J. Radiat. Res.

, 50, 333343 (2009) Regular Paper

Simultaneous Measurements of Radon and Thoron Exhalation Rates

and Comparison with Values Calculated
by UNSCEAR Equation

Masahiro HOSODA1, Atsuyuki SORIMACHI1, Yumi YASUOKA2, Tetsuo ISHIKAWA1,

Sarat Kumar SAHOO1, Masahide FURUKAWA3, Nabil Mohammed HASSAN1,
Shinji TOKONAMI1* and Shigeo UCHIDA1

Radon/Thoron/Exhalation rate/Simultaneous measurements/UNSCEAR equation.

We simultaneously measured radon and thoron exhalation rates in areas of weathered acid rocks in
Japan to investigate the relationship between them and between measured and calculated radon exhalation
rates. To calculate the radon exhalation rate, we used an equation proposed by UNSCEAR. Our analysis
showed that both the radon and thoron exhalation rates measured at one location in a natural environment
fluctuated widely, even within one day. We found a strong correlation between the radon and thoron exha-
lation rates. The measured radon exhalation rates tended to be lower than the calculated values: the mean
ratio of the measured exhalation rate to the calculated rate was 0.65. We concluded that the UNSCEAR
equation is applicable under a controlled environment (temperature, humidity, etc.), but not where there
are artificial underground structures that may influence the transportation of radon in soil.

INTRODUCTION
The global average annual effective dose from natural
radiation is 2.4 mSv.1) The effective doses from radon
(222Rn) and thoron (220Rn) and their decay products comprise
about 50% of this amount. There have been many reports
published on the health effects of radon exposure.25) Radon
and thoron comes from soil, rocks, and building materials.
The soil can be regarded as the main source. Emanation of
radon gas into the atmosphere is dependent on local ground
surface and soil conditions. The exhalation rate of radon is
one of the most important factors that influence indoor and
outdoor radon concentrations. The half-life of radon is
3.82 d and that of thoron is 55.6 s; it is therefore presumed
that their generation points in soil are different. It is thought
that radon and thoron are generated from the depth in soil
and soil surface, respectively. The temperature and moisture
*Corresponding author: Phone: +81-43-206-3104,
Fax: +81-43-206-4098,
E-mail: tokonami@nirs.go.jp
1
National Institute of Radiological Sciences, Research Center for Radiation
Protection, 4-9-1Anagawa, Inage-ku, Chiba-shi, Chiba 263-8555, Japan;
2
Kobe Pharmaceutical University, Institute of Radioisotope Research, 4-19-
1 Motoyamakita, Higashinada-ku, Kobe-shi, Hyogo 658-8558, Japan;
3
University of the Ryukyus, Faculty of Science, 1 Senbaru, Nishihara,
Okinawa 903-0213, Japan.
doi:10.1269/jrr.08121
content at the deep layer differ from them on the soil surface.
This is considered to influence exhalation of radon and
thoron. Although many researchers have investigated the
behavior of radon in soil,69) there are few reports about the
behavior of thoron in soil. Because the half-life of thoron is
shorter than that of radon, it is more difficult to estimate its
exhalation rate. For this reason, an effective method for
measurement of thoron exhalation rate has not yet been
established, and few data on the thoron exhalation rate are
available. If radon and thoron exhalation rates can be simul-
taneously measured with one instrument, the transport behav-
iors of radon and thoron in soil can be considered. However,
there is little published data that present simultaneous field
measurements of radon and thoron exhalation rates.
We previously developed an instrument for the simulta-
neous measurement of radon and thoron exhalation rates and
used it to measure radon and thoron exhalation rates at some
typical Japanese geological sites.1015) In this study, we
measured radon and thoron exhalation rates in areas of
weathered acid rock in Hyogo and Aomori Prefectures and
investigated the relationship between radon and thoron exha-
lation rates. Furthermore, we calculated theoretical radon
exhalation rates in Kobe City (Hyogo Prefecture) by using
an equation proposed by UNSCEAR,1) where reported that
the radon exhalation rate can be mathematically expressed as
a function of the emanation coefficient, porosity, 226Ra
concentration, soil density, and the effective diffusion coef-
ficient. We examined the applicability of the equation pro-

J. Radiat. Res., Vol. 50, No. 4 (2009); http://jrr.jstage.jst.go.jp

334 M. Hosoda et al.

posed by UNSCEAR for calculation of radon exhalation
rates by comparing our measured values with those calculated
by the UNSCEAR equation.1)
MATERIALS AND METHODS
Study areas and measurement conditions
The study areas (Fig. 1) were selected on the basis of
surface geology. The surface geology of Japan can be cate-
gorized into areas dominated by andesite, basalt, pyroclastic
flows, sediments, and strata containing volcanic ash fall.1617)
The distribution of plutonic rocks (e.g., granite) and sedi-
mentary rocks are about 67% in Japan.17) We focused on
areas of weathered acid rock (granite and rhyolite) and
selected two areas with different climates: Kobe City
(3443N, 13517E) in Hyogo Prefecture, and Mutsu City
(4117N, 14112E) and Higashidori Village (4125N,
14127E) in Aomori Prefecture. Altitude of measurement
points in Kobe City and Aomori Prefecture were about 40 ~
90 m and about 10 ~ 100 m, respectively. The bedrock of all
measurement points was weathered acidic rock. The mea-
surement point in Kobe City was granite of Mt. Rokko, and
it was based on generating penetration of Cretaceous period
in Mesozoic era. The measurement points in Mutsu City and
Higashidori Village were rhyolite of tertiary period in
Cenozoic era and granite of Jurassic period in Mesozoic era,
respectively. Kobe City has a moderate climate (annual aver-
age temperature of 17.4C), whereas Aomori Prefecture has
a cool climate (annual average temperature of 10.1C).
Seven measurement points were selected in each area. In
Kobe City, five measurement points were within the grounds
of the Kobe Pharmaceutical University, and two were in an
undisturbed area outside the university. All measurement
points in Aomori Prefecture were in the undisturbed area. At
five of the seven measurement points (Point1, 2, 3, 4, and 6)
in Kobe City, measurements were taken in January, May,
August, and November in order to observe seasonal variations.
Measurements were taken twice (August and November) at
the other two points (Point 5 and 7) in Kobe City. In Aomori
Prefecture, only one set of measurements was taken at each
location. In Kobe City, the day before measurements were
taken in May was rainy, but it was fine or cloudy for the
other measurements (including Aomori Prefecture) taken.
Because one of the aims of this study was to investigate sea-
sonal variations of radon and thoron exhalation rates, all data
(including the data measured in May) were used.

Fig. 1. Map showing the measurement sites for this study.

J. Radiat. Res., Vol. 50, No. 4 (2009); http://jrr.jstage.jst.go.jp

 Simultaneous Measurements of Radon and Thoron
Fig. 2. Diagram of the system used for simultaneous in situ mea-
surement of radon and thoron exhalation rates from the ground.
Measurement of radon and thoron exhalation rates
Radon and thoron exhalation rates were measured with an
instrument (MSZ: Fig. 2) developed and described by Shimo
et al.10) and Saegusa et al..11) We adopted the accumulation
method for our measurements. Because details of the MSZ
have been reported previously,1011) only an outline is pro-
vided here. It is composed of the accumulation chamber
(skirt section) which covers the ground, scintillation detector
with aluminized mylar sheet, light guide, photomultiplier
tube, pulse counting part, scaler and timer. The area of large
acrylic board coated with a ZnS(Ag) scintillator is 1200 cm2.
The ZnS(Ag) scintillator is connected to a photomultiplier
tube with 6.3 cm diameter though a tapering lightguide. The
purpose of skirt section (13 l volume) is for collecting radon
and thoron gases that exhaled from the ground surface.
Measurements were recorded over consecutive 30 s intervals
during a total recording period of 30 minutes after setting it
up on the surface of ground. The thoron exhalation rate ET
was obtained by the following formula;
ET = (N10 Nb) CFT ,
where N10 is the count rate 10 minutes after measurement start
(cpm), Nb is the count rate of background (cpm), and CFT is the
conversion factor for 220Rn (18.1 3.2 mBqm2s1cpm1).
Since the count rate of 220Rn and its decay product (216Po)
reaches equilibrium 7 8 minutes after starting measure-
ment, the count rate of 10 minutes is used for N10. On the
other hand, the count rate of 222Rn and its decay products
(218Po and 214Po) adopts the count rate of 30 minutes after,
in order to continue a gentle increase after subsequent
10 minutes. The radon exhalation rate ER was obtained by
the following formula;
ER = (N30 N10) CFR ,
where N30 is the count rate 30 minutes after measurement
start (cpm), and CFR is the conversion factor for 222Rn (0.521
J. Radiat. Res., Vol. 50, No. 4 (2009); http://jrr.jstage.jst.go.jp
335
0.040 mBqm2s1cpm1).
We conducted a preliminary laboratory experiment to test
whether covering the MSZ during recording would affect the
influence of meteorological factors such as temperature,
atmospheric pressure, and relative humidity of the soil sur-
face. Analysis by t-test of the results of this experiment
clearly showed that meteorological influences were
unchanged whether or not the MSZ was covered during
measurement. The weathering granite soil was used in the
estimate of measurement error. Radon and thoron exhalation
rates of this sample were measured repeatedly several times
by MSZ. Average radon and thoron exhalation rates of this
sample were 20 mBqm2s1 and 3200 mBqm2s1, respec-
tively. In this result, the measurement errors (1) for radon
and thoron exhalation rates were estimated to be 19% and
6.3%, respectively.18) When radon and thoron exhalation
rates obtained by the MSZ were lower than that of detection
limit, these data were excluded in this study.
Measurement of the radon emanation coefficient
According to UNSCEAR,1) the exhalation rate of radon can
be mathematically expressed as a function of the emanation
coefficient, porosity, 226Ra concentration, soil density, and the
effective diffusion coefficient. If such parameters are measured
or theoretically evaluated, the radon exhalation rate can be esti-
mated by using the expression proposed by UNSCEAR.1)
Soil samples were dried (by the same procedure as that
used for soil density and radium concentration measure-
ments, as described below) and then packed roughly into a
stainless steel tray (160 mm wide, 195 mm long, and 35 mm
in height) to a depth of 35 mm. To vary moisture content,
an atomizer was used to spray deionized water onto the soil
samples. In general, the moisture content was taken to be
liquid-phase weight divided by solid-phase weight. We took
measurements for moisture contents ranging from absolutely
dry to 40 wt% water. Soil samples were stirred until the
moisture in the sample was uniformly distributed and then
sealed in an accumulation chamber made of acrylic resin
(1)
(6.7 l volume). After 24 h in the sealed accumulation chamber,
the radon concentration was measured. In this study, the
accumulation period was kept as short as possible so that the
moisture content did not change while the radon gas was accu-
mulating. Therefore, the difference of moisture content before
and after all experiments was small (less than 0.1 wt%). To
evaluate the dependence of the emanation coefficient on
moisture content, it is important that the influence of mois-
ture content (relative humidity) on the response of measure-
ment device is insensitive (e.g., an apparatus using activated
charcoal should not be used). For this reason we used the
Pylon model AB-5 portable radiation monitor and Pylon
model 300A scintillation cell (Pylon Electrics, Inc., Ottawa,
(2)
Canada). A quality assurance comparison of the results of
radon concentration measurements with this device has been
performed by the Japanese National Institute of Radiological
336
Sciences and the German Physikalisch-Technische Bunde-
sanstalt.19) In this result, the error to PTB was estimated
within 5%.20)
Soil samples were collected at each measurement point in
Kobe City, with the exception of Point 4. The radon emana-
tion coefficient (f) of each sample was calculated as follows:
AeqVa
f = , (3)
ARa M
where Aeq is the equilibrium concentration of radon (Bqm3),
Va is the volume of accumulation chamber (m3), ARa is the
radium concentration in soil samples (Bqkg1 dry), and M
is weight of the sample (kg). The radon emanation coeffi-
cient can be determined from Aeq and ARa. We used the
following procedure to determine Aeq.
Air sampling and measurements were performed as fol-
lows (see Fig. 3). First, a valve (V1) between the vacuum
pump and scintillation cell was opened and the scintillation
cell was evacuated. The valve (V1) was then closed. Second,
a valve (V2) between the accumulation chamber and scintil-
lation cell was opened to allow the introduction of an air
sample into the scintillation cell. The valve (V3) of accumu-
lation chamber was also opened simultaneously. The valve
(V2) was then closed. Then, after 3.5 h, radon concentra-
tions (At) were measured in the scintillation cell. While the
soil sample was sealed in the accumulation chamber, the
radon concentration in the chamber gradually increased,
reaching equilibrium after about 30 d. In general, the growth
curve for radon concentration can be expressed:
At = Aeq (1 e t ) ,
where At is the concentration of radon measured at time t
(Bqm3), is the decay constant of radon, and t is the accu-
Fig. 3. Schematic of the experimental system used to evaluate the
emanation coefficient of radon.
J. Radiat. Res., Vol. 50, No. 4 (2009); http://jrr.jstage.jst.go.jp
M. Hosoda et al.
mulation time for sampling (s). Aeq can then be calculated
because all other variable in equation (4) are known. Then,
after determination of the soil parameters discussed below,
the radon emanation coefficient (f) can be calculated from
equation (1).
Estimation of soil parameters
Moisture content, dry bulk density, density, porosity, and
concentration of 226Ra were measured as follows.
(1) Volumetric water content
Volumetric water content in soil samples was measured
using a soil aqua-meter (DIK-691A-B1, Delta-T Devices,
Cambridge, England) at each exhalation rate measurement
point. These measurements were taken during the radon
exhalation rate measurement. Because the sensor length is
5 cm, we measured volumetric water content at a depth of
5 cm in the soil. As the sensor signal is proportional to the
permittivity of the soil, the volumetric water content is mea-
sured directly by this device.
(2) Dry bulk density
The dry bulk density b (gcm3) was calculated as fol-
lows:
M
b = . (5)
VS
where M (g) is the weight of the soil sample, and VS (cm3)
is the volume of the dry soil.
(3) Density
The density (gcm3) of the soil sample was calculated
using the following procedure.21) First, the soil sample was
(4)
dried for 24 h at 105C. Second, after weighing an empty
specific-gravity bottle (Wf), it was filled with water and
weighed (Wa). The water was then removed from the specific-
gravity bottle, and the bottle was dried. The bottle was then
approximately one-third filled with dry soil and weighed
(W). Finally, the remaining two-thirds of the bottle was filled
with water and it was placed in a vacuum desiccator and
evacuated. Because initially there were bubbles in the bottle,
the desiccator formed only a quasi-vacuum. This operation
was repeated until there were no bubbles. After one week,
the bottle was removed from the vacuum desiccator, filled
with water, and weighed (Wb). The unit of all W is gram. The
density of the soil was calculated as follows:
W Wf
= . (6)
(W W f ) + (Wa Wb )
(4) Porosity
Five soil samples were taken from a depth of 5 cm at each
measurement point. The porosity was estimated as follows:
b
= 1 . (7)
(5) 226Ra concentration in soil
Measurements of rays emitted from nuclides of 226
Ra
 Simultaneous Measurements of Radon and Thoron
were made by counting photons in the photoelectric peak
channels of 352 keV for 214Pb and 609 keV for 214Bi, after
radioactive equilibrium of 226Ra with 214Pb and 214Bi had
been achieved. 228Ra was measured by counting photons in
the photoelectric peak channel of 911 keV for 228Ac. Mea-
surement of radium concentrations in soil samples was as
follows. First, the soil samples were enclosed in a cylindrical
polypropylene container of 48 mm 55 mm (U8 container)
after drying for 24 h at 105C. The prepared soil sample was
then enclosed in an air-tight container for 40 d to allow
radioactive equilibrium between 226Ra and 222Rn to be
reached. Soil samples were then analyzed using a high-puri-
ty germanium detector. The measurement time was 80000 s.
In this study, the average concentration of 214Pb and 214Bi
were used as the 226Ra concentration in the soil samples.
RESULTS AND DISCUSSION
Radon and thoron exhalation rates in Kobe City
The average ( standard deviation) of the radon and
thoron exhalation rates at the seven measuring points in
Kobe City were 12 6 and 1210 1110 mBqm2s1,
respectively (Table 1). These results are similar to those from
other weathered granite soils (radon, 10 3 mBqm2s1;
thoron, 1290 260 mBqm2s1) reported by Hosoda et
al..22) The maximum average radon exhalation rate (17
11 mBqm2s1) was measured at Point 6; the minimum (3
1 mBqm2s1) was measured at Point 5. The maximum
average thoron exhalation rate was measured at Point 4
(2560 1940 mBqm2s1); the minimum was measured at
Point 3 (640 640 mBqm2s1). The geological environ-
ments at all measurement points were similar (weathered
granite soil of Mt. Rokko), but the exhalation rates differed
considerably between them. This suggests that different sub-
surface structures may have influenced the exhalation rates.
The largest coefficient of variation (CV) of the measured
radon exhalation rates was at Point 3 (66%, Table 1) and the
smallest was at Point 7 (16%). The CVs for radon at other
measurement points ranged between approximately 40%
and 60%. The largest CV for thoron exhalation rate was also
at Point 3 (100%), whereas that at Point 1 (22%) was the
smallest of all the measurement points.
Radon and thoron exhalation rates in Aomori Prefecture
Average radon and thoron exhalation rates in Mutsu City
(Table 2) were 13 8 and 750 460 mBqm2s1, respectively:
the corresponding values in Higashidori Village were 17 11
and 1040 710 mBqm2s1. The bedrock at Mutsu city is
rhyolite and that at Higashidori Village is granite. Granite and
rhyolite are both classified as acid rocks, according to their
SiO2 content (over 66 wt%).2324) Comparison of the radon and
thoron exhalation rates at the two locations in Aomori
Prefecture showed that both were higher in Higashidori
Village: radon by a factor of 1.3 and thoron by a factor of
J. Radiat. Res., Vol. 50, No. 4 (2009); http://jrr.jstage.jst.go.jp
337
1.4. However, t-test of data from all measurement points in
Aomori Prefecture showed no significant difference in the
radon and thoron exhalation rates measured at Higashidori
Village and Mutsu city (p > 0.05). Similarly, there was no
significant difference between the exhalation rates measured
in Aomori Prefecture and those measured in Kobe City (p >
0.05). The measurement points in Higashidori Village were
all located within an area of 1 km radius, as was the case in
Kobe City. On the other hand, the measurement point of
Mutsu city was large area. Thus, we presumed that within
each of these areas, the measurement points were in areas of
the same bedrock. However, the maximum radon and thoron
exhalation rates in Higashidori Village differed by factors of
3.4 and 5.0, respectively. The CVs for radon and thoron
exhalation rates in Higashidori Village were 63% and 69%,
respectively. Although the measurements in Higashidori
Village were conducted within one day, there were large
variations of radon and thoron exhalation rates at the same
measurement point. This suggests that underground struc-
tures might have influenced the movement of soil radon in
Aomori Prefecture, as well as in Kobe City.
Relationship between radon and thoron exhalation
rates at each study site
The ratio between the radon and thoron exhalation rates
can be estimated by a theoretical approach that assumes that
228
Ra and 226Ra contents in the soil are the same. We con-
sidered a comparison of the measured ratio with the theoret-
ical ratio derived from the following relationship would be
useful. The ratio of the thoron exhalation rate J220 to the
radon exhalation rate J222 was estimated as follows:
J 220 220 L220
= , (8)
J 222 222 L222
where is the decay constant (radon, 2.1 106 s1; thoron,
0.012 s1), and L is the diffusion length (m), which was cal-
culated from the relationship between effective diffusion
coefficient De and the decay constant.:
De
L= . (9)
The effective diffusion coefficients of radon and thoron
were presumed to be approximately equal because the only
important difference in their physical characteristics is their
mass number (radon, 222; thoron, 220). Assuming the
porosity of dry soil was 0.30, the effective diffusion coeffi-
cient was 3.0 106 m2s1.25) Moreover, this value decreased
as moisture content increased. By using these values of De
and in Eq. (9), the diffusion lengths of radon and thoron
were estimated to be 120 and 1.6 cm, respectively. Eq. (8)
implies that the thoron exhalation rate from the soil surface
to the atmosphere is about 76 times that of radon.
The average of Tn/Rn ratios for all the data in Kobe City
and Aomori Prefecture were 144 174 and 57 9, respec-
338 M. Hosoda et al.

Table 1. Measurements of radon and thoron exhalation rates in Kobe City.

222
Point Date of measurement Rn exhalation rate Tn exhalation rate Rn/220Rn ratio
(mBqm2s1) (mBqm2s1)
2007/5/27 11 5 750 170 66
2007/8/23 33 500 130 152
2007/11/27 43 560 140 142
Point 1
2007/11/28 12 5 850 190 72
2008/1/11 94 590 150 68
Ave. (CV) 8 4 (52) 650 140 (22) 100 43
2007/5/27 63 470 120 77
2007/8/23 17 6 930 200 54
Point 2 2007/11/27 27 7 1040 220 38
2008/1/11 10 5 990 210 104
Ave. (CV) 15 10 (63) 860 260 (31) 68 29
2007/5/26 53 86 42 19
2007/5/27 84 460 120 58
2007/8/23 15 5 620 150 42
Point 3 2007/11/26 17 6 1810 360 105
2008/1/11 74 800 180 116
2008/1/12 22 80 41 38
Ave. (CV) 9 6 (66) 640 640 (100) 63 39
2007/5/26 74 940 210 141
2007/8/23 17 6 1900 370 110
2007/11/26 16 6 5840 1050 363
Point 4 2007/11/28 ND 2830 530
2008/1/11 16 6 1570 320 101
2008/1/13 84 470 120 57
Ave. (CV) 13 5 (39) 2560 1940 (86) 154 120
2007/8/24 43 470 120 124
Point 5 2007/11/27 22 1550 310 815
Ave. (CV) 3 1 (47) 1010 760 (76) 470 489
2007/5/26 22 7 2080 400 95
2007/8/23 30 8 2010 390 68
2007/11/26 43 2160 420 527
Point 6 2007/11/27 53 1920 380 427
2008/1/12 25 7 360 100 14
2008/1/13 16 6 690 160 44
Ave. (CV) 17 11 (64) 1540 790 (52) 196 222
2007/8/24 10 4 530 130 55
Point 7 2007/11/27 84 1690 340 219
Ave. (CV) 9 1 (16) 1110 820 (74) 137 119
Total average (CV) 12 8 (66) 1210 1110 (92) 144 174
ND = not determined, CV = Coefficient of variation
Point 1 and 2: undisturbed area
Point 3 to 7: university

tively (Tables 1 and 2). These values are 1.9 and 0.75 times but the average 228Ra/226Ra ratios for Kobe City and Aomori
higher than the theoretical values for Kobe City and Aomori Prefecture were almost the same (1.3 and 1.5, respectively;
Prefecture, respectively. The thoron exhalation rates in Kobe data not shown).
City tended to be higher than those in Aomori Prefecture, The relationship between radon and thoron exhalation

J. Radiat. Res., Vol. 50, No. 4 (2009); http://jrr.jstage.jst.go.jp

 Simultaneous Measurements of Radon and Thoron 339

Table 2. Measurements of radon and thoron exhalation rates in Aomori Prefecture.

Date of Rn exhalation rate Tn exhalation rate 222
Point Rn/220Rn ratio
measurement (mBqm2s1) (mBqm2s1)
Point 1 2007/8/29 94 520 130 56
Point 2 2007/8/30 23 7 1280 270 57
Mutsu city
Point 3 2007/8/30 84 450 120 53
Ave. (CV) 13 8 (60) 750 460 (62) 55 2
Point 1 2007/11/16 74 540 130 72
Point 2 2007/11/16 25 7 1310 270 52
Higashidori Village Point 3 2007/11/16 29 7 1920 370 67
Point 4 2007/11/16 94 380 110 45
Ave. (CV) 17 1 (63) 1040 710 (69) 59 13
CV = coefficient of variation.

Fig. 4. Relationship between radon and thoron exhalation rates measured in Kobe City. (Left, excluding points 1 and 2; right,
Points 1 and 2 only)

rates in Kobe City is shown in Fig. 4. The decision coeffi-

cient (R2) for all data from Kobe City was 0.078; that is, no
significant correlation was observed (p > 0.05). However, the
results for Points 1 and 2 alone showed a good correlation
(R2 of 0.65, p < 0.05). The relationship between the mea-
sured radon and thoron exhalation rates in Aomori Prefec-
ture is shown in Fig. 5. R2 for all data from Aomori Prefec-
ture was 0.95. In Kobe City, measurement Points 3 to 7 were
within the university campus, where artificial structures such
as underground pipelines may affect path of radon, whereas
Points 1 and 2 were in the undisturbed area outside the uni-
versity. All measurement points in Aomori Prefecture were
located in the undisturbed area. Thus, for data from natural
environments, the exhalation rates of radon and thoron
showed a strong correlation.
Megumi and Mamuro reported that maximum thoron
exhalation rates are attributable to thoron within the upper- Fig. 5. Relationship between radon and thoron exhalation rates
most 4 cm of soil.26) This suggests that artificial structures measured in Aomori Prefecture.

J. Radiat. Res., Vol. 50, No. 4 (2009); http://jrr.jstage.jst.go.jp

340 M. Hosoda et al.

deeper than this might not affect thoron exhalation from soil.
Consequently, the correlation between radon and the thoron
exhalation rates may be unrecognizable in areas where there
are artificial underground structures. Many researchers have
reported that radon exhalation rate is influenced by various
environmental factors, such as moisture content, differential
pressure, and soil grain size.18,2634) In addition to these influ-
ences, artificial materials laid under ground might affect
exhalation rates in urban areas.
measured exhalation rate. The radon exhalation rate J from
radium-in-soil concentration ARa was calculated as follows:1)
J = De f (1 ) ARa , (10)
where f is the soil emanation coefficient of radon, is the
soil particle density (kgm3), and De is the effective diffu-
sion coefficient of radon (m2s1). The relationship between
the effective diffusion coefficient De and moisture saturation
m was reported by Rogers and Nielson25) as:

Comparison of measured and calculated radon exhala-

(
De = D0 exp 6 m 6 m14 ) , (11)
tion rates where D0 is the diffusion coefficient of radon in the atmo-
According to UNSCEAR,1) the radon exhalation rate can sphere (1.1 105 m2s1) and is the porosity of the soil.
be expressed as a function of the emanation coefficient, We obtained moisture saturation m by dividing water content
porosity, 226Ra concentration, soil density, and the effective (m3m3) by porosity . All other parameters except D0 were
diffusion coefficient. We calculated radon exhalation rate by determined by analysis of the soil samples (Table 3). These
using this relationship and compared the results with the values agreed well with values typically reported in the lit-

Table 3. Parameter values used for the calculation of the radon exhalation rate. In this table, dry bulk density, soil density, porosity,
and 226Ra concentrations in soil were the averages for each measurement point. Because the effective diffusion coefficient and ema-
nation coefficient changed with soil water content (depending on soil conditions), these data are shown for each measurement date.
226
Point Dry bulk density Density Porosity Moisture Diffusion Ra concentration Emanation Calculated value of Meas./
(gcm3) (gcm3) saturation coefficient in soil (Bqkg1dry) coefficient exhalation rate Cal.
(m2s1) (mBqm2s1)
0.259 4.3 106 0.35 11 1.32
0.462 2.0 10 6 0.36 8 0.54
Point 1 1.06 0.19 2.67 0.06 0.61 0.07 10.1 0.4
0.121 7.1 10 6 0.33 13 0.37
0.172 1.7 106 0.35 8 1.46
0.504 1.8 10 6
0.33 14 0.58
0.257 4.4 106 0.31 20 1.11
Point 2 1.01 0.11 2.63 0.03 0.60 0.04 20.6 0.7
0.147 6.5 106 0.27 22 1.63
0.238 1.9 106 0.31 14 0.88
0.803 2.8 10 6 0.39 14 0.50
0.612 1.7 10 6 0.39 33 0.37
0.703 8.8 10 6 0.39 24 0.95
Point 3 1.52 0.14 2.67 0.03 0.43 0.05 29.7 1.4
0.209 6.4 10 6 0.39 64 0.41
0.523 3.1 106 0.40 46 0.23
0.784 6.7 10 6
0.38 20 0.15
0.257 6.0 106 0.33 31 0.19
Point 5 1.59 0.09 2.63 0.02 0.40 0.03 17.1 0.5
0.230 6.3 10 6 0.33 32 0.09
0.429 3.4 106 0.30 35 0.94
0.272 5.3 10 6 0.30 44 1.00
0.173 6.9 106 0.30 51 0.12
Point 6 1.47 0.21 2.68 0.01 0.45 0.08 29.7 0.6
0.171 6.9 106 0.30 51 0.13
0.431 3.2 10 6 0.31 35 1.09
0.427 3.2 106 0.31 35 0.67
0.467 3.0 10 6 0.35 26 0.56
Point 7 1.48 0.09 2.64 0.01 0.44 0.03 20.1 0.6
0.223 6.1 106 0.32 35 0.33
Note: Soil samples were not taken at Point 4.

J. Radiat. Res., Vol. 50, No. 4 (2009); http://jrr.jstage.jst.go.jp

 Simultaneous Measurements of Radon and Thoron
erature. A comparison of measured and calculated radon
exhalation rates (average for each point) is shown in Fig. 6.
The t-test results for each measurement point show no sig-
nificant difference between the measured and calculated val-
ues for Points 1 and 2 (p > 0.05). However, the calculated
values for Points 3, 5, 6, and 7 are significantly higher than
Fig. 6. Comparison of the measured and calculated radon exhala-
tion rates for Kobe City data. The measured values are the average
values for all the data at each measurement point.
Fig. 7. Frequency distribution for the ratio of the measured exha-
lation rate to the calculated exhalation rate for Kobe City data.
J. Radiat. Res., Vol. 50, No. 4 (2009); http://jrr.jstage.jst.go.jp
341
the measured values (p < 0.05). This result suggested that
the artificial structures such as underground pipelines may
affect path of radon. Therefore, we considered that the mea-
sured values were lower than the calculated ones. The
UNSCEAR equation should not be applied where there are
artificial structures such as underground pipelines.
Figure 7 shows the frequency distribution for the ratio of
the measured exhalation rate to the calculated exhalation
rate. The average of this ratio was 0.65, and the measured
values tended to be lower than the calculated values. As can
be seen in Eq. (11), the effective diffusion coefficient for
radon can be expressed in terms of porosity and moisture
saturation. Moreover, many researchers have reported that
water content is a dominant influence on the radon emana-
tion coefficient.3536) It is known that exhalation rate is
affected not only by porosity and water content but also by
environmental factors such as soil temperature, humidity,
and differential pressure.33) In dry soil, the measured exha-
lation rate agreed well with the value calculated using Eq.
(11). For the typically wet soils of Japan, the errors in cal-
culations using Eq. (11) are large, and the calculated values
are higher than the measured ones.37) Therefore, the radon
exhalation rate estimated by substituting Eq. (11) into the
UNSCEAR equation (Eq. (10)) may give erroneously high
values. Temperature dependency of the effective diffusion
coefficient was reported by Schery and Wasiolek38) and
Zhuo et al..39) In particular, Zhuo et al. reported a range of
effective diffusion coefficient of 0.991.07 corresponding to
soil temperatures from 1 to +28C; they estimated the vari-
ation to be less than 10% in typical Japanese environ-
ments.39) Thus, we considered that the effect of soil temper-
ature on the radon exhalation rate was small in our
calculation. Moreover, Iskandar et al. reported that the ema-
nation coefficient is affected by both soil temperature and
water content.40) When we used the temperature data of
Zhuo et al.,39) the radon emanation coefficients increased by
up to 42%. Although UNSCEAR reported that Eq. (10) is
valid for dry soil, the exhalation rate we estimated from Eq.
(10) did not agree well with the measured value, even under
dry conditions.
CONCLUSIONS
In this study, we measured radon and thoron exhalation
rates simultaneously in an area of weathered acid rock in
Kobe City (Hyogo Prefecture) and in Mutsu City and
Higashidori Village (Aomori Prefecture). The measured
radon and thoron exhalation rates fluctuated over a wide
range despite being measured in areas of similar bedrock.
Thus, our results suggest that radon and thoron exhalation
rates are strongly influenced by underground structure. We
found a strong correlation between exhalation rates of radon
and thoron in areas of natural environment. However, there
was no correlation in areas where there were artificial under-
342 M. Hosoda et al.
ground structures. These results suggest that the selection of
measurement locations is very important. Therefore, the
simultaneous measurement of radon and thoron exhalation
rates is important as the data can be used to determine the
validity of a measuring location. We also examined the
application of an equation proposed by UNSCEAR for cal-
culation of radon exhalation rates by comparing our mea-
sured values with those calculated by the UNSCEAR meth-
od. The measured values tended to be lower than the
calculated values and the average ratio of measured value to
calculated value was 0.65.
We concluded that the UNSCEAR equation is applicable
under a controlled environment (temperature, humidity,
etc.), but it is not applicable in an uncontrolled environment,
or where there are artificial underground structures that may
influence the transportation of radon in soil.
ACKNOWLEDGEMENTS
The authors are grateful to Dr. Hideki Kimura of the
Aomori Prefectural Nuclear Power Safety Center, as well as
Mr. Hiroyuki Kawakami of the Higashidori Village office
and Mr. Michio Ito of the Mutsu City office, for their help
in carrying out the measurements in Aomori Prefecture. This
work has been partially supported by the Agency for Natural
Resources and Energy, the Ministry of Economy, Trade and
Industry (METI), Japan.
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Received on November 26, 2008
Revision received on April 23, 2009
Accepted on April 29, 2009
J-STAGE Advance Publication Date: June 9, 2009