Applied Radiation and Isotopes 156 (2020) 108949

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Applied Radiation and Isotopes

journal homepage: http://www.elsevier.com/locate/apradiso

Calculation of decision threshold and detection limit in radiometric

measurements using a Monte Carlo Method
€ck a, b, *, L. Persson a, C. Ekberg b, P. Lindgren a, M. Bruggeman c
H. Rameba
a
Swedish Defence Research Agency (FOI), CBRN Defence and Security, SE-164 90, Stockholm, Sweden
b
Chalmers University of Technology, Department of Chemistry and Chemical Engineering, Nuclear Chemistry, SE-412 96, G€
oteborg, Sweden
c
Belgian Nuclear Research Centre (SCK-CEN), Boertang 200, B-2400, Mol, Belgium

A R T I C L E I N F O A B S T R A C T

Keywords: Calculation of the decision threshold and detection limit of a measurement, or measurement method, are crucial
Decision threshold in order to decide if an analyte is present or not and with what confidence it can be quantified. That decision is
Detection limit important in view of possible actions if something would be detected. In this work, a method for calculating these
Minimum detectable activity
limits using a Monte Carlo method is presented. In the Monte Carlo method any a priori distribution (e.g. normal
MDA
Monte Carlo
distribution, rectangular distribution, triangular distribution) of an input quantity can be selected. Differences
between the Monte Carlo calculated characteristic limits and the ones calculated according to ISO 11929:2010 is
presented. Moreover, suggestions how to calculate the detection limit when it can not be calculated according to
the ISO 11929:2010 are given.

1. Introduction distribution of the measurand will be skewed already at relative stan­

Calculation of the characteristic limit detection limit (minimum
detectable activity, MDA) according to the international standard ISO
11929:2010 (ISO 11929:2010, 2010) states that the MDA is a function of
the value of the measurand and its associated uncertainty. This uncer­
tainty comprises both the uncertainty of the background signal and of
the conversion factor applied to calculate an activity from a net number
of counts. However, according to the ISO 11929:2010 standard the de­
cision threshold is only a function of the uncertainty of the net signal for
the background since, in the uncertainty propagation, the uncertainty of
the conversion factor will not contribute to the uncertainty at the de­
cision threshold (ISO 11929:2010, 2010; de Felice et al., 2017). More­
over, in the standard it is assumed that the uncertainty of all input
quantities can be expressed as a standard deviation. For normal distri­
butions this is straight forward, and according to GUM (JCGM 100,
2008), this can be achieved also for other distributions. However, if the
width of e.g. a rectangular distribution is large, the resulting distribution
for the measurand will not be a normal distribution (Sima and L� epy,
2016; Rameb€ ack and Lindgren, 2018). It has also been shown that for a
normal distribution having a large standard uncertainty, the resulting
distribution of the measurand will be skewed for input quantities in e.g.
the denominator (Rameba €ck and Lindgren, 2018). The resulting
dard uncertainties in an efficiency transfer correction factor kET of about
2–3%.
The decision threshold is defined as the level of the measurand where
there is a pre-set risk of detecting something not present in a sample
(Type I error, e.g. the 95% percentile of the background distribution, i.e.
representing an α ¼ 5% risk of a false positive), and the MDA is defined
as the level where there is a risk of not detecting something although
present (Type II error e.g. the 5% percentile of the probability density
functions PDF for the measurand, i.e. representing a β ¼ 5% risk of a false
negative). The shape of the PDF of the background and the signal by the
analyte (activity) respectively, will then be important for determination
of the percentiles, since it might not always hold that these distributions
are Gaussian, although this is the most often used assumption. In the
classical approach for calculating the characteristic limits, the percen­
tiles are calculated based on quantiles for the standard normal distri­
bution (Currie, 1968). Now, if the PDF of the measurand are
non-Gaussian, this might result in an error in the calculated limits.
With a large uncertainty of the conversion factor, the method based
on propagation of uncertainties given in the ISO 11929:2010 might
result in negative MDA (Glavi�c-Cindro et al., 2017; Wilson et al., 2004).
For a standard uncertainty in the conversion factor of about 60.8%, and
for α ¼ β ¼ 5%, the detection limit will be infinite and with further

* Corresponding author. Swedish Defence Research Agency (FOI), CBRN Defence and Security, SE-164 90, Stockholm, Sweden
E-mail address: henrik.ramebeck@foi.se (H. Rameb€
ack).

https://doi.org/10.1016/j.apradiso.2019.108949
Received 8 May 2019; Received in revised form 4 September 2019; Accepted 15 October 2019
Available online 18 October 2019
0969-8043/© 2019 Elsevier Ltd. All rights reserved.
H. Rameb€
ack et al.
increasing the uncertainty it will be at negative infinity whereafter it
will stay negative. The consequence is that the MDA can not be defined,
since negative MDA is non-physical. Such large uncertainties in the
conversion factor include situations like in situ gamma spectrometric
measurements, and for samples with large unknown inhomogenities
(Glavi�c-Cindro et al., 2017). (An in situ gamma spectrometric measure­
ment for an unknown radionuclide distribution in and/or on the ground
might be seen as equivalent to a large unknown inhomogeneity.)
Another situation is attenuation in samples with an unknown composi­
tion, and especially when measuring radionuclides emitting low energy
gamma photons like 210Pb with gamma spectrometry, although there
are ways to correct for this attenuation (Cutshall et al., 1983). Finally,
this would also be the situation for waste measurements where large
drums are to be measured and the uncertainty in the detection efficiency
might be large due to a combination of radionuclide and material dis­
tributions as well as sample matrix composition.
In this work a Monte Carlo Method (MCM) for calculating charac­
teristic limits is presented. The method can handle any predefined
probability distribution of the conversion factor (or of any quantity
included in the conversion factor). In particular, the characteristic limits
as a function of the uncertainty in the correction factor for efficiency
transfer (kET) in gamma ray spectrometry (Vidmar et al., 2010) was
studied. The modelled distributions of kET included rectangular distri­
bution, triangular distribution, normal distribution, truncated normal
distribution and log normal distribution.
2. Theory
2.1. Model for the MCM
The model equations used in the MCM for calculating the decision
threshold and MDA were
ðNnet þ NBG Þ N ’BG
A¼ (1)
tmeas ⋅ε0 ⋅Iγ
Ncal
ε¼ (2)
tcal ⋅Acal ⋅Iγ
(3)
0
ε ¼ ε⋅kET
where A is the decision threshold or MDA expressed in activity units,
Nnet is the net number of counts in a measurement, NBG and N’BG the
number of counts in the background at two locations close in energy
(paired observation) during the measurement, tmeas the measurement
time, ε0 the measurement efficiency for the geometry used and Iγ the
photon emission probability. In this work N’BG can be seen as the
background in the Compton continuum in a gamma spectrometric
measurement for a region, having the same width as the region of in­
terest at the peak location with NBG as the number of background counts
in the Compton continuum. Here it was assumed that the measurement
time of the background count was the same as for the sample mea­
surement, which would be the case in gamma spectrometry if the
different regions of interests have the same width. Observe that for a
single point calibration the uncertainty of the photon emission proba­
bility will cancel out. In the efficiency calibration (single point cali­
bration with the same radionuclide as in the measurement) the number
of counts was Ncal during the time tcal using an activity standard with an
activity Acal. Eq. (3) gives the corrected efficiency due to efficiency
transfer applying the correction factor kET. This correction can be
needed due to differences in geometries between the calibration and the
measurement, and/or differences in attenuation if the matrices are
significantly different. It should be stated that although gamma ray
spectrometry was used in this work as an example, Eqs. (1)–(3) can be
applied to any radioanalytical method after replacing some of the input
quantities with the specific ones for any other particular method.
2
Applied Radiation and Isotopes 156 (2020) 108949
Basically, determining if something is present in a sample is nothing
else than hypothesis testing, i.e. determine at a pre-defined probability
level if two distributions are different or not. Actually, based on a hy­
pothesis test one calculates which instrumental signal that is needed in
order to decide at a pre-set significance level if a radionuclide under
study is present in the sample, e.g. which signal level results in a
significantly different activity distribution compared to the distribution
of the background. The decision threshold is defined as the (1-α)
percentile of the PDF when no analyte is present, i.e. the risk of detecting
something not present is α. The MDA is then computed from the mean of
the activity distribution having its β percentile equal to the decision
threshold, e.g. the risk of not detecting something present, while there is,
is β.
The decision threshold according to ISO 11929:2010 can be calcu­
lated explicitly, whereas the MDA would need an iterative approach
(ISO 11929:2010, 2010), but explicit equations for calculating MDA has
been derived (de Felice et al., 2017; Glavi�c-Cindro et al., 2017), which
will work in most applications. However, there might be situations when
the uncertainty in the conversion factor will exceed the limit for which
the MDA cannot be calculated with the uncertainty propagation method.
In this work, the characteristic limits as calculated with the MCM were
compared to limits calculated using such explicit expressions.
The model used in this work can be seen as a single channel analyzer
(or as in the gamma spectrometric case a dual channel analyzer), where
one region of interest is set in an energy region where a peak is expected,
and another region of interest is set just above the peak in order to
determine N’BG used for calculating the Nnet needed to just match the
pre-set criteria of the MDA. Using this approach it is assumed that the
background is flat enough in the studied energy interval. If this would
not be the case, another background can be set below the peak (in en­
ergy) and the average of the limits can be calculated. In this work it was
assumed that the background is uncorrelated to analytical peaks in the
spectrum (Berlizov, 2007). The equation used for the explicit calcula­
tions (de Felice et al., 2017):
- Decision threshold:
qffiffiffiffiffiffiffiffiffiffi
Lc ¼ kw 2N ’BG (4)
where w is the conversion factor for calculating the decision threshold in
activity units (here w ¼ 1/(tmeas⋅ε⋅Iγ⋅kET)), k ¼ k1-α is the quantile for the
specified error of the first kind (k1-α ¼ 1.645 if α ¼ 5%), and N’BG the
number of counts in a region of interest for estimation of the
background.
- MDA:
pffiffiffiffiffiffiffiffiffiffi
k2 þ 2k 2NBG
MDA ¼ w (5)
1 k21 β u2rel ðwÞ
where k1-β is the quantile for the pre-set risk of not detecting anything
present in a sample (e.g. k1-β ¼ 1.645 if β ¼ 5%) and urel(w) is the relative
uncertainty of the conversion factor. Here k ¼ k1-α ¼ k1-β has been
assumed. In this work, the same measurement set-up as presented earlier
was used (Rameba €ck and Lindgren, 2018). The only difference is in Eq.
(1), where the influence of a background has been included.
2.2. MCM
Here, in order not to overload the notation, random quantities and
corresponding samples are used interchangeably. All quantities were
considered random quantities, except the measurement times tm and tcal
which were considered as constants. Each input quantity were sampled
according to its known, or assumed, PDF. Moreover, an activity sample
percentile was estimated by the empirical percentile of the MC sample.
The MCM was similar to the one used by Rameba €ck and Lindgren
H. Rameb€
ack et al.
Fig. 1. The PDFs of the measurand when no analyte is present and when the
analyte is present at a level equal to the MDA for a low uncertainty (1%, k ¼ 2)
in the conversion factor. The vertical lines represents here the 95% percentile
for the PDF of the decision threshold, and the 5% percentile for the MDA.
(2018) (Rameba €ck and Lindgren, 2018) utilizing Microsoft Excel 2013
(Microsoft Corporation, WA, USA). For each input quantity, 100 000
samples were generated according to assumed predefined PDF (rectan­
gular PDF, triangular PDF, Gaussian PDF, truncated Gaussian PDF and
lognormal PDF). One difference compared to the earlier work by
Rameb€ack and Lindgren (2018) was that the number of counts was
modelled using a Poisson distribution. Inverse transform sampling was
used throughout, where a uniform probability sample is generated, and
then the inverse cumulative distribution function is applied. However,
inverse transform sampling from a Poisson distribution in Excel is not
possible since its inverse cumulative distribution function is not imple­
mented. This was solved by sampling from the binomial distribution for
a low probability p and large number of trials n, since the binomial
distribution then will reduce to the Poisson distribution (Larson and
Marx, 1990). The probability sample was generated using Excel’s
pseudo-random number generator from the function RAND(). When a
truncated Gaussian was used for kET, the probability sample was trun­
cated at the lower end in order to restrict kET to positive values only. The
rationale for this is that the efficiency ε0 should only be positive. In this
work, kET was restricted to be 0.01 as its lowest value for the truncated
case. Of course, this restriction is arbitrary and could have any value,
and is to be chosen by the analyst based on previous experiences and/or
scientific judgement. The triangular distribution was always modelled as
being equilateral. Sampling from different PDF has been described
earlier (JCGM 101, 2008).
From 100 000 runs the decision threshold was estimated using the
PERCENTILE function in Excel. Here, the 95% percentile of the PDF for
the measurand when no analyte is present and corrected for background
was defined as the decision threshold. The MDA was estimated as the
mean value for the PDF having a 5% percentile equal to the 95%
percentile of the decision threshold. In order to achieve more stable
mean values from the calculation of the MDA when the uncertainty of
kET was large (>40%) and its PDF was modelled as a non-truncated
Gaussian, a trimmed mean was used (Leonowicz et al., 2005). The
trimmed mean was achieved by simply discarding the outermost per­
centiles of the MDA distribution, typically the 0.001 and 0.999 per­
centiles. This resulted in dramatically more stable mean values. For a
relative standard uncertainty of kET of 60% the mean value of the MDA
was (34 � 23) Bq, k ¼ 1, if all 100000 samples were used (standard de­
viation based on 10 replicates with 100000 samples in each calculation).
If the 0.001 and 0.999 percentiles of the MDA are discarded, the MDA¼
3
Applied Radiation and Isotopes 156 (2020) 108949
Fig. 2. The PDFs when no analyte is present and with the analyte present at a
level of the MDA for a rectangular distribution having a half-width of 95%
for kET.
(30.15 � 0.86) Bq, k ¼ 1. Discarding the 0.001 and 0.999 percentiles
resulted in discarding the 100 lowest and 100 largest values in the
calculation if 100000 samples were used.
The calculation of the decision threshold is straight forward: it is
simply the chosen percentile representing the risk of false positives. In
this work α ¼ 5% was chosen, i.e. the decision threshold is then the 95%
percentile of the PDF for the measurand when no analyte is present.
Then the net number of counts for the MDA was iterated in order for the
5% percentile of the PDF of the MDA to match the 95% percentile for the
decision threshold. When a truncated Gaussian was chosen for model­
ling of kET, the mean value for the original untruncated distribution was
changed in order to get a mean value for the truncated distribution equal
to one. For the lognormal distribution, the mean value of kET was also
always equal to one. The criteria in the iteration of the MDA was that the
percentiles should match within about 1%.
3. Results and discussion
First, the MCM was tested relative Eqs. (4) and (5). The result is
shown in Fig. 1. The decision threshold and MDA agreed within 0.5%
between the MCM and Eqs. (4) and (5) when the uncertainty in kET was
low (1%). At low uncertainties in kET the explicit equations should be
expected to work well. Moreover, since the number of counts for the
background was high, and the uncertainties of all input quantities in the
conversion factor had a low uncertainty, one would expect the PDF for
the decision threshold and the MDA to be Gaussian, which is actually the
case here.
For a non-Gaussian and wide PDF of the conversion factor, a non-
Gaussian PDF of the measurand when no analyte is present and when
present at the level of the MDA will be obtained as can be seen in Fig. 2.
This is due to the fact that the model is non-linear and to the impact of a
non-Gaussian input quantity. The same was observed earlier regarding
the uncertainty for non-linear models with large uncertainties
(Rameba €ck and Lindgren, 2018).
3.1. Decision threshold
In ISO 11929:2010 the calculation of the critical limits are based on
propagation of uncertainties. One consequence of this is that the un­
certainty of the conversion factor w will not have any influence on the
decision threshold since the term comprising the relative uncertainty in
the conversion factor will be zero for a zero net signal (NBG-N’BG ¼ 0,
H. Rameb€
ack et al.
Fig. 3. PDFs of the net signal for two blanks, Eq. (1) when Nnet ¼ 0, having
either an uncertainty or no uncertainty in the conversion factor. No uncertainty
in kET represents the case using propagation of uncertainties.
Fig. 4. The calculated decision thresholds for different PDF of kET. The decision
threshold for the triangular PDF of kET is hidden among the curves for the
Gaussian, rectangular and truncated Gaussian cases. The standard uncertainty
for the triangular reached about 39%, since (a–b)/2 was at its maximum 95%.
Small fluctuations in some of the plotted series is due to a relatively small
inherent variability in the MCM, in particular for large uncertainties in the
conversion factor. This does not influence the general results.
since NBG and N’BG are expected to have the same mean values for equal
tm). However, exploring the PDF of the decision threshold from a MC
calculation reveals an impact of urel(w), although the average of the net
signal is zero. The effect can be noted in the tails of the PDF of the de­
cision threshold, see Fig. 3. The decision threshold (as well as MDA) has
to be expressed in units of the measurand, i.e. in activity units, since the
(1-α) percentile of the decision threshold should match the β percentile
of the distribution of MDA. As mentioned above, the term comprising
urel(w) will be zero when uncertainty propagation is applied and
therefore the uncertainty in the conversion factor does not contribute.
However, in a MC calculation a single sample of (NBG-N’BG) will rarely
be zero, although the average of 100 000 calculation is very close to
zero. This, in combination with a large uncertainty in w, will give a
fraction of the results out in the tails of the PDF when samples of kET are
drawn far away from its mean value, which will influence the (1-α)
percentile of the decision threshold. The result is that the decision
threshold will be higher as compared to the one calculated using
4
Applied Radiation and Isotopes 156 (2020) 108949
Fig. 5. The PDF of the MDA in one simulation for a standard uncertainty of the
conversion factor of 62%. Here, the 5% percentile was at about A ¼ -30 Bq.
Increasing the net number of counts will not help, but rather decrease the
5% percentile.
propagation of uncertainties since the percentile representing the deci­
sion threshold will be higher. Fig. 4 shows the decision threshold as a
function of the relative standard uncertainty for different PDF of kET.
Clearly, there is a difference between the decision threshold calculated
based on uncertainty propagation or when using the MCM already
below a relative standard uncertainty of 20% in the conversion factor. As
mentioned above, this is due to the increase of the tails of the PDF of the
measurand when no analyte is present. From Fig. 4 it is clear that not
taking the uncertainty in the conversion factor into account will un­
derestimate the decision threshold. Moreover, for relative standard un­
certainties in kET up to about 30%, the MCM yields about the same
decision threshold independent of the assumed PDF of kET. For values
above 30% the decision threshold starts to deviate. The decision
threshold is about 36% higher as compared to when no uncertainty in
the conversion factor is included, or when computed directly from
equation (4). It is obvious that the decision threshold for a rectangular
PDF of kET will be higher as compared to the other distributions, since
the increase in the tails will be more pronounced, see Fig. 3.
3.2. MDA
One problem applying uncertainty propagation for estimating the
MDA is that after about 60.8% relative standard uncertainty (at 5%
risks) of the conversion factor, the MDA will be negative since the de­
nominator in Eq. (5) will be zero at about 60.8% relative uncertainty and
thereafter it will switch to negative values. This can be understood ac­
counting for the fact that a large fraction of the PDF of the MDA will be
negative, and eventually it will not be possible to get its 5% percentile to
reach the 95% percentile of the decision threshold, see Fig. 5.
Simulation of the MDA gave about the same result as the MDA
calculated based on uncertainty propagation: at about 61% standard
uncertainty of the conversion factor it will not be possible to calculate an
MDA, since its 5% percentile will have a negative value. However,
increasing the risks of false positive and false negative will move the
point at which the denominator in Eq. (5) will switch from a positive to
negative. This moves the percentiles to reach a relevant value of the
MDA. For example, at α ¼ β ¼ 10%, the denominator in Eq. (5) will be
negative after about 78% relative uncertainty in the conversion factor.
Although such risks might be acceptable in some situations, it might be
inappropriate for other applications (Glavi�c-Cindro et al., 2017).
The MDA as a function of the standard uncertainty of kET are shown
in Fig. 6. The results show that calculation of MDA based on uncertainty
H. Rameb€
ack et al.
Fig. 6. MDA calculated using uncertainty propagation and with the MCM
assuming different PDF of the conversion factor. The MDA for the triangular
PDF of kET is hidden among the curves for the Gaussian, rectangular and
truncated Gaussian cases. Small fluctuations in some of the plotted series is due
to a relatively small inherent variability in the MCM, in particular for large
uncertainties in the conversion factor. This does not influence the gen­
eral results.
propagation gives good results up to about a relative uncertainty in the
conversion factor of 35–40%. Moreover, by restricting the correction
factor kET to being only positive, it is possible to calculate MDA even
above 61% relative uncertainty in the conversion factor. This restriction
would be justified by the fact that otherwise it would give negative
efficiencies.
In this work different shapes for the PDF of kET were used, involving
Gaussian, rectangular, triangular, truncated Gaussian, and lognormal
shapes. These are examples exploring consequences of assumptions
regarding the PDF of kET when e.g. limited knowledge is present of the
input quantity. Of course, other PDF would be interesting to explore,
which furthermore, restrict the conversion factor to only positive values.
Moreover, the choice of PDF for kET should be based on previous
knowledge if that exist. If such knowledge does not exists, it has to be
assumed based on e.g. scientific judgement and that assumption involves
the assumption of the PDF. This is the normal way according to GUM for
Type B evaluations using uncertainty propagation as well.
For e.g. spectroscopic measurements, more information about the
background can be obtained by setting a wider region of interest (which
would be equivalent to the case when the background is measured
longer than the sample). However, here it has been assumed that the
width of the two regions are equal. It has also been assumed that the
calculation is done for the case when no analyte is present in the sample.
If the analyte is present in the sample, the calculation of the decision
threshold and MDA still can be done with a small modification of the
model equation, Eq. (1), (de Felice et al., 2017).
At the very end of this study, there were new ISO standards issued
relating to the calculation of characteristic limits in e.g. the measure­
ment of radionuclides (ISO 11929-1, 2019; ISO 11929-2, 2019; ISO
11929-3, 2019). In particular the ISO 11929–2 relates to the work pre­
sented here. In the light of the newly issued ISO standards this work is a
direct application of the guidance given for calculating decision limit
and MDA in radiometric measurements when commonly used uncer­
tainty propagation will be inappropriate.
4. Conclusions
In this work it was demonstrated with MCM that uncertainty in the
Applied Radiation and Isotopes 156 (2020) 108949
conversion factor will modify the decision threshold as compared to the
method suggested in ISO 11929:2010. With the ISO, uncertainty in the
conversion factor cancels out when using uncertainty propagation to
compute the decision threshold. The MDA as calculated using uncer­
tainty propagation starts to differ from the MCM results when a relative
uncertainty in the conversion factor exceeds 35–40% (α ¼ β ¼ 5%). For
uncertainties larger than about 61% (normal distribution) and for
α ¼ β ¼ 5%, it is not possible to compute a MDA for the MCM. This is due
to the fact that a too large part of the PDF for the MDA will be on the
negative side. Solutions to this problem might be to model the conver­
sion factor with different PDF than Gaussian, e.g. a rectangular, trian­
gular, truncated Gaussian or lognormal. However, at a relative
uncertainty of the conversion factor of 60.7% the MCM resulted in a
relevant measure of MDA, whereas the uncertainty propagation method
start to reach very high values and at the limit it will reach infinity.
Acknowledgement
This work was funded by the Swedish Ministry of Defence, project
no. A404619.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.apradiso.2019.108949.
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