Environmental Pollution 129 (2004) 31–37

www.elsevier.com/locate/envpol

Constraints on the use of 137Cs as a time-marker to support CRS

and SIT chronologies
J.M. Abril*
Dpto. Fı´sica Aplicada I. University of Seville, E.U.I.T.A., Carretera de Utrera km 1, D.P. 41013. Seville, Spain

Received 12 April 2003; accepted 3 October 2003

‘‘Capsule’’: Simple methods based on the identification of 137Cs fallout peaks cannot provide a definite support for CRS
and SIT chronologies.

Abstract
CRS and SIT are two 210Pb-based models widely used in the radiometric dating of recent sediments. 210Pb chronologies should be
validated using at least one independent tracer, such as 137Cs. This paper demonstrates that simple methods based on the identifi-
cation of 137Cs fallout peaks cannot provide a definitive support for CRS and SIT chronologies. Two main arguments will support
this assertion: Firstly, the 137Cs time-marks cannot support a CRS or SIT chronology if the derived sedimentation rates cannot
explain the whole 137Cs activity profile without postulating mixing. Secondly, the support by the 137Cs time-marks for a given CRS
or SIT chronology cannot be considered as definitive if other dating models can equally explain the whole set of data, thereby
producing a different chronology. Several case studies selected from the literature are used to support the present discussion.
# 2003 Elsevier Ltd. All rights reserved.
Keywords: Sediment dating; 137Cs dating; CRS model; SIT model; 210Pb dating

1. Introduction and no post-depositional mixing. In this model the

Studies on the behaviour of particle-associated tracers
in aquatic sediments are of widespread interest. Thus,
radiotracers can provide valuable information on
mixing and rates of sedimentation. This information is
necessary for the interpretation of historical records of
particle-associated substances in sediment cores and for
the study of the behaviour of hazardous chemicals.
The 210Pb dating method is widely applied in the
study of recent (up to 130–150 years) accumulation
rates in sediments, peat bogs and other natural deposits.
A summary of the 210Pb cycle in nature and a review of
the most common dating models for 210Pb can be found
in Robbins (1978). The simplest situation corresponds
to a constant 210Pb flux and a constant sedimentation
rate; whereby the 210Pb activity profile follows an
exponential decrease with mass depth.
The CRS model (Appleby and Oldfield, 1978)
assumes a constant rate of supply of unsupported 210Pb
* Tel.: +34-954486420; fax: +34954486436.
E-mail address: jmabril@us.es (J.M. Abril).
0269-7491/$ - see front matter # 2003 Elsevier Ltd. All rights reserved.
doi:10.1016/j.envpol.2003.10.004
sediment accumulation rate can be variable, (e.g. the
specific 210Pb activity decreases when the sedimentation
rate increases). This model is widely known and applied;
and updated presentations can be found in Appleby
(1998) and Appleby (2001).
The SIT model (Carroll et al., 1995,1999) allows the
interpretation of 210Pb profiles which result when both
sediment accumulation rates and the 210Pb fluxes vary
with time. This model assumes that there is no post-
depositional redistribution of radionuclides (mixing
processes). Non-exponential changes in 210Pb activity
caused by sedimentation are modelled by a Fourier sine
series while changes produced by other processes
(changes in 210Pb fluxes) are modelled by a Fourier
cosine series. Once the average sedimentation rate and
the present day surface value of the 210Pb concentration
have been stated, the values of the Fourier coefficients
are determined from the measured data by inverse
numerical analysis. The interpretation of sediment ages
gives an age range for each depth interval, which is then
presented as a probability distribution. Historical events
(such as represented by the 137Cs time-marks) can then
32 J.M. Abril / Environmental Pollution 129 (2004) 31–37
be used to constrain the probability distributions of
sediment ages. Applications of the SIT model can be
found in the aforementioned references and, among
others, in work from Waugh et al. (1998) and Somaya-
julu et al. (1999).
The IMZ model (Abril et al., 1992) assumes the
existence of a mobile fraction in radionuclide activity
(dissolved radionuclides, and those attached to colloids
and very small particulate matter), which is rapidly and
homogeneously mixed (through the connected pore
water) within a top zone in the sediment core. On the
other hand, settled particles have an irreversibly boun-
ded fraction of activity, and can undergo aggregation
processes in which part of their free surface becomes
unavailable for any further radionuclide exchange.
The model approaches this situation assuming that a
fraction g of the incoming flux undergoes a fast and
complete mixing within a top sediment zone of mass
thickness ma, while the remaining fraction does not fol-
low any post-depositional redistribution. This model is
applicable for 210Pb and for fallout radionuclides with
time-dependent fluxes (such as 137Cs). The correspond-
ing analytical solutions and some applications can be
found in Abril et al. (1992) and in Abril (2003).
Difficulties arise when the same 210Pb data can be
explained by different models leading to different
results. Thus, constant 210Pb activities often found in
top sediment layers can be equally explained by a
change in sedimentation rate or by a mixing zone with
high diffusion (Robbins, 1978). Moreover, Smith (2001)
proposed a protocol for research journals for the
acceptance of papers that rely on 210Pb dating to
establish a sediment core geochronology: ‘‘The 210Pb
geochronology must be validated using at least one
independent tracer which separately provides an unam-
biguous time-stratigraphic horizon’’. Therefore, the
simultaneous study of man-made fallout radionuclides
such as 137Cs, 239+240Pu or 241Am (with a well-defined
peak in atmospheric deposition occurring in 1963)
represents a valuable and necessary additional test for
210
Pb chronology.
Many applications involving artificial fallout radio-
nuclides automatically associate the year 1963 to the
sediment layer where a peak in activity occurs, or use a
similar approach with other time-markers (for example,
von Gunten et al., 1987; Waugh et al., 1998; Santschi et
al., 2001). Furthermore, in the cases with constant 210Pb
activity in the topmost sediments, the presence of a dis-
tinct 137Cs peak within the 210Pb plateau has been used
as a definitive demonstration of acceleration (increase in
the sedimentation rate in recent years) versus fast mix-
ing (Appleby, 2000, 2001). Abril (2003) pointed out
limitations in the use of such qualitative arguments. In
particular, this author demonstrated how the incom-
plete mixing within the top sediment zone (described
through the IMZ model) could quantitatively and
simultaneously explain the presence of a distinct 137Cs
peak and the flattening in the 210Pb activity profile. This
paper represents a further advance on these ideas, and
tries to demonstrate that simple methods based on the
identification of the fallout (and the Chernobyl) peaks
cannot provide a definitive support for CRS and SIT
chronologies. Two main arguments will support this
result: Firstly, 137Cs time-marks cannot support a CRS
or SIT chronology if the derived sedimentation rates do
not explain the whole 137Cs activity profile without pos-
tulating mixing, since both models are based upon the
assumption of no post-depositional effects. Secondly,
137
Cs time-marks cannot unambiguously support a CRS
or a SIT chronology when other dating models can
equally explain the whole set of data and produce a dif-
ferent chronology. Several case studies selected from the
literature will be used to support the present discussion.
137
2. Constraints on the use of Cs as a time-marker to
support CRS dates
To illustrate limitations in the use of 137Cs peaks as
time-marks to support CRS dates, two case studies have
been selected from the scientific literature: a sediment
core from Lake Zürich (Erten et al., 1985) and another
from the Black Sea (Gulin, 2000). The first core was
sampled in the northern part of Lake Zürich in August
1979 (at 61 m water depth and approximately 1 km
from the shoreline). A detailed description of this
aquatic system can be found in Erten et al. (1985) and in
von Gunten and Moser (1993). The second core was
sampled in the western abyssal basin of the Black Sea
(43
26.00 N-32
08.50 E, 1971 m deep, on 15 June 1993)
where permanent anoxic conditions prevail (see Gulin
2000 for a more detailed description of the area).
Fig. 1 shows the corresponding computed CRS ages
(age zero corresponds to the time of sampling) and the
Fig. 1. Computed CRS ages for sediment cores from Lake Zürich
(data from Erten et al., 1985) and the Black Sea (data from Gulin,
2000).
 J.M. Abril / Environmental Pollution 129 (2004) 31–37
137
Cs time-marks. These time-marks are from one
independent tracer and seem to provide an unambig-
uous time-stratigraphic horizon supporting the CRS
dates. Thus, they fulfil the criterion proposed by Smith
(2001).
The authors from the above references did not present
the historical records of the 137Cs atmospheric deposi-
tion for the studied areas. Nevertheless, it is well known
that 137Cs concentrations in air are relatively homo-
geneous with geographical longitude while they vary
with latitude (see Kathren, 1984). Thus, the historical
records of 137Cs atmospheric deposition measured by
the Risø National Laboratory in Denmark can provide
a first reference (see this paper for a comparison
between estimated atmospheric deposition in the Great
Lakes area and the corresponding Risø data). Devi-
ations from these reference values due to latitude and
local effects (annual rainfall, topography, etc.) can, as a
first estimate, be treated as a global correction factor.
This factor is introduced along with the normalization
factor (the ratio between the measured inventory in
sediments and the cumulative atmospheric deposition).
Thus, from the estimated 137Cs atmospheric deposition
and using the (variable) sedimentation rates resulting
from the CRS model, it was possible to compute the
expected 137Cs versus depth distribution in the two
sediment cores (provided that no post-depositional
mixing occurred, as is stated in the CRS model). Results
are shown in Figs. 2 and 3. We bear in mind that the
1986 peak has a high regional variability, and the value
from Denmark is not justified for the Black Sea.
Nevertheless, a different value wiould not significantly
alter the present discussion.
From Figs. 2 and 3 it is apparent that the CRS model
cannot explain the size of the peak, nor the presence of
Fig. 2. 137Cs specific activity (in dpm/g) versus mass depth profiles in
the sediment core from Lake Zürich: Measured (from Erten et al.,
1985) and computed values (boxes). The latter from the CRS sedi-
mentation rates and the historical records of 137Cs atmospheric
deposition measured by the Risø National Laboratory in Denmark
(after normalization).
33
137
Cs in the deeper layers. Thus, one has to accept
that mixing occurs at least for 137Cs. Some questions
then arise. First, the mixing could be translocational
(Robbins and Edgington, 1975) and therefore the dates
associated with the 137Cs marks should be questioned.
Alternatively, the mixing could be only diffusional,
thereby preserving the position of the peaks, which begs
the question as to how the mixing takes place: as a
mixing of solid particles, through the pore water, or by
both mechanisms. In the first and last cases, the mixing
necessarily has to affect 210Pb, and thus the CRS model
cannot be properly applied. The second case requires
the additional hypothesis that this pathway of mixing
does not affect 210Pb. In any case, the whole measured
137
Cs activity profile should be modelled from these
hypotheses with reliable mixing coefficients. However,
even if this last requirement could be fulfilled, a final
difficulty would arise when a reasonable interpretation
of experimental data from alternative modelling
approaches is possible (and therefore with different
chronologies).
To illustrate this point, the 137Cs profile in the sedi-
ment core from Lake Zürich was studied using a model
with a constant mixing coefficient and the aforemen-
tioned records of 137Cs atmospheric deposition. The
model used a mixing coefficient of 0.002 g2 cm4 year1
and a constant mean value of the mass sedimentation
rate of 0.075 g cm2 year1 (from CRS results). It pro-
vided a reasonable description of the data, as shown in
Fig. 4, although activities in the deepest layers were
poorly described. Nevertheless, this particular diffusion
model is not compatible with the CRS model since it
considers the mixing of the total specific activity, and
thus affects solid particles.
The IMZ model from Abril et al. (1992) is applied to
incomplete mixing and allows 137Cs to reach deep sedi-
ment layers whilst maintaining the position of the
peaks. This model could reasonably explain both 137Cs
Fig. 3. As Fig. 2, but for the core from the Black Sea (data from
Gulin, 2000).
34 J.M. Abril / Environmental Pollution 129 (2004) 31–37
and 210Pb specific activities versus mass depth profiles,
as shown in Fig. 4. The model used a constant value for
the mass sedimentation rate of 0.075 g cm2 year1, a
mixing zone at the top of the sediment with a mass
depth of 1.1 g cm2 and a mixing fraction g=0.6 (the
same parameter values as for 137Cs and 210Pb). We note
that the mass sedimentation rates from the CRS model
are variable, increasing from 0.03 g cm2 year1 at 14
cm depth up to 0.09 g cm2 year1 at the top. From a
mathematical point of view the IMZ model is more
constrained since it contains only three free parameters
applying to two independent data sets (210Pb and 137Cs
profiles). On the other hand, the CRS model works with
a variable sedimentation rate (its values are determined
from each experimental data point in the 210Pb profile);
and this model has to be complemented with a diffusion
model for the 137Cs data set, introducing additional
hypothesis and a new free parameter (the diffusion
coefficient).
In the core from the Black Sea, the 137Cs profile
reveals the existence of mixing. Although it was not
conclusive from the time resolution in this core (about 5
years), Gulin (2000) found the 137Cs weapon maximum
in the layer dated (by the CRS model) as 1966 instead of
1963. Indeed, the settling of particles and the vertical
diffusion of dissolved radionuclides in a water column
approximately 2 km deep is a slow process, and could
result in a significant change in the input function and
a displacement of the 137Cs time-marks. Thus, Edging-
ton et al. (1991) pointed out the effect of the residence
time of 137Cs in the water column in Lake Baikal.
Nevertheless, we note that the water-column processes
cannot be used to explain the presence of 137Cs at mass
depths deeper than 0.3 g cm2 in this sediment core (see
Fig. 3).
Fig. 4. 137Cs and unsupported 210Pb activities versus mass depth pro-
files in the sediment core from Lake Zürich (data from Erten et al.,
1985). A model of constant diffusion fits the 137Cs profile. The IMZ
model provides an independent fit for both 137Cs and 210Pb data,
leading to a different chronology (see text).
3. Constraints on the use of 137
Cs as a time-marker to
construct SIT chronologies
The use of 137Cs as a time-marker to support the SIT
model leads to similar situations to those studied in the
previous section, and will be illustrated with an appli-
cation using literature data from Waugh et al. (1998).
Waugh et al. (1998) studied a sediment core from a
uranium-contaminated pond located at the US Depart-
ment of Energy facilities in Grand Junction, western
Colorado. The pond was first excavated in the early
1920s. In 1943 the area was used by the US War
Department to stockpile uranium ore and extract ura-
nium from it. The measured 137Cs and unsupported
210
Pb activities appear in Fig. 5. These authors applied
the SIT model to interpret the unsupported 210Pb pro-
file, using two historical events to constrain the prob-
ability distributions of sediment ages. First, 137Cs was
still present at the base of the core; hence this base must
have been formed latter than approximately 1950.
Second, the peak in 137Cs activity was interpreted as
the 1963 maximum in the atmospheric fallout of 137Cs.
Therefore the SIT model satisfactorily explained the
unsupported 210Pb profile, producing the corresponding
chronology (see Fig. 6).
Fig. 7 plots the historical records of 137Cs atmo-
spheric deposition measured by the Risø National
Laboratory in Denmark compared against the esti-
mated atmospheric deposition in the Great Lakes area
(from Robbins and Edgington, 1975). As discussed
above, these historical records can be considered as a
reasonable estimate of the 137Cs atmospheric deposition
in western Colorado, provided a global normalization
factor is used.
Fig. 5. Measured (by Waugh et al., 1998) 137Cs and unsupported
210
Pb specific activities versus normalized depth profiles (points with
error bars). The lines are only guidelines. Boxes correspond to the
theoretical 137Cs profile derived from the atmospheric deposition
(Fig. 7, with a normalization factor of 0.54) and from the sediment-
ation rates estimated by Waugh et al. (1998)—see Fig. 6 —. These
authors normalized the depth of each interval below the sediment/
water interface to the lowest measured porosity (0.37).
 J.M. Abril / Environmental Pollution 129 (2004) 31–37
Using the atmospheric deposition from Fig. 7, the
sedimentation rates derived from Fig. 6, and assuming
no post-depositional mixing, it was possible to compute
the theoretical profile of 137Cs specific activity versus
normalized depth. Results appear in Fig. 5. The nor-
malization factor was 0.54. Clearly, these results do
not follow the pattern of the measured data. This under-
lines the limitations in the use of the 137Cs time-marks
without considering the whole activity profile. In this
particular case, the mixing affecting only 137Cs could
not easily explain the observed discrepancies. On the
other hand, an alternative modelling approach was also
possible.
The application of the IMZ model using the estimated
atmospheric deposition records of 137Cs from Fig. 7
Fig. 6. Estimated ages versus normalized depth (cm), from Waugh et
al. (1998).
Fig. 7. Historical records of 137Cs atmospheric deposition measured
by the Risø National Laboratory in Denmark (from 1950 to 1985)
compared against those estimated (from Robbins and Edgington,
1975) for the Great Lakes area (from 1954 to 1973). The latter have
been extended from 1950 to 1953 and from 1973 to 1985 using the
Risø data, and after 1986 using a constant, almost null, value (no
effects from the Chernobyl accident were considered). A third curve
has been constructed from the IAFE model with kr=0.15 year1. All
the data were corrected by radioactive decay referring to the date of
sampling.
35
provided only a rough understanding of the measured
137
Cs profile (see Fig. 8). In areas highly influenced by
inputs of matter from the catchment, as the studied
pond could be, the integration of atmospheric fluxes in
the catchment area could dominate the input of radio-
nuclides onto the sediment (Abril and Garcı́a-León,
1994). The integrated-atmospheric-flux-effect (IAFE)
model, provided by these authors, approaches this pro-
cess by introducing an effective transfer rate kr (T1), at
which radionuclides are transferred from the catchment.
Fig. 7 shows an input function constructed with the
IAFE model using kr=0.15 year1 (this value was
selected to fit the data). Abril and Garcı́a-León (1994)
found kr values of 0.043 and 0.10 year1 for Lake
Krageholmsjön (Sweden) and the Palace Moat (in
Tokyo), respectively. These values are comparable to the
one used in this work. With this input, the IMZ model
could reasonably explain the observed 137Cs activity
profile in the sediment, as shown in Fig. 8 (using a
sedimentation rate r=0.41  0.02 normalized cm y1,
a mixing depth ma=9.2  2.4 normalized cm, and a
mixing fraction g=0.68  0.19). Errors were estimated
from the
P curvature in the parametric
2 lines of the function
Q 2 ¼ i Ai;Theor  Ai;Meas =i2 ; where Ai,Theor and
Ai,Meas are, respectively, the computed and measured
specific activities at the same normalized depth interval
i, and i is the associated analytical error. While the
model assumes a constant sedimentation rate, random
fluctuations over its averaged value (due to natural
yearly variability) can produce perturbations in the
activity profile, although the general trend is preserved.
The same model could equally explain the 210Pb data.
We note that the integrated atmospheric effect under
constant atmospheric input leads to a steady-state
situation. In this way, the natural component of 210Pb
may be different from the direct atmospheric deposition.
Fig. 8. Comparison between measured and computed (lines) 137Cs
specific activity versus normalized depth profiles. The computed values
correspond to the IMZ model operating with the direct atmospheric
deposition and with that deposition derived from the IAFE model
with kr=0.15 year1 (see Fig. 7). In both cases the IMZ model uses the
same parameter values (see text).
36 J.M. Abril / Environmental Pollution 129 (2004) 31–37
However, it will be equally constant. Thus, the IAFE
model does not need to be formally applied to 210Pb
data. Nevertheless, we note that the uranium mill
enhances the 222Rn emissions (Whicker and Schultz,
1982) and hence increases the local atmospheric deposi-
tion of 210Pb. Fig. 9 plots the total U (ppm) measured
by Waugh et al. (1998) versus the sediment dates (esti-
mated from the sedimentation rate found from our IMZ
model applied to the 137Cs profile). The temporal extent
of the uranium ore processing activity could be mod-
elled by a Gaussian function (see Fig. 9). This served to
estimate the anthropogenic component in the atmo-
spheric 210Pb fluxes. Thus, the time-dependent atmo-
spheric deposition of 210Pb was constructed from a
constant baseline (the naturally occurring component)
and the anthropogenic component given by a Gaussian
function. The values of the maximum and the baseline
(50 and 250 Bq m2, respectively) were found from fit-
ting the IMZ model to the measured unsupported 210Pb
activity in the sediment (see Fig. 10). The application of
the IMZ model to the 210Pb data used the same para-
meter values for 137Cs. We observe that the fraction of
mixed activity for Pb and Cs can be different. Thus, a
value of g=0.5 produced slightly better results, despite
the large errors in the 210Pb data.
The baseline flux of 50 Bq m2 year1 of 210Pb is
consistent with the values reported by Appleby (1998)
for western North America, and the anthropogenic
contribution is not unrealistic. On the other hand, the
derived chronology, when compared against the total U
profile, is consistent with the peak period of uranium
related activities at this site in the early 1960s (see
Waugh et al., 1998).
In the studied case, the 137Cs time-marks were not
used as an independent support for SIT dates, but
served to construct the SIT chronology itself. Never-
Fig. 9. Total U (ppm) measured (continuous line) by Waugh et al.
(1998) versus the sediment dates given by the IMZ model (present
work). The effect of the uranium ore processing is approached by a
Gaussian function centred in the year 1963 and with a sigma value of
10 years.
theless, the 137Cs activity profile is not consistent with
the derived chronology nor with the basic assumption of
non-mixing in the SIT model. We note that the use
of an input function from the IAFE model along with
the variable sedimentation rates from the SIT model
could not explain the observed 137Cs profile. Again, an
alternative modelling approach could reasonably repro-
duce the whole set of observational data on a different
basis; therefore resulting in a different chronology
(although the basic conclusions from Waugh et al.,
1998, would not be essentially altered). Furthermore, the
alternative modelling approach is more restricted from a
mathematical point of view (fewer free parameters). An
exercise consisting of the application of a best-fit mathe-
matical model without taking the sediments as such into
account can be considered as an exercise in futility.
Nevertheless it has the value of questioning the metho-
dology in the application of the SIT model.
4. Concluding remarks
210
Pb geochronologies must be validated using at least
one independent tracer, which separately provides an
unambiguous time-stratigraphic horizon. For this pur-
pose, artificial fallout radionuclides such as 137Cs repre-
sent a useful tool. Nevertheless, it has been demonstrated
that simple methods based on the identification of the
137
Cs fallout peaks cannot provide a definitive support
for CRS and SIT chronologies. The study of the whole
137
Cs activity profile is a more powerful tool and con-
tains additional valuable information. Further work is
needed for the development of suitable models. Simi-
larly, more effort is required to identify and provide more
basic data from sediment cores and their environments
to support suitable radiometric dating models.
Fig. 10. Comparison between measured (from Waugh et al., 1998)
and computed (by IMZ model) unsupported 210Pb profiles. The input
function was FðtÞ=50+250 Exp{-l(t-63)2/100} Bq m2 year1. Model
1 used the same parameter values as for 137Cs (Fig. 8 and text) while
Model 2 used a lower value for g (0.5).
 J.M. Abril / Environmental Pollution 129 (2004) 31–37
Acknowledgements
This work has been partially supported under con-
tract I+D with the Spanish ENRESA (Project 774511,
Code 0770105). The author sincerely recognises the
merit of the works from Erten et al. (1985), Waugh et al.
(1998) and Gulin (2000); and hopes that the new ideas
presented here will contribute to an increase in their
relevance for the scientific community.
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