted by the decay of Rn
has generally been considered to be proportional to the
initial Rn concentration, without considering the gas con-
dition with respect to radioactive equilibrium. The CRAS
method is shown to be effective to derive Rn concentration
for soil gases under both nonequilibrium conditions, in
which the total number of decays increases with time, and
equilibrium conditions, which are typical of normal soil
under low gas flux. The CRAS method in conjunction
with finite difference method simulation is applied to
the analysis of two active fault areas in Japan, and it is
K. Koike (&)
Graduate School of Science and Technology,
Kumamoto University, 2-39-1 Kurokami,
Kumamoto 860-8555, Japan
e-mail: asaue-h@aist.go.jp
T. Yoshinaga
Technical Division, Faculty of Engineering,
Kumamoto University, 2-39-1 Kurokami,
Kumamoto 860-8555, Japan
H. Asaue
Institute for Geo-Resources and Environment,
Geological Survey of Japan, AIST, 1-1-3 Higashim Tsukuba,
Tsukuba, Ibaraki 305-8567, Japan
demonstrated that this combination could detect the sharp
rises in 222Rn concentrations associated with faults. The
method also allows the determination of fault geometry
near the surface based on the asymmetry variation of the
Rn concentration distribution when coupled with a
numerical simulation of 222Rn transport. The results for the
new method as applied to the two case studies are con-
sistent with the data collected from the geological survey.
It implies that the CRAS method is suitable for investi-
gating the fault system and interstitial gas mobility through
fractures. The present analyses have also demonstrated that
high Rn concentrations require the recent and repeated
accumulation of 222Rn parents (230Th and 226Ra) in fault
gouges through deep gas release during fault movement.
Keywords Radon-222
a-scintillation counter

Radioactive equilibrium
Active fault
Fault geometry

Finite difference method
Introduction
The radon concentration in soil gas and groundwater is an
effective indicator of subsurface gas and water flows
related to geologic structures (Chung 1981; Gingrich
1984; Nielson et al. 1984; Lindmark and Rosen 1985; Ball
et al. 1991; Torgersen and ODonnell 1991). Mercury,
hydrogen, helium, methane, and carbon dioxide have also
been utilized in this type of flow analysis (e.g., Sorey et al.
1993; Heinicke et al. 1995; Sugisaki et al. 1996). The
prevalent use of Rn as an indicator is attributable to the
fact that Rn is chemically inert, not organic (compared to
CH4 and CO2), soluble in water, and naturally occurring as
a radioactive gas. Furthermore, Rn can be detected at
extremely low concentrations. The numerous applications
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of Rn in geological analyses can be classified into four
major categories: detection of latent faults (Duddridge
et al. 1991; King et al. 1996; Ciotoli et al. 1998), explo-
ration of uranium deposits (Miller and Ostle 1973; Smith
et al. 1976), clarification of relationship between Rn
concentration and volcanic eruptions (Chitkov 1975;
Gasparini and Mantovani 1978; Toutain et al. 1992), and
detection of precursory and coseismic phenomena
accompanying earthquakes (Hauksson 1981; Virk and
Singh 1994; Heinicke et al. 1995; Igarashi et al. 1995;
Tsunogai and Wakita 1995; Chyi et al. 2002).
In these applications, the Rn concentration in soil gas
and groundwater is measured by a-track, a-scintillation,
and ionization chamber methods for gaseous Rn, and by a
liquid scintillation counter method for dissolved Rn in
fluids. The a-scintillation counter method is the most
suitable method for in situ measurement, as it does not
require chemical processing such as etching (required for
the a-track method) and measurement can be completed
quickly. Detailed mapping of Rn concentrations is there-
fore possible by setting a short distance between adjacent
sample points. Rn isotopes, 222Rn and 220Rn that are pro-
duced in the decay series of uranium and thorium,
respectively, are the isotopes measured in such analyses,
considering the half-life and abundances of the Rn iso-
topes. Another advantage of the a-scintillation counter
method is its ability to separate the total decay numbers
into those originating from 222Rn and 220Rn by virtue of the
large difference in half-lives, 3.58 days for 222Rn and 53 s
for 220Rn. Thus, 222Rn concentrations also provide infor-
mation on soil-gas conditions in a wider area through
longer migration.
In most researches based on a-scintillation counter
measurements, however, the radioactive equilibrium con-
dition of Rn gas is not considered, and the decay number is
regarded as being equivalent to the true (initial) Rn con-
centration. The measurement time adopted in the method is
typically 3 min, which is too short to correctly judge
whether the Rn gas is in equilibrium. In order to deal with
this problem, a calculation method is proposed in this study
for determining the initial 222Rn and 220Rn concentrations
based on the decay law between the two nuclides and their
daughters. The effectiveness of the method is evaluated
based on the correspondence between estimated high 222Rn
concentrations and faults locations, and the spatial corre-
lation structure of concentrations around the faults. The
spatial distribution of 222Rn concentration is demonstrated
to be useful for elucidating fault configurations with
respect to width and orientation in two active fault areas in
Japan. A numerical simulation is also performed using a
finite element method to examine the transport of 222Rn in
shallow soils for combination with fault shape estimation.
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Environ Geol (2009) 56:15331549
Estimation of initial Rn concentrations in soil gas
Fundamental equations
A RDA-200 detector (Syntrex Inc.) was used in the initial
Rn survey to detect the a particles emitted by the a decay
of 222Rn, 220Rn, 218Po, and 216Po (218Po and 216Po are the
daughter nuclides of 222Rn and 220Rn, respectively). A hole
of 65 cm in depth and 3 cm in diameter was dug into the
soil at the study site and sheathed with vinyl chloride
piping. Soil gas was then sampled by a hand pump into a
cell of 160 cm3 in volume. The internal surface of the cell
had a scintillator coating of ZnS (Ag). The number of a
particles emitted per minute was measured by the detector,
and the data were subsequently corrected by subtracting the
background due to residual Rn in the cell. The cell was
exchanged when the background values became too large.
The total net numbers of a particles in each minute of
the first 3 min are denoted by D1 (01 min.), D2 (1
2 min.), and D3 (23 min.). According to the empirical
equation by Morse (1976) obtained by RDA-200 for
treating the data, the total number of a particles,
D1 + D2 + D3, is divided into the two decay quantities
D222Rn and D220Rn as follows:


D222 Rn 0:868D3 0:317D2  0:339D1
1
D220 Rn D1 D2 D3  D222 Rn
D222Rn and D220Rn have generally been assumed to rep-
resent the initial Rn concentrations in fault surveys using
the RDA-200 (e.g., Yamaguchi et al. 1984; Sugiyama et al.
1986; Duddridge et al. 1991; Ciotoli et al. 1998). Despite
such prevalent usage, the equation does not consider the Rn
gas condition with respect to radioactive equilibrium. The
coefficients in Eq. (1) must be changed for nonequilibrium
conditions, as the sum of the decays of Rn and its daughters
increase with time under the nonequilibrium condition but
remains constant with respect to the ratio of 222Rn and
218
Po decays in equilibrium.
To overcome this problem and estimate the Rn con-
centration directly, a calculation method is proposed to
determine the numbers of Rn isotope atoms and daughters
at the start of measurement (termed as CRAS: calculation
method of numbers of Rn isotope atoms and their daugh-
ters at the start of measurement). As the half-life of 222Rn is
6,000 times longer than that of 220Rn, CRAS attaches great
importance to the radioactive equilibrium relationship
between 222Rn and 218Po. Expressing the time at which the
Rn gas was generated as t = 0, the number of 222Rn and
218
Po isotopes at t = 0 is denoted by N0. The soil gas is
sampled at a time T (s) from t = 0, and represents the age
of the Rn gas. The number of 222Rn, 218Po and 220Rn
isotopes at the start of measurement (t = T) is denoted by
Environ Geol (2009) 56:15331549 1535

N222, N218, and N220. The time at which 222Rn and 218
Po Vk Vk222 Vk218 Vk220


reach equilibrium is given by k222 Dt  exp k218 sk1 exp k218 sk
    k222 2Dt N222
1 k222 k218  k222
teq log 1980s 2 fexp k218 sk1  exp k218 sk gN218
k222  k218 k218
2fexp k220 sk1  exp k220 sk gN220 7
Here, k 222 and k218 are the decay constants of 222Rn,
and 218Po. If T is shorter than teq, N222 and N218 can be The unknown N222, N218, and N220 can be calculated from
obtained from the law of radioactive decay as follows: Vk and Eq. (7) by a least-squares method, allowing T to be
9 estimated from Eq. (4).
N222 N0 expk222 T >
>
>
> When T is not determined, the Rn gas is assumed to
k222 >
=
N218 N0 fexp k222 T  exp k218 T g have reached radioactive equilibrium at the start of mea-
k218  k222 surement. In this case, the relation
  >
>
dN218 >
>
* k222 N222  k218 N218 >
; N218 rN222 8
dt
3 holds, and Vk(218) is expressed by
Vk218 r 1Vk222
From the above two equations, T can then be expressed
by r 1N222 fexp k222 sk1  exp k222 sk g

9
1 Rk218  k222
T log 1  4
k222  k218 k222 where r = k222/k218. Finally, in the case of T [ teq, Vk can
be summarized by
where R = N218/N222. It is necessary that R should be
smaller than k222/(k218 k222) = 5.45 9 10-4 from the Vk 2 r fexp k222 sk1  exp k222 sk gN222
equilibrium condition. In the case where T is greater than 2fexp k220 sk1  exp k220 sk gN220 10
teq, the value of T cannot be determined because R takes a
constant value of 5.45 9 10-4. N222 and N220 can also be obtained by a least-squares
If the time difference between the start time and each analysis of Vk.
minute of measurement is denoted by sk = kDt (k = 1,...,n;
n is the number of measurements and Dt = 60 s is the time Confirmation of CRAS applicability
interval), the number of 222Rn and 218Po decays between
t = T + sk-1 and t = T + sk for T B teq (Vk(222) and CRAS was tested for soil gases at four sites in the hot
Vk(218), respectively) are approximated by spring areas of Mt. Aso in southwest Japan (see Fig. 2).

9
Vk222 N222 fexp k222 sk1  exp k222 sk g >
>
  >
>
k222 DtN222 *Dt  1=k222 4:83  10 5 >
>
=
k222 5
Vk218 fk222 Dt  exp k218 sk1 expk218 sk gN222 >
>
>
k218  k222 >
>
>
;
fexp k218 sk1  exp k218 sk gN218 k222 DN222

As the half-life of 220Rns daughter, 216Po, is very short
(0.158 s), the number of 216Po decays can be assumed to be
approximately equal to that of 220Rn. The resultant Vk(220)
is given by
Vk220 2fexp k220 sk1  exp k220 sk gN220 6
In measurement, the total number of decays between
t = T + sk-1 and t = T + sk, denoted by Vk (k = 1,..., n),
is counted sequentially. Vk can then be rearranged as
follows:
Three of the sites, of A and B type were sampled near
fumaroles, and the other C type site was located in an area
with no signs of hydrothermal alteration or fumaroles.
Figure 1 shows the temporal change in the total number of
decays per minute over 20 min at the sampled sites. The
soil gases of types A and B are under nonequilibrium
conditions, as indicated by the increase in the total number
of decays over time due to the increase in 218Po decays.
However, the soil gas of type C reaches an equilibrium
condition after the first few minutes, in which total decays

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1536 Environ Geol (2009) 56:15331549

Fig. 1 Typical patterns of total

decay counts per minute over
20 min for three types of Rn
gas. A: radioactive
nonequilibrium condition with
monotonic increase in decay
count, where A-1 gas has longer
apparent life than A-2. B:
nonequilibrium condition with
relatively high abundance of
220
Rn. C: equilibrium condition
in normal soil. Solid line
represents CRAS calculation,
and open circles denote
measurements

decrease due to the decrease in 220Rn decays. This confirms 222

that the 220Rn decay represents a large proportion of the
total decays in gases under equilibrium conditions. Thus,
for the calculation of N222, N218, and N220, Eq. (7) should
be applied to the data of type A and B, and Eq. (10) to data
of type C. Conversely, these parameters can be use to
predict the total decays in each minute using Eq. (7) or
(10).
It is worth noting that the predicted total decays agree
well with the measurement data for all data types, dem-
onstrating the validity of the CRAS approach. The
difference in the temporal changes for gas types A and B
originates from the greater abundance of 220Rn in type B
gas, resulting in a monotonic increasing trend. The type A
gas can be further divided into types A-1 and A-2, which
have different rates of increase after the first few minutes.
The apparent lives are calculated using Eq. (4) to be 102
and 17 s for the A-1 and A-2 data, respectively. The high
rate of increase seen for the A-2 gas reflects the shorter
apparent life.
The total decays of 222Rn and 220Rn in the first 3 min
calculated using both the empirical formula of Eq. (1) and
CRAS are compared in Table 1. Although the sum of the
two total decays obtained by Eq. (1) is almost the same as
that by CRAS, the ratios of 222Rn decays in the summa-
tions differ significantly between the two methods. This
difference can be clearly seen for the decay ratio of
Rn/220Rn, which for gas A-1 is smaller than 0.5, by
Eq. (1) and almost 100 times larger by CRAS. The CRAS
results indicate that most of the decays in nonequilibrium
Rn gas are derived from the decays of 222Rn, whereas the
decays of 220Rn by Eq. (1) make up a larger fraction than
those of 222Rn. For the equilibrium gas C, Eq. (1) is unable
to determine the 222Rn concentration because D222Rn \ 0,
which means that 222Rn is not present in the soil gas. By
CRAS, the decays of 222Rn make up the same proportion of
the total decays as those of 220Rn. Thus, the empirical
formula tends to underestimate the decays of 222Rn and
therefore the abundance of 222Rn in soil gas.
Use of CRAS for detecting faults
Relationship between Rn concentration and faults
The effectiveness of CRAS for geological exploration was
examined by investigating the positional relationship
between Rn concentration and lineaments associated with
the existence of faults by CRAS. The Futagawa fault area
in southwestern Japan was selected for this investigation
(Fig. 2). This 23.5 km-long fault trends eastnortheast to
westsouthwest from the western edge of the Aso caldera
to the lowland in the Kumamoto plain through zones
covered by late Pleistocene Aso pyroclastic flow deposits

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Environ Geol (2009) 56:15331549 1537

Table 1 Total decay counts for 222Rn and 220Rn during the first 3 min for samples described in Fig. 1 under the nonequilibrium and equilibrium
conditions of Rn gas
Condition of Rn gas Nonequilibrium Equilibrium
Gas type A-1 A-2 B C
Calculation method Empirical equation CRAS Empirical equation CRAS Empirical equation CRAS Empirical equation CRAS
222
Decays of Rn (cpm) 1,326 4,373 1,792 5,316 917 2,993 -4 55
220
Decays of Rn (cpm) 3,127 106 4,042 463 2,706 698 140 98
222
Decay ratio Rn/220Rn 0.42 41.3 0.44 11.5 0.34 4.3 -0.03 0.56
222 220
They are calculated as Eq. (1) using the empirical formula and CRAS. The decay ratios of Rn to Rn are largely different between the two
methods, and the empirical formula underestimates 222Rn concentration

(Aso-1, 2, 3, and 4 in ascending eruption order), andesitic
lava (eruptions of lateral craters), and pre-Aso volcanic
rocks (Fig. 3a). Aso-1 is distributed only sparsely around
the fault. According to Watanabe (1984), Aso-4 is com-
posed of unwelded pumice flows containing white bubbly
pumice, and Aso-2 and -3 are composed of weakly welded
scoria flows containing black scoria and volcanic glass.
The ages of Aso-2, -3, and -4 are 140,000, 120,000, and
90,000 years, respectively. These lithologies, the fluvial
terraces, and the Holocene scarps are displaced at several
sites by the Futagawa fault, representing evidence of recent
activity. The Research Group for Active Faults of Japan
(1991) estimates the average displacement velocity of the
fault to be 0.20.5 m/103 years. The Futagawa fault con-
sists of a number of smaller subordinate faults.
Six transects were set north to south across the Futagawa
fault along paths through forests and valleys, with attention
paid to ensure that transects were as straight as possible.

Fig. 2 Location map showing

the positions of transects A, B,
C, and C0 in the Futagawa fault
area, southwest Japan

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1538 Environ Geol (2009) 56:15331549

Fig. 3 a Geological map

produced by Kumamoto
Prefecture and Kumamoto City
(1994). The thick line denotes
the main fault. 1 fault, 2
alluvium, 3 talus deposits, 4
effusive rocks from Aso central
crater, 5 Kugino layer, 6 terrace
deposits, 7 Takayubaru lava, 8
Aso pyroclastic flow deposit, 9
pre-Aso volcanic rocks, 10
Paleozoic and Mesozoic
formations, and 11 metamorphic
rocks. b Arrangement of
transects (bold line), and
lineaments (Kumamoto
Prefecture 1997) associated
with the main fault (gray thick
line), subordinate faults (thin
line), and a latent subordinate
fault (gray broken line)

As the fault runs across the edge of mountains to the south
(Fig. 2), the end points were at higher elevations than the
start points. Data for the three longest of these transects are
reported here to evaluate CRAS with respect to the spatial
correlation between Rn concentrations and fault location.
The results of the entire data set analysis and details of the
measurements are described in Koike et al. (2000). The
three transects, A, B, and C (Fig. 3b), were 380, 380, and
350 m in length, with altitude differences of 28, 33, and
15 m, respectively, between the start and end points. Fig-
ure 3b shows the configuration of the transects. The distance
between adjacent two measurement points was set at 2.5 m
for all transects, giving a total of 153, 153, and 141 mea-
surements points for transects A, B and C. The lineaments
identified by aerial photography (Kumamoto Prefecture
1997) across each transect are depicted in Fig. 3b.
Figure 4 compares the CRAS results for the number of
222
Rn isotopes, N222, with the number of decays, D222Rn,
by Eq. (1) obtained at each location along the transects.
The 90% cumulative frequency of the data for each transect
is shown in Fig. 4 to emphasize the highest 222Rn con-
centrations. Although the general trends in the results by
the two methods are similar, the D222Rn values are nega-
tive at 15 points where the total decays in the first 3 min
was low. The CRAS value, N222, takes clear maximum
values at locations corresponding to the main fault in all
the three transects, whereas the maximum D222Rn values
are located on the subordinate faults or at a distance from
any fault. This difference is most apparent for transect C.
The locations of points characterized by values
exceeding the 90% cumulative frequency level around the
faults are also good indices to compare the two methods.
Five N222 anomalies are located successively or at one
point apart around the main fault on the transect A, while
the D222Rn anomaly points are only two, as shown in
Fig. 4. Although the same number of anomalous values are
recorded around the main fault on transect B, the asym-
metric shape of the 222Rn concentration distribution across
the fault is more evident in the N222 distribution. In this
asymmetry, the 222Rn concentration increases gradually
toward a maximum on the northern side of the main fault,
then drops sharply to the south. On the basis of geological
investigations (Watanabe 1984), the Futagawa fault is
thought to dip northward. This configuration therefore
appears to affect the distribution of 222Rn concentration,
which is consistent with a simple assumption that the
carrier gas velocity and diffusive coefficient of 222Rn in the
fault zone are larger than in the surrounding soil. For
transect C, the N222 results contain more anomalous values
around the faults than the D222Rn results. Thus, the

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Environ Geol (2009) 56:15331549 1539

Fig. 4 Comparison of N222

(lower column) and D222Rn
along transects A, B and C. The
90% cumulative frequency of
data is indicated for each
transect. Arrows indicate the
locations of the main (thick line)
and subordinate (dotted line)
faults, and circled portions are
anomaly concentrations in the
vicinity of the faults

anomalous CRAS values appear to concentrate in the
vicinity of faults, demonstrating the capability of the CRAS
approach for detecting hidden faults.
Another interesting feature is that the three anomalous
N222 values in the vicinity of the main fault on transect B
can be judged to represent nonequilibrium condition.
Although the total decays at most points follow the typical
equilibrium pattern of type-C gas in Fig. 1, gases of types
A and B were detected at the three points around the fault
(Fig. 5). This observation confirms that Rn gas can be in
nonequilibrium without an active rise in carrier gas in such
geothermal areas.
Figure 6 shows the distribution of the ratio of D222Rn to
the total number of decays, D222Rn/(D220Rn + D222Rn)
compared to the normalized N220. These data have also
been used as indices for locating faults (Isra/l and
Bjornssin 1966; Gingrich 1984; Yamaguchi et al. 1984;
Sugiyama et al. 1986; Duddridge et al. 1991). However,
neither measure resolves the locations of faults reliably,
although the N220 data includes strong anomalous values in
the vicinity of the main faults on transect C. Therefore, the
220
Rn concentration is not a suitable universal index for
Rn-based fault investigation.
222
Spatial correlation of Rn concentration

In addition to the above magnitude distribution, it is nec-

essary to evaluate the spatial correlation of the Rn
concentration, representing the randomness or reciprocal
relationship between adjacent points. If the Rn concentra-
tion is entirely random along a transect, then it is
impossible to determine the existence of a fault or the
influence of the fault on the Rn data. The spatial correlation
can be expressed by the semivariogram, c(h), which is a
geostatistical function that takes the data locations into
consideration. The semivariogram is defined in terms of the
variance of a data pair, z(x + h) and z(x), separated by
distance h, as follows:
h i
ch E fzx h  zxg2 =2 11

where z(x) is a data value at location x and E is the

Fig. 5 Total decay count per minute at three points on and around the expectation. In general, the values of regionalized data are
main fault on transect B judged to be under radioactive nonequilib-
rium conditions. The 10 m point is estimated to correspond to the similar within small distances and become different with
main fault distance, which causes an increase in c(h). As the variance

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1540 Environ Geol (2009) 56:15331549

Fig. 6 Distribution of D222Rn/

(D220Rn + D222Rn) ratio (upper
column) and N220 along
transects A, B, and C with the
locations of faults marked by
arrows

becomes small when the data in the pair have similar
values, the distance range in which spatial correlation
exists is found by c(h)
Figure 7 compares the experimental c(h) for the D222Rn
and N222 for the three transects. The two c(h) series are
almost the same for transects A and B, although c(h) for
N222 is slightly smaller than that for D222Rn, representing
better spatial correlation. It is worth noting that both the
c(h) series exhibit periodic behavior, with a half period
seen on transect A, and 1.5 periods on transect B. This may
be related to the existence of two faults (Fig. 3b), indi-
cating that the range of effect on the 222Rn concentration
due to the presence of a fault is approximately 100200 m.
A similar periodic c(h) was obtained for N222 on transect C,
which also crosses two faults and where the range of
influence appears to be 100 m.
To further check the influence of faults, an additional
transect of 100 m in length (C0 ) was set parallel to transect
C, but away from the main fault (Figs. 1, 3b). Transect C0
was located on a gentle grassy slope of weathered volcanic
rock, whereas transect C was located on talus deposits
(Fig. 3a). Figure 8 shows the distribution of N222 along
transect C0 . Although the values do not differ significantly
from those on transect C, a major difference can be seen in
the c(h) analysis. For transect C0 , c(h) does not increase
smoothly even within short distances, and the series takes
almost the same values over distances larger than 15 m. In
contrast, the c(h) series for N222 on the first three transects
take local maximums within 1020 m, become almost flat
for a distance, and then increase again toward regional
maxima (Fig. 7). These characteristics can be explained as
representing a short-range structure for N222 in normal soils
without faults, and a long-range structure when associated
with a fault system. Consequently, faults are confirmed to
be responsible for the spatial correlation of Rn concentra-
tion, and this correlation is more accurately detected by
CRAS than empirical calculations.
Combination of CRAS and finite difference method
for estimating fault-zone geometry
222
Numerical simulation of Rn transport
Another merit of CRAS is the ability to directly apply the
Rn concentration obtained to numerical simulation of Rn

Fig. 7 Comparison of
experimental semivariograms
for normalized D222Rn (broken
lines) and N222 (solid lines) data
along transects A, B, and C

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Environ Geol (2009) 56:15331549 1541

Fig. 8 Distribution of N222

along the transect C0 which does
not cross the Futagawa fault
(left), and comparison of
experimental semivariograms of
N222 data for transects C and C0
(right)

transport in order to estimate geologic structures such as the vertical direction for the surrounding zone. Gas trans-
fault-zone geometries. As indicated by Soonawala and port outside the fault zone is restricted to vertical movement
Telford (1980) and Schery et al. (1984), the Rn concen- only. As a boundary condition, the N222 at the source
tration in shallow soils is generally accepted to be (reference plane of the Rn concentration) in the fault-
controlled by the diffusion of Rn and by the ascent of gas surrounding zone is fixed at 106. The Rn source depth is
carrying Rn. While the diffusion of Rn occurs directly uniformly defined as 20 m parallel to the surface terrain.
upward (positive z direction), a carrier gas may move in The distance between two adjacent grid points is set at
any direction. For analysis of fault-zone geometries, a 0.5 m along both the x and z axes, as shown in Fig. 9. As the
steady-state condition of constant Rn concentration N at values of D and m are small, the depth range that affects the
222
arbitrary depth is assumed, that is, qN/qt = 0. Under this Rn concentration near the ground surface is restricted to
assumption and the conditions of diffusion and advection be shallow. If the source is too shallow, however, the lateral
of Rn, the fundamental equation for Rn concentration in a range of high Rn concentration attributable to the inclina-
two-dimensional regime (e.g., along a transect) can be tion of the fault will become narrow, making it difficult to
expressed by estimate the dip angle. The source depth was set at 20 m
based on these considerations.
o2 N mx oN mz oN k
   N0 12
oz2 D ox D oz D
where D is the diffusion coefficient, mx and mz are the
components of the carrier gas velocity, m, along the x and z
axes (where the x axis is horizontal), and k is the decay
constant of 222Rn. Here, only 222Rn is considered because
the range of 220Rn migration will be small due to its short
half-life.
As it is difficult to analytically solve Eq. (12), the
equation is discretized using a finite difference technique.
With an approximation for the first derivative by spatial
backward difference and gridding over the calculation
regime, Eq. (12) can be replaced by a differential equation,
which can then be used to calculate the 222Rn concentration
at each grid point. This calculation was simplified by
dividing the regime into a fault zone and a surrounding
zone, in which the values of D and m in each zone are
constant. The finite difference method (FDM) simulation
makes it possible to model the fault-zone geometry that has
the greatest effect on the spatial distribution of 222Rn
concentration. Details of FDM are described in Appendix.
The values of D and m are defined in reference to Megumi
and Mamuro (1973) and Owczarski et al. (1990) as being
5 9 10-6 m2/s (D) and 3 9 10-5 m/s (m) along the dip of Fig. 9 Example of grid generation used in the FDM for calculating
the fault in a fault zone, and 4 9 10-6 and 1 9 10-5 m/s in 222
Rn concentrations in shallow soil

123
1542
Case study of the Futagawa fault
As the 222Rn concentration in shallow soil was shown to be
particularly high in the vicinity of the main and subordinate
fault on transects A and B (Fig. 4), the N222 was calculated
at the grid points at a depth of 0.5 m to estimate the fault-
zone geometry. The location, dip direction and angle,
width, and N222 at Rn source were chosen as unknown
variables, and the N222 data near the faults were selected
for modeling (Fig. 10). The simulation was iterated with
different parameter values until the calculated N222 corre-
sponded to the distribution of measured N222. In the
iteration, the step widths of dip angle, zone width, and
222
Rn source number were set at 1, 0.5 m, and 0.1 9 106,
respectively, and the model minimizing the squared error
was accepted as the final result. In order to consider the
spatial variation in the dip angle, the angle step width was
set small. In the following discussion, however, the faults
with dip angles within 10 are regarded to be similar in
accordance with usual fault analysis.
Fig. 10 (1) High N222 values extracted from the vicinity of faults (top), (2) 222Rn concentrations calculated by the FDM (middle), and (3) fault-
zone models used for calculation (bottom)
123
Environ Geol (2009) 56:15331549
Figure 10 shows the resultant fault-zone models for
each transect along with the distributions of 222Rn num-
ber. The general trends of measured N222 and the
simulated N222 are confirmed to be similar. All the fault-
zone models dip northward, which signifies a normal fault
type based on the topography. This dipping configuration
corresponds to the geological insight (Watanabe 1984)
and deep structure of fracture zones to a depth of 10 km
determined by magnetotelluric survey across the Futaga-
wa fault (Asaue et al. 2004). Figure 11 shows the
superposition of the fault models on the lineaments. The
models belonging to the main fault indicate dips of 69
(A), 75 (B), and 55 (C; corrected to 69), with an
estimated fault zone width of 10 m. For the subordinate
faults, the models indicate a dip of 69 and 55, gentler
than for the main fault
Based on the exact spatial relationship with the linea-
ments, the consistency of dip directions, and the similarity
of dip angles, the fault-zone models are considered to
reasonably express the configuration of the shallow part of
Environ Geol (2009) 56:15331549 1543

Fig. 11 Configuration of two sets of fault-zone models correspond-

ing to the main and subordinate faults superimposed over the
observed lineaments

the Futagawa fault system. An important feature is that the

dip of the subordinate fault is quite similar to that of the
main fault, implying that faults with similar orientations
tend to be formed in a common tectonic regime, although
the continuities may be different. The lowland area
extending to the northwest of the Futagawa fault area is
thought to be a graben structure based on the subsurface
structures of pyroclastic flow deposits and andesitic lava
(Matsumoto 1974). The graben must have been formed by
normal faulting movement, further supporting the features
of the fault-zone models derived here.
A drilling survey close to the start point on transect B
has revealed a fracture zone located in the Aso-2 member
at depths of 39.144.7 m (Kumamoto Prefecture 1997).
The dips of the fault gouges have been reported to be in the
range 5080. Although the parameter values used in the
FDM, particularly D, m, and source depth, were defined
arbitrarily and different values will produce different
models, the model dip angles correspond well with the
observed values. The parameter values and FDM procedure
employed here can therefore be considered valid. Fig. 12 a Location of the Kinbara area through which the Neodani
fault pass, Gifu Prefecture in central Japan, b distribution of N222
Case study of the Neodani fault along the transect, c N222 calculated from the finite difference method,
and d fault-zone model and sketch of a part of the trench section until
the 5-m depth quoted from Miyakoshi et al. (1993)
Transect A crosses a trench corresponding to the main
fault, which has been reported to exhibit 5 m lateral dis-
placement of the Futagawa fault based on the offset of a For this purpose, a part of the Neodani fault in the
small fluvial channel, but for which only vague evidence is Kinbara area of Gifu, central Japan, was selected for
available for the vertical displacement and fault configu- analysis, as this fault is a well-studied seismogenetic fault
ration (Kumamoto Prefecture 1997). Recent movement of that moved during the Nobi Earthquake (M 8.0) in 1891
the Futagawa fault and the shallowness of the trench (5 m) with clear evidence on the ground surface. The movement
may have obscured older vertical movements. Thus, it is history of the fault has been investigated by a trench survey
necessary to crosscheck the results of CRAS and FDM with (Miyakoshi et al. 1993). Figure 12 depicts a sketch of the
a well-identified fault configuration. part of the trench section down to a depth of 5 m quoted

123
1544
from the reference, showing a fault in the channel deposits
and on the top of basement rocks with an eastward dip of
80 accompanied by a fracture zone of 12 m in width. A
transect of 50 m in length was set parallel to the trench
section and analyzed by the same Rn survey and modeling
procedure as for the Futagawa fault area. However, the
analysis was simplified in this case because the topography
along the Neodani transect is almost flat.
In the distribution of N222 along the transect (Fig. 12),
local triangular peaks are present, with a gradual increase
toward the west and sharp decrease following the maxi-
mum. The location of the highest N222 point is consistent
with the location of the main fault as determined by trench
survey. A typical nonequilibrium pattern of type-A gas can
also be seen at this point. The FDM simulation was focused
on the data in the vicinity of the main fault and was per-
formed assuming N222 at Rn source of 2.4 9 106 in the
fault zone and of 1.0 9 106 in the surrounding area. All
other parameters were set the same as for the Futagawa
case. The best-matched calculation by the FDM was
obtained for a model with an eastward dip of 79 and a
fault zone width of 12 m, which is almost identical to the
actual fault geometry. This further demonstrates the capa-
bility of a combined CRAS and FDM approach for
modeling fault-zone geometry.
Discussion
Comparison with resistivity distribution
Electric sounding is also a widely used traditional method
of fault investigation. The resistivity has been shown to be
related to fault features such as gouges and geologic dis-
continuities (e.g., Suzuki et al. 2000; Wise et al. 2003). To
evaluate the usefulness of Rn surveys, electric sounding
using a dipoledipole array was conducted in the Futagawa
fault area to parallel the Rn measurements. The sounding
was restricted by natural features on transect B due to a
lack of bare ground near the start point. The sounding
survey on transect C was limited to the region around the
main fault.
Figure 13 shows the resistivity distributions derived by
inversion analysis of the obtained apparent resistivity on
each transect. On transect A, the main fault is located at the
edge of a zone of relatively high resistivity ([200 X
m),
but the resistivity pattern does not clearly represent the
fault shape. In contrast, the subordinate fault can be iden-
tified from a drop in the resistivity along transects A and B.
Although the dips determined by the CRAS approach and
resistivity measurements differ by about 25, the dip trend
is the same: both dip northward. Notably, the resistivity at
the main fault on transect B is lower than 25 X
m,
123
Environ Geol (2009) 56:15331549
however, its relation to the fault is ambiguous because the
resistivity is located on the transect edge. For transect C,
which was covered by talus deposits, the resistivity does
not respond to the fault, instead exhibiting a horizontally
layered structure with no fault manifestations. Conse-
quently, the 222Rn concentrations are considered to be
more sensitive to the presence of faults, regardless of sur-
face lithologies, and can provide more reliable fault-zone
models than electric sounding.
Mechanism of sharp rise in Rn concentrations
in fault zones
In the fault-zone models, the 222Rn concentrations at
source depth in the fault zone were assumed to be higher
than in the surrounding zone. To confirm the validity of
this assumption, soil samples were taken from above the
fracture zone in boring cores from the Futagawa fault area,
and the radioactivity of the samples were measured using a
1480 Wizard Gamma Counter (Wallan Inc.). This instru-
ment has a built-in cylindrical photo-amplifier of 75 mm in
diameter and 80 mm in height, which is coated with NaI.
The target of measurement is 214Pb, the first daughter
nuclide of 222Rn and which emits c-rays upon decay
(222Rn?218Po?214Pb). Therefore, the 222Rn concentration
can be estimated from the c-ray counts based on the pro-
portionality relation of half-life.
Four samples were collected, from depths of 0.5, 5.8,
23.2, and 43.3 m, corresponding to topsoil, Aso-4, Aso-2,
and the fracture zone, respectively. After drying, the sam-
ples were crushed and divided into two specimens of 30 g
each. Reference data were also obtained for a large fracture
zone (10 m width) in a gabbro quarry, 30 km north of the
Futagawa fault area (data 5) in Fig. 14, and for top soil from
the grounds of Kumamoto University (data 6). Figure 14
shows the results of measurements as the averaging of the
two data at each depth. Maximum values were obtained in
the range of 340360 keV for samples from the boring
cores, and the values increased in approach to the fracture
zone. This corresponds well to the target c-ray energy level
of 352 keV for the parent nuclides of 214Pb, indicating an
abundance of these isotopes in the fracture zone. The two
reference data do not exhibit peaks within that energy range,
consistent with the absence of active faults in the quarry
area, which lies in a regional metamorphic zone (the Sangun
metamorphic zone). Although many fracture zones are
present in the quarry, they must have been formed under old
tectonic stress fields unrelated to the present field.
On the basis of these results, a significant reservoir of
222
Rn and its parents appears to have accumulated in the
fracture zone of these recently active faults. Several studies
have indicated that Th is strongly adsorbed by kaolinite,
while Ra is adsorbed onto mineral surfaces such as quartz,
Environ Geol (2009) 56:15331549
Fig. 13 Resistivity distribution
obtained by inversion analysis
of apparent resistivity by
electric sounding using a dipole-
dipole array along the transects
A, B, and C
kaolinite, and other clay minerals (Riese 1982; Ames et al.
1983a, b; Wanty and Schoen 1993). In the U decay series,
230
Th and 226Ra can be accumulated in fault gouges,
resulting in a sharp rise in 222Rn concentrations in soil
gases in fault zone due the relatively long half-lives of
these isotopes (8.0 9 104 and 1.62 9 103 years, respec-
tively). This relationship between cause and effect is
similar to the accumulation of U in rocks to produce
anomalous Rn concentrations in groundwater (Wanty and
Gundersen 1987), with a direct correlation with Rn con-
centrations in the overlying soils (Gates and Gundersen
1989). The Rn activity of geopressured solution gas is
known to be directly proportional to the amount of Ra
contained in the aquifer water (Kraemer 1986). The
1545
concentrations of 230Th, 226Ra, and 222Rn in shallow soils
in areas without active fault zones must be generally low,
as indicated by data (5) and (6) in Fig. 14.
A question then arises as to from where do the radio-
nuclides originate. Pumping effects caused by earth tides
are known to increase Rn concentrations (e.g., Barnet et al.
1997; Lenzen and Neugebauer 1999; Groves-Kirkby et al.
2006), but tectonically induced fault movements may have
stronger effect on the increase and spatial variation of Rn
concentrations than earth tides. Gold and Soter (1984/85)
stated that major earthquakes are often accompanied by the
eruption of high-pressure gas from great depth via frac-
tures. This gas may carry radionuclides from deep crust and
fluids to the near surface, to accumulate in fault gouges.
123
1546 Environ Geol (2009) 56:15331549

Fig. 14 Gamma-ray spectra of

six specimens sampled from
depths of (1) 0.5, (2) 5.8, (3)
23.2, and (4) 43.3 m (gouge
sample) at a boring site near the
start point of transect B; and
samples from (5) a large
fracture zone in an amphibolite
quarry in the Sangun
metamorphic zone 30 km north
of the Futagawa fault area, and
(6) the top soil of Kumamoto
University. Arrows denote the c-
ray energy level of 214Pb decay

This mechanism is shown schematically in Fig. 15. The
two conditions that are essential for reaching high Rn
concentrations in shallow soil under nonequilibrium Rn gas
conditions are the repetition and recentness of fault
movement. As the half-lives of 230Th and 226Ra are short
on a geological time scale, the concentrations of these
isotopes in gouges will decrease with time, making it
impossible to reach significant Rn concentrations in soil
under low velocities of gas ascent. However, repeated
supply of high-pressure gas during faulting can elevate the
concentration to very high levels. This mechanism is sup-
ported by the low 214Pb concentration in the fracture-zone
sample from the quarry, which had a wide gouge zone. The
limitations of Rn surveys of soil gas should therefore be
considered in terms of fault detection.
Conclusions
A new calculation method, CRAS, was introduced to
estimate the Rn concentration in soil gas more accurately
by the a-scintillation counter method. The method con-
siders the Rn gas condition in terms of radioactive
equilibrium, and allows the populations of 222Rn, 218Po,
and 220Rn to be determined at the start of measurement.
This method was applied to nonequilibrium gases sampled

Fig. 15 Schematic mechanism

of sharp rise in 222Rn
concentration and generation of
nonequilibrium Rn gas
conditions at faults based on
repetitive and recent fault
movement. Th and Ra are
trapped in fault gouges as parent
nuclides of 222Rn, 230Th and
226
Ra, with half-lives much
longer than that of 222Rn

123
Environ Geol (2009) 56:15331549 1547

near fumaroles in a hot spring area and equilibrium gases
sampled from normal soil. The total decays tend to increase
with the time under nonequilibrium conditions, whereas the
decays decrease rapidly within a few minutes down to a
constant value under equilibrium conditions. The CRAS
method was shown to be effective for both gas types and
suitable for predicting the temporal change in Rn decay.
The method also allows the gas age to be estimated, pro-
viding information on the activity of ascending gas. It was
demonstrated that the empirical formula used for process-
ing measurement data underestimates the 222Rn
concentration, which is more useful for detecting latent
faults than 220Rn due to the much longer half-life of 222Rn.
The improved accuracy of 222Rn concentrations
obtained by CRAS compared to the empirical formula-
based concentrations was clarified through analyses of
sample data taken along transects crossing active Futagawa
and Neodani faults. The CRAS results exhibit a clear
correlation with lineaments associated with the main and
subordinate faults in terms of position and magnitude,
displays clear spatial self-correlation due to the existence
of faults, and produces a remarkable geometry-related
distribution of concentration across faults. The Rn gas in a
fault zone was also found be under nonequilibrium con-
ditions, without an active rise in carrier gas.
The combination of CRAS and FDM simulation was
shown to be effective for modeling the shallow part of a
fault with respect to width and dip direction and angle. The
FDM was performed for the diffusion and advection of Rn
in arbitrary terrain. Fault-zone models were constructed for
on the characteristics of these isotopes, the repetition and
recentness of fault movement is considered essential for
reaching high Rn concentrations in shallow soils under
nonequilibrium Rn gas conditions and low-gas ascent
velocity.
Acknowledgments The authors wish to express their gratitude to
Mr. Yasutaka Koba and the graduate students, who assisted in the
radon and electrical surveys and data analysis, and Mr. Jitsuya
Uemura of the Radioisotope Center of Kumamoto University for
instruction regarding the measurement of c-ray spectra. Sincere
thanks are extended to Dr. Eveln Roeloffs, of U. S. Geological Sur-
vey, for helpful comments to improve the clarity of the manuscript.
The anonymous reviewers valuable comments are also gratefully
appreciated.
Appendix
As the terrain on which the transects were set was not flat, a
uniform mesh composed of simple rectangular or square
elements cannot be used for the FDM simulation. Thus, a
mapping of the actual terrain of the calculation regime (xz
plane) to a simple rectangular regime (ng plane) by
coordinate transformation is considered. The differential
equation is then solved in the ng plane. The mapping
function between the two planes is expressed by
)
n nx; z
A1
g gx; z
The partial derivatives then give

9
oN oN oN >
nx gx >
>
ox on og >
>
>
>
oN oN oN =
nz gz A2
oz on og >
>
2     2 2 2 >>
>
oN oN oN 2 o N o N 2 o N >
>
2
n z g z n z 2
2n z g z g z 2
;
oz oz n oz g on onog og

two study areas by matching the 222Rn concentrations by where the subscripts denote the derivative with respect to x
FDM to those by CRAS. The method revealed that the or z. Using equations (A2), Eq. (12) can be rewritten as
main and subordinate faults in the Futagawa fault are, to be follows:
subparallel with normal faulting configuration, in agree-
ment with geologic investigations. The model produced for o2 N o2 N 2  vz  oN
2o N vx
the Neodani fault area was also consistent with the geo- n2z 2
2n g
z z g z 2
nzz  nx  nz
on onog og D D on
metric features determined by trench survey.  vx vz  oN k
From an c-ray scintillation survey of the soil and rock gzz  gx  gz  N0 A3
D D og D
samples, the parent nuclides of 222Rn, 230Th and 226Ra
were estimated to be trapped in the gouges of active fault. By applying the spatial backward difference to
These nuclides may be entrained in the eruption of high- Eq. (A3), the following difference equation can be
pressure gases from great depth during earthquakes. Based obtained:

123
1548 Environ Geol (2009) 56:15331549

N nDn;g2N n;gN nDn;g Ames LL, McGarrah JE, Walker BA, Salter PF (1983b) Sorption of
n2z uranium and radium by biotite, muscovite, and phlogopite. Clays
Dn2

Clay Miner 31:343351
N n;gN n;gDgN nDn;gN nDn;gDg Ball TK, Cameron DG, Colman TB, Roberts PD (1991) Behaviour of
2nz gz
DnDg radon in the geological environment: a review. Q J Eng Geol

N n;gDg 2N n;gN n;gDg 24:169182

g2z Barnet I, Prochazka J, Skalsky L (1997) Do the earth tides have an
Dg2
  influence on short-term variations in radon concentration? Radiat
vx vz N n;gN nDn;g Prot Dosimetry 69:5160
nzz  nx  nz
D D Dn Chitkov AM (1975) Radon as a possible criterion for predicting
 vx vz  N n;gN n;gDg k eruptions as observed at Karymsky Volcano. Bulletin Volcanol
gzz  gx  gz  N n;g 0
D D Dg D 39:126131
Chyi LL, Chou CY, Yang FT, Chen CH (2002) Automated radon
A4
monitoring of seismicity in a fault zone. Geofis Int 41:507511
where Dn and Dg are the grid intervals along the n and g Chung Y-C (1981) Radium-226 and radon-222 in southern California
goundwaters: spatial variations and correlations. Geophys Res
axes.
Lett 8:457460
Equation (A4) can then be transformed to an expression Ciotoli G, Guerra M, Lombardi S, Vittori E (1998) Soil gas survey for
involving an arbitrary grid point (i, j) in the n-g plane. The tracing seismogenic faults: a case study in the Fucino basin,
222 Central Italy. J Geophys Res 103:23,78123,794
Rn concentration, diffusion coefficient, and gas velocity
Duddridge GA, Grainger P, Durrance EM (1991) Fault detection
components at n = iDn and g = jDg are denoted by Nij,
using soil gas chemistry. Q J Eng Geol 24:427435
Dij, and (mxij, mzij), respectively. Following Koike et al. Gasparini P, Mantovani MSM (1978) Radon anomalies and volcanic
(1996), the diffusion coefficient and gas velocity between eruptions. J Volcanol Geotherm Res 3:325341
two adjacent grid points are approximated suitably by the Gates AE, Gundersen LCS (1989) Role of ductile shearing in the
concentration of radon in the Brookneal zone, Virginia. Geology
harmonic average, as follows:
9 17:392394
Dij 2Dij Dij1 =Dij Dij1 > >
Gingrich JE (1984) Radon as a geochemical exploration tool.
= J Geochem Explor 21:1939

mxij 2mxij mxi1j =mxij mxi1j A5 Gold T, Soter S (1984/85) Fluid ascent through the solid lithosphere
>
> and its relation to earthquakes. Pure Appl Geophys 122:492530

m 2m m =m m ;
zij zij zij1 zij zij1 Groves-Kirkby CJ, Denman AR, Crockett RGM, Phillips PS,
Gillmore GK (2006) Identification of tidal and climatic influ-
By these parameters, Eq. (A4) can be finally transformed ences within domestic radon time-series from Northamptonshire,
into the following expression. UK. Sci Total Environ 367:191202

( ) 9
1 n2z   2nz gz g2z >
>
Nij   2 Ni1j  B Ni1j  C Nij1  Ni1j1  2 Nij1 >
>
A Dn DnDg Dg >
>
>
! !>
>
>
2 2 mv 
v 
v 
v  >
>
k n 2n g g 1 1 >
gzz   gx   gz >
 z z xij zij xij zij
A   2  2 nzz   nx   nz >
>
Dij Dn DnDg Dg Dn Dij Dij Dg Dij Dij =
! A6
n2 2n g 1 vxi1j vzi1j >
>
B 2  z z  nzz   nx   nz >
>
>
>
Dn DnDg Dn Di1j Di1j >
>
! >
>
>
>
2n g g 2
1 v 
v  >
>

C  z z
2
xij1
gzz   gx   gz
zij1 >
>
DnDg Dg Dg Dij1 Dij1 ;

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