WATER RESOURCES RESEARCH, VOL. 25, NO.

8, PAGES 1795-1803, AUGUST 1989

Radon in Groundwater: A Tool to Assess Infiltration

From Surface Waters to Aquifers
E. HOEHN AND H. R. VON GUNTEN 1

Paul $cherrer Institut, Villigen PSI, Switzerland

We measuredthe concentrations
of natural222Rn(half-life3.8 days)in groundwaterat three sitesin
Switzerland; here groundwater is rechargedmainly by river water. Upon infiltration and movement in
the ground, the radon concentration in the water increases by more than two orders of magnitude to
reach a steady state. This increase was found at two of the three sites. At the site of main interest, we
used the ingrowth of radon between the river and nearby observation wells to estimate groundwater
residence times of up to about four half lives. We assumedthat the ingrowth of radon can be described
by the growthlaw of radioactivity,that the progenitorsof radon (226Ra,238U)are homogeneously
distributed in the aquifer, and that the freshly infiltrated water is not mixed significantly with older
groundwater. A linear regressionthrough the data at the site of main interest yielded an average flow
velocity of 4.6 m d-1, which confirmsearlier tracer observations.Radon accumulatesto higher
concentrations, when the top soil layer is frozen or exhibits a high moisture content. During these
conditions the radon data cannot be used for dating purposes.

INTRODUCTION used as a tracer for qualitative investigations. For the

estimation of groundwater residence times, it has so far been
In a large part of Europe, a significant fraction of the
of limited use, due to its short half-life.
groundwater is recharged through infiltration of river water
To investigate the mixing of waters from influent rivers
to water table aquifers [e.g., Triieb, 1977]. The impact of
with older groundwater,chemicalparametersor $•80 mea-
contaminated rivers on groundwater quality is of major
surements are used [Stichler et al., 1986]. Rivers from high
concern. The concentrations of many contaminants in
alpinecatchmentareashavelower $•80 valuesthanground-
groundwater are influenced by infiltrating river water and
water in lowland aquifers [e.g., Siegenthaler und Schotterer,
changenear the rivers dependingon the seasonalconditions
1977]. This difference allows to recognize infiltrated river
in biological activity [e.g., Schwarzenbachet al., 1983; Von
water and to estimate its contribution to an aquifer.
Gunten and Kull, 1986; Jacobs et al., 1988; Kuslys, 1988].
In this paper, we report on radon concentrations in three
For an estimation of the migration of contaminants, it is
shallow glaciofluvial aquifers adjacent to recharging rivers,
therefore desirable to know the flow velocity of the ground-
in the perialpine belt of Switzerland. We sampled ground-
water. Tracing the river artificially is not feasible in general: water from observation wells at various distances from these
large water masses would have to be tagged to observe a rivers. At the site of main interest, we interpreted the results
response in the groundwater. We therefore investigated in terms of flow velocities.
possibilities to use a natural environmental tracer.
Radon (the term "radon" refers here to the radioactive
isotope222Rn)has been used as a tracer in a numberof THEORY

studies of the aquatic environment. Imboden and Emerson

Radon 222 (half-life 3.8 days) is one of the products of the
[1978] and Nyffeler et al. [1983] have studied vertical mixing
radioactivedecayseriesof 238U.It emanatesfrom mineral
processesin Swiss lakes using radon which emanatesfrom
grains by alpha recoil or diffusion. The emanation rate of
the sediments across the sediment-water interface. Among
radon dependsin part on the microstructure of rocks and the
the early measurements of radon, those of Ramsey [1915] environmental conditions. A microstructural view of the
have shown that radon concentrations in shallow springs emanation process of radon in granular aquifers indicates
increase with increasing discharge. More recent investiga- that the grain size distribution, the alteration of grain sur-
tionsin Japandiscussed the 222Rncontentin shallowuncon- faces, and the pore water content seem to be the controlling
fined groundwaters [e.g., Fukui, 1985]. factors for the radon transport [Andrews and Wood, 1972;
Radon concentrationsin rivers are generally low, except Tanner, 1978; Rama and Moore, 1984; Krishnaswami and
in areas where large masses of radon-bearing groundwater $eidemann, 1988]. As an inert gas, radon is quite susceptible
relative to the river exfiltrate into the stream [Rogers, 1958]. to migration. It can diffuse from grain surfaces or nanopores
The low concentrations in rivers are due to a small source
to intergranular space. In water-saturated aquifers, the con-
strengthof the radon in the river bed and due to outgassing tribution of diffusion to the radon transport in groundwaters
to the atmosphereduring turbulent flow conditions. In areas dependson the flow velocity. Diffusion may be an insignif-
where surface waters infiltrate to aquifers, radon may be icant contribution to the overall transport in the deep satu-
rated zone of aquifers, compared to advection. Outgassingto
•Also at Laboratoriumfar Radiochemie,UniversitfitBern, Bern,
Switzerland.
the atmosphere through the unsaturated aquifer depends on
the water content of the soil.
Copyright 1989 by the American Geophysical Union. Chronologies with radionuclides are based on either the
Paper number 89WR00768. decay of a radioactive nuclide, or the ingrowth of a radioac-
0043-1397/89/89 WR-00768505.00 tive daughter product to attain secular equilibrium with its
1795
1796 HOEHN AND VON GUNTEN: RADON IN GROUNDWATER

parent. The ingrowth of a daughter from its parent is neck Canal in the central River Aare valley (Figure l c), both
described by Switzerland.
Figures l a through l c show schematicallythe placement
At = Ae[1 - exp(-At)] (1)
of the wells and pipes used for this study, at the three sites.
where A t is the activity of the daughternuclideat time t (here The wells are located at different distances from the river
t is assumedto be the residencetime); A e is the activity of bank (Table 1). The polyvinyl chloride (PVC) piezometer
daughter at secular equilibrium with parent nuclide; and ,• is pipes are screenedwith rows of slots. The slotted sectionsof
the radioactivedecayconstantof daughter,(i.e., 0.18day-1 most pipes are located in the shallow part of the saturated
for 222Rn).The activityis proportionalto the concentration aquifer. Table 1 shows that the screens extend over short
(Ax = ,•.Nx, where Nx is the numberof atomsof nuclidex). vertical distances. Wells G2, G4, and G6 are "bundled
Upon infiltration of water from a river with negligible piezometers"; such wells are composed of two or three
radon concentration to the shallow aquifer, the radon con- pipes in the same borehole [Cherry et al., 1983]. With this
centration increases with increasing residence time in the set-up it is possible to sample groundwater from different
ground to reach concentrations indicative of a steady state. depths of the aquifer. In this paper we use the following
The steady state between radium (and other progenitors in notationfor the pipes of a bundle: s, shallow, m, middle, and
the decaychainof 238U)andemanatingradonis, for practi- d, deep.
cal purposes, establishedafter a residence time of about 20 The aquifer in the Glatt valley consistsof tightly packed
days (about five half-lives); then, the radon concentration in glaciofluvial outwash deposits, which are 25-30 m thick.
the water is approximately equal to its supply [Krish- Core material from wells G1, G2, G4, and G5, showed
naswami et al., 1982]. interbedded layers of poorly sorted sands and gravels con-
It should, in principle, be possible to apply (1) for an taining quartz, calcite, dolomite, and aluminum silicates. A
estimation of the residence time of freshly infiltrated water in detailed descriptionof the River Glatt valley aquifer is given
a field situation. An application is, however, limited by the by Hoehn et al. [1983]. At the River Aare site and the
validity of the following assumptions:(1) the average distri- Hagneck Canal site, the aquifer formation is of a similar
bution of the radon progenitors(i.e., uranium and radium) in sedimentological and mineralogical composition as at the
the aquifer materials is homogeneous on a macroscopic River Glatt site [Jtickli und Ryf, 1978; Kellerhals und
scale; (2) the steady state radon concentrationsmeasured at Haefeli, 1989].
greater distances from the river are representative of the The River Glatt meanders in the valley and recharges the
investigated water flow path; (3) losses of radon from the aquiferovera distanceof about3 km at a rateof 0.4-0.8 m3
groundwater to the unsaturated aquifer and to the atmo- d-1 per squaremeterinfiltrationarea.The widthof the river
sphere are constant; (4) the flow distance of the water to a is about 18 m. The direct contribution by precipitation to
samplingwell is constant even in the case of varying water aquifer recharge is negligible at this study site [Hoehn and
table elevations; and (5) the infiltrating water does not mix Santschi, 1987]. Water which has infiltrated from the river
with older groundwater. penetratesthe uppermost part of the saturated aquifer with-
The method for the estimation of residence times relies on out a significantdispersion in vertical direction, due to the
concentrations relative to a steady state, rather than on stratification of the aquifer. Admixture with older ground-
absolute values. If initial and steady state values are known, water is negligiblein the top part of the aquifer but increases
the values in-between allow to make this estimation. with depth. Details of the flow pattern were obtained by
The pronounced differences in radon concentrationsbe- Hoehn and Santschi [1987] in a study of tritium transport.
tween surface water (essentially zero) and steady state in The hydraulic situation at the River Aare site is qualita-
groundwater may also be used for a qualitative measure of tively similar to that at the River Glatt site, the recharge rate,
infiltration or exfiltration. If a significant infiltration exists, however, is unknown. The Hagneck Canal recharges the
groundwater collected close to the shore of surface waters aquiferat about0.3 m• day-1 per squaremeterinfiltration
(rivers, lakes, estuaries, and shallow basins of the sea) will area [Kellerhals und Haefeli, 1989].
always show radon concentrations which are lower than
steady state. On the other hand, exfiltrating groundwater METHODS
may be detected in surfacewaters. Under certain conditions
exfiltration may be quantified [Rogers, 1958]. Sampling
After flushing the test wells with 2-3 well volumes to
EXPERIMENTAL SITES
remove stagnant water, we sampled the groundwater into
An experimental site was used in the valley of the River sphericalglassflaskswith a narrow neck (volume about one
Glatt, Switzerland (Figure la). It represents a common liter) using a submersible pump (COMET, D-6239 Kriftel,
hydrogeological situation of the perialpine belt of central Federal Republic of Germany) at a flow rate of less than 1 L
Europe [Hoehn et al., 1983]. At this site, the behavior of min-1. This flow rate minimized the disturbance of the local
contaminants during infiltration of the water from the River groundwaterflow and reduced lossesof radon by outgassing,
Glatt to unconfined groundwater has been studied by and it yielded reproducible results. The sampling tube was
Schwarzenbach et al. [1983], Von Gunten and Kull [1986], placed at the bottom of the glassflask to minimize escapeof
Waber et al. [1987], von Gunten et al. [1988], Jacobs et al. radon. The glassflasks are filled with water up to the narrow
[1988], and Kuslys [1988]. Radon was measured at this site neck. The amount of water sampled was measured by
between May i985 and July 1987.-To check a m6re gen6ral weighing.In order to ensurethat only the fresMy infiltrated
applicabilityof the method, three radon measurementswere water was sampled,we maintainedthe samplingpositionin
made in summer 1987at a site in the lower River Aare valley the pipes of the wells at 0.5 m below the groundwater table
(Figure lb), and four measurements 1987/1988at the Hag- and within the screenedsectionof a well, in most cases.Due
 HOEHN AND VON GUNTEN: RADON IN GROUNDWATER 1797

distance --100 m

375 -

370-
.... '..... GiG•G3_.
I[[--G4m
IGS s
{?rn
;[
365-
GROUNDWATER
FLOW{iG2d
! WATER
I
360-- = 'LEVEL
,

355 -
• • -• AQUIFER
5m G7 'G8

LOWER CONFINING BED

•/. Ca v ,/'--'/--'•-- ß--,..... GROUND-

I- I 'A2 •A3 --
GENEVA •--J310 LEVEL
<• AQUIFER

I ' I
5m

•• 445 HAGNECK
C AL __•
H1
Q _• • ..• .... •._ GROUND-
• 440 • ' --'- •'- WATER
• 435
• •, AQUIFER •' LEVEL
5m

Fig. 1. Location and schematiclayout of study sites:(a) River Glatt site, (b) River Aare site, and (c) Hagneck Canal
site. For distancesand depths of wells and pipes from surfacewaters and depths of pipes, see Table 1. Dashed lines'
screened sections of pipes.

to changinggroundwater levels it was, however, not always TABLE 1. Technical Details of Wells Shown in Figure 1
possible to follow this procedure. Deeper groundwater was
Linear Distance Upper and
sampled within the screened sections of wells located en- From River Lower Depth
tirely in the saturated zone. Well Bank to Well, of Screen,
No. m m Remark

Extraction River Glatt Site

2.5* 374.0-372.1 inclined at 35 ø
We adoptedanextractionmethodof HoriuchiandMura- G2s
G1 5.0 373.8-370.8 shallow pipe of bundle
kami[1979,1981]for thedetermination
of radonby liquid G2m 5.0 368.9-366.9 middle pipe of bundle
scintillationcounting(LSC). Immediatelyafter sampling,20 G2d 5.0 364.9-362.9 deep pipe of bundle
mL of a toluene-based liquid scintillator (LS; Packard) was G3 7.0 370.7-367.7
14 374.0-371.0 shallow pipe of bundle
addedin the narrow neck of the flasks. The presenceof G4s
14 369.0-367.0 middle pipe of bundle
toluene
ontopofthewatersample
reduced
thelossofradon G4m
G4d 14 365.0-363.0 deep pipe of bundle
drastically
dueto a distribution
coefficient
toluene/water
of G5 26 373.3-364.3 diameter 4 inch
45 at 20øC. [Horiuchi and Murakami, 1979]. In the labora- G6s 100 370.5-367.5 shallow pipe of bundle
tory, radon is extracted into the LS by vigourous shakingfor G6m 100 366.2-363.2 middle pipe of bundle
5.0 354.3-351.3 deep well
5 min,with subsequent
pipetting
(aftercleanseparation
of G7 100 357.8-354.8 deep well
thetwophases)
of10mLoftheLSintoacounting
vial.After G8
River Aare Site
addition of an other 10 mL of LS, the procedure was
A1 4.0* 318.9-317.2 inclined at 35 ø
repeated to increase the overall yield (extraction and count- A2 6.5 318.9-316.9
ing) from 50 to about 75%. A3 11 317.8-314.5

Hagneck Canal Site

Counting H1 14 442.7-432.7
H2 33 444.0-434.0
Radon disintegrates through a series of four short-lived
daughter products, and radioactive equilibrium is estab- *From river bank to screened section.
1798 HOEHN AND VON GUNTEN: RADON IN GROUNDWATER

lished about 3 1/2 hours after the extraction. The fifth are large temporal fluctuations in the radon concentrations in
daughter,2•øpb(half-life22 years),doesnot affectthe radon groundwater. Two types of variations may be distinguished:
measurements.Integral counting of the a and/3 radiation of (1) fluctuations which arrive almost simultaneously in all of
radon and its daughterswith an LSC was used. The samples the observation wells and (2) fluctuations which occur in a
were analyzed 10-30 hours after sampling, in general, and limited number of wells (often in only one). After omission of
more than 3.5 hours after extraction, allowing ample time for the largest fluctuations, the expected increase of the radon
the radon daughters to reach radioactive equilibrium. LSC concentrationswith increasingflow distance (equation (1)) in
lasted one hour for each sample. The counting error (1rr) was the aquifer is evident. In the following sections we evaluate
always less than 10%. and explain the observationsand give possibleexplanations
We used LSC after 1985. In 1985, the radon concentra- for the fluctuations mentioned above.
tions were obtained from measurementsof the 609-keV 7
Radon Distribution at the River Glatt Site
raysof 2•4Biusinga Ge(Li) detector.The two methodswere
normalized by comparing several sampleson the two detec- Horizontal distribution. At the River Glatt site, radon
tion systems. builds up in the infiltrating water with increasing flow dis-
The radon concentrationat the time of sampling,N O, is tance from the river (wells G 1 to G6, at shallow depths). This
calculated from the counting rate, A = AN, see above, as is attributedto the ingrowthof 222Rnemanating
fromaquifer
grainswhichcontain226Ra,mainlyfrom grainssmallerthan
No = N exp [At'(f/V)] (2)
2 i•m [Surbeck and Voelkle, 1987] which make up 0.5-2.0
where V is the volume of the water sample, t' is the time weight percent of the studied outwash deposits. The ob-
elapsed between sampling and counting, and f is the overall served ingrowth to the water with increasing infiltration
yield (extraction and counting) of the procedure derived distance is in reasonably good agreement with (1). In pipe
from the measurement of 226Ra standard sources. The con- G6s, at 100 m distance from the river, we assume a steady
centrationsN and N Oare given in Becquerelsper liter (Bq state radon concentration for the shallow groundwater. The
L-•) (1 Bq = onedecay/second).
The detectionlimit of both values between river and steady state cover more than two
methodsis about0.02 Bq L -•. ordersof magnitudein 222Rnconcentrationandallowa more
detailed analysis (see below). Although we did not measure
Laboratory Experiment the contents of radium in the soil or the groundwater, the
assumption of a rather homogeneousspatial distribution on
The basic assumptionsof the radon method were tested in
the scale of a few meters seemsto be fulfilled approximately.
a sandbox designedfor two-dimensional flow investigations
This agrees with results of Pearson and Jones [1965], who
[Stauffer and Dracos, 1986]. In this experiment, tap water
found no horizontal gradients of radon concentrations in
containing no radon was allowed to flow through the box at
a constantvelocity of about 0.5 m d-I; the water needed their study of the unsaturated zone.
Vertical distribution. In Table 3 we compare the radon
about 10 days to pass the box. We monitored the water
concentrations at different depths of the aquifer: (1) at 5 m
residence time at seven probes by electrical conductivity
distance from the river, (2) at 14 m distance, and (3) at 100 m
with a step input of a salt solution. These probes also
distance. Near the river, the vertical distribution is different
allowed to sample water for radon measurements. We fol-
from that farther away. We found concentrations increasing
lowed the ingrowth of radon as a function of time and
with depth. The low concentrations just below the ground-
distance. The steady state radon concentration was obtained
water level in pipe G2s result from the freshly infiltrated
after the experiment from water which was left in the tank
water. At greater depth one assays older water with a larger
for 30 days. The residence times of the water based on the
residence time in the ground and therefore with higher radon
radon measurements agreed with the breakthrough of the
concentrations. The highest radon concentrations were mea-
salt solution. The results of this laboratory experiment
sured at 20 rn depth in well G7. At this depth outgassingto
confirmed that the ingrowth of radon is governed by radio-
the unsaturated zone is negligible. Tritium measurements in
active laws (equation (1)).
well G7 showed an age of more than 2 years [Hoehn et al.,
Errors
1983].
With increasing distance from the river, the radon concen-
Based on multiple measurements of samples from the tration gradient diminishes such that shallow groundwater
samewells, the extractionof 226Rastandardsolutions,and finally reaches the steady state. At 100 m distance the
tests for Rn losses, we estimate the overall errors to be in the difference in the radon concentrations between well G6s and
order of +20%. They include uncertainties in sampling, in the deep well G8 amounts to only about 20%. This is in
the chemical procedure, and the counting statistics. agreement with results of Fukui [1985], who assumed diffu-
sional losses of dissolved radon to the unsaturated zone of
RESULTS AND DISCUSSION
the aquifer and to the atmosphere. The depth dependenceof
Radon has been measured in the rivers and the wells, radon concentrations in the near field of infiltration creates
shown in Figure 1. The results of all the measurementsin the problems in the measurementsduring transient groundwater
wells are presented in Tables 2-6. Measurements in the flow conditions, i.e., changing groundwater levels.
surface waters of the three sites showed radon concentra- Temporal variations. Figure 2a shows time series mea-
tionsto be between0.1 and 0.4 Bq L -•. Radonconcentra- surements of radon concentrations in selected wells (for all
tions in rain have been reportedby Andrews and Wood values see Table 2). Most of the temporal variations can be
[1972]to be at about0.1 Bq L -•. explained by special climatic conditions and/or by the vari-
It is evident from Table 2, which presents the complete able groundwater levels. Figure 2b shows that the ambient
data set for the main wells at the River Glatt site, that there air temperatures dropped below freezing in both winters of
 HOEHN AND VON GUNTEN:RADONIN GROUNDWATER 1799

TABLE 2. Radon Concentrations in Wells of River Glatt Site

Date G1 G2s G2m G3 G4s G4m G5 G6s G7

1985
May 14 2.6* ...... 7.6* '" 7.2* .........
June 11 6.7* ...... 13' "' 7.4* .........
July 2 6.6' ...... 11* '" 7.9* .........
July 23 4.0* ...... 13' "' 7.5* .........
August 13 7.0* ...... 13' '" 7.4* .........
September 5 4.8* ...... 13' '" 11' .........
October 1 7.1' ...... 12' '" 12' .........
1986
January7 9.5 '" 15 9.2 -" 16 18 18 15
January28 6.3 -" 8.9 6.6 '" 14 14 14 -"
February4 9.2 ............ 9.9 '" 15 20
February17 13 '" 13 15 '" 20 21 20 25
March 11 15 '" 20 13 "' 21 22 21 27
March 18 7.4 '" 18 11 '" 21 ...... 26
March25 6.1 '" 12 10 '" 18 22 21 26
April 4 6.1 '" 14 12 ...... 22 21 25
April 14 2.2 '" 8.7 7.7 ......... 14 24
May 6 2.6* '-' 7.4 8.0* '" 8.0 9.5* 15' 23
May 20 3.4* '" 9.0 8.5* '" 8.3 10' 17' 26
June3 3.9* 6.9* '" 5.8 10' '" 10' 18' 26
June16 3.3* 6.2* "' 12 9.0* '" 11' 16' 25
June30 3.2* 6.0* "' 13 10' '" 10' 15' 26
July 14 3.8* 6.2* --' 15 10' '" 13' 16' 26
July28 4.0* 6.1' '" 15 8.4* '" 14' 16' 26
October1 4.4* 7.0* '" 14 7.2* "- 15' 16' 27
October28 5.1' 8.7* '" 11 12' "' 14' 16' 24
December2 5.0* '" 15 12' '" 12 14' 17' 23
December23 6.3* '-' 15 12' "' 11 14' 18' 24
1987
January13 ...... 16 14 '" 14 15 17 24
January20 6.9 '" 18 15 '" 16 17 18 25
January26 8.8 '" 21 19 '" 18 18 20 26
February3 7.6 '" 18 12 '" 16 17 19 23
February10 8.1 "' 18 18 '" 15 17 18 24
February24 8.5 '" 17 17 '" 15 17 19 21
April 22 8.0 '" 18 18 '" 15 15 19 25
May 25 5.8* '" 17 17' "' 15 16' 19' 24
July 14 5.1' 6.8* '" 14 10' '" 14' 17' 27

All measurements
aregivenin Becquerels
perliter;errors+20%.Average
RiverGlattconcentrations
is 0.1BqL-•.
*Valuesselectedfor groundwater
datingwith radon,seeTable4, Figure3 andtext.

the measurement period.Duringthe coldseason(February- Theseeffectswerelesssignificant

in early 1987probablydue
April, 1986andJanuary-March,1987),the groundsurfaceat to the fact that the soil moisture content was lower before
the sitewas oftenfrozenand snow-covered. In winter 1986, freezing. We attribute the enrichment of the radon in the
the soil moisturewas high before the long-lastingcold groundwaterin periods with frozen and water-saturated soils
weatherstarted.Air temperatures belowfreezingeffectively to a restricteddiffusionfrom the unsaturatedaquiferto the
cappedthe unsaturatedzone,causinga sharpincreasein the atmosphere.Pearson and Jones [1965] observed a marked
radon concentrationsin the shallowgroundwater.Radon
decreasein the rate of radonemanationfrom the soilgasof
concentrations duringthis periodof unusuallycold weather
the unsaturatedzone to the atmosphere,in periods with
were ultimatelyhigherthan normal, by a factor of about 2.
frozensoils.The soilmaystillretardradonemanationduring
thaw, when melting ice and snow form a seal at the soil
TABLE 3. Vertical Distribution of Radon in Groundwater at surface. Due to the restricted emanation of radon, the
River Glatt Site
measurementsmade during the winter months are not suit-
Linear DistanceFrom River Bed to Well, m able for an estimationof groundwaterresidencetimes (see
Depth Below below).
Groundwater 5.0 (G2, G7), 14(G4), 100(G6, G8), Heavy rainfall in springof 1986led to a significantrise in
Level, m June1986 June1986 May 1987 the groundwatertable, shownin Figure 2c. The rise of the
0.5 6.0 10 19 groundwater table to above the filter screens of well G3
3.0 13 14 21 correlates with the increasingradon concentrationsin this
6.0 22 20 '"
15 ...... 22
well, shownin Figure 2a. Keepingthe samplingpoint at a
20 26 ...... constant elevation within the screened section of well G3
resultedin an increaseddepthof the samplingpointfrom the
All valuesare givenin Becquerelsper liter. Errors +20%. groundwatertable. Hence the deepergroundwatersampled
1800 HOEHN AND VON GUNTEN: RADON IN GROUNDWATER

TABLE 4. Radon Concentrations (Means and Standard Deviations) and Corresponding Residence
Times at River Glatt Site

Estimated Radon
Linear Distance Effective Flow Number of Concentrations, Residence
Well From River Bank Distance,m Measurements Bq L -• Time, days
G1 2.5 13.5 20 4.7 - 1.5 1.8 _ 0.06
G2s 5.0 16 8 6.7 - 1.0 2.8 _ 0.04
G3 7.0 18 12 11 - 3 6.4 _ 1.4
G4 14 25 15 9.1 - 1.7 4.2 _ 0.08
G5 26 37 13 13 _ 2 7.9 _ 1.3
G6s 100 111 13 17 _ 1' >15

Selected measurements from Table 2.

*Assumed to be at steady state.

under these conditions contained higher radon concentra-
tions.
The high groundwater table allowed samplingin the shal-
lowest pipes of the bundled piezometers, G2s and G4s,
between June and October 1986 and again in July 1987.
During the rest of the time, samplingwas performed in the
middle pipes of the bundles. Moving from pipe G2s to G2m
in December 1986 and back in July 1987 resulted in the
changesof the radon concentrations, as shown in Figure 2a.
The relatively low radon concentrationsin well G7 in early
1986 may be artifacts due to incomplete flushingof the well.
The radon in the stagnant water of the well was not in
contact with the aquifer grains and therefore not supported
by its radium parent.
After April 1986, well G1 showed a continuous rise in
radon concentrations.With the groundwater level remaining
essentially constant in this well, we postulate that local
cloggingof the river bed or changesin the water flow path
may lead qualitatively to the observed effect.
Residence times andflow velocities. The results allowed
an estimation of groundwater residence times between the
river and the wells and the correspondingflow velocities. We
calculated means and their standard deviations of radon
concentrationsselectedfrom measurementsgiven in Table 2
and present them in Table 4. The selectedvalues are labelled
in Table 2 with an asterisk. We omitted measurements(1) of
the winter months becauseof restricted radon outgassing;(2)
of samples collected significantly deeper than 0.5 m below
the groundwater table; and (3) of samples not collected
within the screened section of the wells.
We then solved (1) for t, of which we assume that it
represents the residence time, using the radon concentra-
tions of Table 4. The residencetime is the time elapsedfrom
the moment of infiltration of river water into the subsurface
to the moment the water reaches a well. We assumed that
the mean value of pipe G6s in Table 4 of 17 Bq L -• is
approximately the steady state concentrationof radon in the
groundwater at shallow depths. A residence time of more
than 15 days for the flow to this well, calculated with the
radon method, agrees with the value of about 18 days of
Hoehn and Santschi [1987] and Santschi et al. [1987]. These
authors reported the effects of a pulse of tritiated water
(about 500 Ci) accidentally dischargedinto the Glatt River,
which resulted in a tritium plume infiltrating to the ground-
water. A residencetime of about 8 days for the flow to well
G5, calculated with the radon method, compares with the
highest tritium concentration measured in this well after 7
days.
In Figure 3 we plot the residencetimes (Table 4) obtained
with the radon method versus the distance of the wells from
the right-hand-side river bank. The plot suggestsa linear
relationship (except well G3). Zero residence time of this
linear regressionpoints to a mean infiltration boundary near
the center of the river bed (about 11 m distance from the
right bank).
The linear regressionthrough the data points of Figure 3
yieldsan averagegroundwaterflow velocity of 4.6 m d-•.
This agreeswith valuesof 3-6 m d-• of Hoehnand Santschi
[1987] obtained from the tritium plume. For the calculation
of the flow velocity, these authors measured, however,
linear flow distances to the wells starting from the river
bank, rather than from the center of the river. Had they
added to their flow distances the 11 m between the center of
the river and the bank, as is suggestedhere, their values for
flow velocitywouldincreaseto 4.4 and6.1 m d-•, for wells
G5 and G6s, respectively.
The radon concentrationsof well G3 correspondto longer
than average residence times. Some of the measurements
(e.g., May 6 and 20, 1986) show concentrations of 8-9 Bq
L-•, valueswhichwould yield a residencetime of about4
days and hence would agree with the straight line of Figure
3. Possible explanations for the seemingly long residence
times at well G3 are (1) enhanced mixing with older ground-
water and (2) flow through less permeable layers at different
TABLE 6. Radon Concentrations at Hagneck Canal Site

Well HI Well H2
TABLE 5. Radon Concentrations in Groundwater at River Aare
Site Date Radon $•80 Radon $•80

Date Well A1 Well A2 Well A3 September 1987 19 - 12.68 17 - 11.33

May 1988 11 - 12.87 22 - 12.69
April 1987 13 16 14 June 1988 11 - 12.89 19 '"
May 1987 15 16 13 November 1988 19 = 11_77 21 - 11.99
October 1987 17 19 '"
All values are given in Becquerels per liter; errors ___20%.Here
All values are given in Becquerelsper liter; errors ___20%.
River •80 valuesare givenin per mille; errors _+0.04.HagneckCanal:
Aare concentrations
are 0.4 Bq L -•. Radon0.1 Bq L -• and •80 -13.16.
 HOEHNANDVONGUNTEN:
RADON
IN GROUNDWATER 1801

3O

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A S 0 N D J F M A M J J A S 0 N D J F M A M J J
1985 1986 1987
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1985 1986 1987

Fig.2. Selected
timeseries
measurements
attheRiver
Glattsite(foralldataseeTable2):(a)radonconcentrations
(errors
-+20%)'
(b)ambient
temperatures
(5day's
means)'
and(c)water levels. Solid
squares,
River Glatt;
open circles,
wellGI' open
squares,
pipeG2s'open
squares
withpoint,
pipeG2m; open triangles,
wellG3;solidinverted
triangles,
pipe G6s' andopeninvertedtriangles,well G7.
1802 HOEHN AND VON GUNTEN'
RIVE
RGLATT A•'••r•G•
iG1 F-I'.....
G2s',
+ '- ....
I •
15m I
I tration/exfiltration) dependingon the canal's water level.
I
I
I uranium
I
I I
-10 0 10 20
DISTANCE FROM RIVER BANK,m
Fig. 3. Dating with radon' (a) schematic cross section of River
Glatt site and (b) linear regressionthrough data points from Table 4
(r = 0.63; errors: mean statistical errors).
groundwater levels leading to longer effective distancesfrom
the river. Both explanations disagree with our model as-
sumptions.
We know little about the infiltration processalong a flow
line at distances of less than 2.5 m from the river
banks. It is not possibleto install wells at a location closer to
the river because of the man-made bank consisting of large
and uneven granite blocks. The effect of temporal cloggingof
the river bed may result in a much lower hydraulic conduc-
tivity, and the effect of the variable river stage results in
varying hydraulic gradients. Both processes affect the
groundwater flow velocity and thus the radon distribution
near the influent river. Here the ingrowth of the radon
concentration exhibits a steep gradient, thus small changes
of flow velocity result in big changes of radon gradients.
Radon Distribution at Two Other Sites
To compare with the results of the Glatt River site, we
measured the distribution of radon concentrations
other sites, near a losing river and a losing canal. The results
of three measurements made at the River Aare site during
summer 1987 (Table 5) differ from the measurements at the
River Glatt site. Here, steady state concentrations of radon
were found in all the wells, pointing to residencetimes of the
groundwater between river and wells of more than 15 days.
Schwarzenbach et al. [ 1983] estimated residence times of the
groundwater of up to 1 month from a delayed responsein the
groundwater to the seasonal temperature extrema and to
high concentration spikesof chlorinated hydrocarbonsin the
River Aare.
The results of four recent measurements at the Hagneck
Canal site (Table 6) differ from those of the two sites
discussedabove. Here steady state radon concentrations are
found in fall (September/November), pointing to residence
times of the groundwater of more than 15 days. Infiltration of
water from the canal is, however, evident from lower radon
concentrationsduring the early summer months (May/June),
when the water level in the canal is high. The concomitant
/5•80 measurements indicated absence of infiltration with
values between - 11 and - 12 per mille in fall, except for well
RADON IN GROUNDWATER
H1 in September,1987. The 8180 measurements
in early
summer supportthe results of the radon method. The radon
and the oxygen isotope measurementscorroborate observa-
tions of Kellerhals und Haefeli [1989], who reported a
change in the hydraulic gradients of the groundwater (infil-
At the Aare River and the Hagneck Canal site, the steady
state radon concentrations of the shallow groundwater of
about17-22Bq L-1 are, withinthe accuracyof our method,
in agreement with those at the Glatt River site. Thus the
and radium contents seem to be rather constant and
more or less uniformly distributed in all these glaciofluvial
outwash deposits, independent of their origin from different
areas.
APPLICABILITY OF THE METHOD
The radon method may be used to quantify the flow
velocity of the freshly infiltrated water, when the following
conditions are fulfilled: (1) the steady state radon concentra-
tion at a site has to be known for at least one well which is
located at a sufficiently large distance from the infiltrating
surface water (residence time must be more than 20 days);
and (2) at least one additional well must be installed at a
location, for which the residence time t of the groundwater is
between 0.5 and 8 days. These constraints result from the
width of the time window which is applicable, based on (1),
bed and the half-lifeof 222Rn(3.8 days), and the estimatederrorsof
the methodof _+20%. At the flow velocitiesof about5 m d-•,
which are typical for perialpine outwash aquifers, wells
giving access to freshly infiltrated water should thus be
located between 2 and 40 m, with the well for the steady
state condition at a distance of more than 100 m. Our
assumptionof an ingrowth of the radon accordingto the laws
of radioactivity is a large oversimplification. Besides the
ingrowth of the radioactivity, several transient processes
occur which complicate an accurate mathematical modeling
very much, e.g., variations in the rate of outgassing, mixing
with increasingflow distance, and dispersion.
CONCLUSIONS
at two We have measured the radon concentrations in groundwa-
ter wells at three sites which are instrumented for the study
of the infiltration of river water to groundwater and arrive at
the following conclusions:
1. In freshly infiltrated groundwater, radon builds up with
increasingflow distance from the river where the concentra-
tions are very low. The ingrowth can be approximated with
the laws of radioactivity.
2. The radon method allows dating of infiltrating surface
water to groundwater. This is an advantage over other
methods. Residencetimes of the water in the ground of up to
about 15 days, i.e., about four half-lives of the tracer, and
related groundwater flow velocities can be obtained, under
favorable conditions.
3. Knowledge of steady state radon concentrations and
radon measurements in at least one well near the infiltration
boundary are necessary. For the glaciofluvial outwash sed-
iments studied here, the samplingwells should be located at
flow distancesbetween 2 and 40 m and at more than t00 m
for an estimation of the steady state condition.
4. Radon concentrations in the water of shallow water
table aquifersare influencedby the rate of outgassingto the
 HOEHN AND VON GUNTEN:
atmosphere. If the soil is frozen or has a high water content,
radon accumulates to higher concentrations in the ground-
water.
5. Based on the fair agreement of the measured steady
state radon concentrations we conclude that the uranium and
radium concentrations in the aquifer material are rather
similar at the three investigated sites with glaciofluvial
outwash deposits of a different origin.
Acknowledgments. We thank Th. Dracos, F. Stauffer, and Ch.
Haefeli for providing experimental facilities and related discussions.
We thank D. Baccala, W. G6rlich, G. Karametaxas, M. Kuslys, and
C. Vogel for their assistance, A. Grfitter, H. H. Loosli, and H.
Surbeckfor discussions,
and U. Siegenthaler
for the $•80 measure-
ments. H. Gfiggeler, B. Honeyman and the two anonymousreview-
ers improved the manuscript through critical comments and propo-
sitions. E. R6ssler drew the figures. The work was partly supported
by the Swiss National Science Foundation.
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(Received October 3, 1988;
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