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Radiation Measurements 125 (2019) 34–39

Contents lists available at ScienceDirect

Radiation Measurements
journal homepage: www.elsevier.com/locate/radmeas

A machine learning approach to glow curve analysis T


a a,∗ a b
Kevin Kröninger , Florian Mentzel , Robert Theinert , Jörg Walbersloh
a
Technische Universität Dortmund, Lehrstuhl für Experimentelle Physik IV, Otto-Hahn-Str. 4a, 44227, Dortmund, Germany
b
Materialprüfungsamt NRW, Marsbruchstr. 186, 44287, Dortmund, Germany

A R T I C LE I N FO A B S T R A C T

Keywords: We present a first study of using artificial neural networks to estimate the fading time and irradiation dose using
TL-DOS glow curve data from LiF thermoluminescent (TL) dosemeters. The resulting uncertainties in the inference
Thermoluminescence process are compared to those obtained in previous studies without machine learning algorithms. The current
Glow curve analysis study is based on measurement and simulated data using an effective model of the kinetic parameters. We show
Fading time estimation
that the resulting uncertainties of the estimated quantities can be significantly reduced with the machine
Irradiation dose estimation
Machine learning
learning algorithm applied: fading times of up to 30 days can be predicted with an uncertainty of up to 10%,
irradiation doses larger than 1 mSv can be estimated with an uncertainty of up to 10% for batch-calibrated
dosemeters.

1. Introduction sets used are that described in Ref. Theinert et al., 2018. Instead of
using the peak heights and their ratios directly to estimate the irra-
Personal dosimetry is an important aspect of radiation safety. A diation dose and the fading time, respectively, we train shallow neural
large variety of systems exist to measure and quantify irradiation doses, networks to combine the information and correlate their output with
e.g. film-badge dosemeters, electronic dosemeters and dosemeters either of these two quantities.
based on the phenomenon of luminescence. For systems based on In supervised machine learning, the availability of ground-truth
thermoluminescence, the time-resolved response of the dosemeter to data is a key to success. Since, however, the data set at hand is limited
heating is referred to as glow curve and it is characterized by a se- to a few well-defined irradiation doses and fading times, an effective
quence of glow peaks. While the total number of photons of a glow model is developed which allows the simulation of glow curves. These
curve gives information about the irradiation dose, we have shown in simulations are used to optimize, test and validate the machine learning
Ref. Theinert et al. (2018) that the relative peak heights can give fur- algorithm used in this study. The simulated data are also compared to
ther dosimetric information, in particular on the time between irra- measured data.
diation and readout. The estimation of this time span, also known as The structure of this publication is as follows: the glow curve model
fading time, is of special dosimetric interest as its correct reconstruction and its simulation are described in Sections 2 and 3, the experimental
provides the date of irradiation for single irradiation scenarios. The setup and the data set used in this study are summarized in Section 4.
knowledge of the fading time also provides a non-destructive approach Section 5 introduces the machine learning algorithms used for the in-
towards irradiation dose estimation under the impact of ambient tem- ference problem at hand and the results of the studies are presented in
perature signal loss (see Ref. Theinert et al. (2018) for details). In Sections 6 and 7. Section 8 summarizes the studies and gives an outlook
comparison, the successfully used and well known method of post ir- to possible improvements and further applications of machine learning
radiation annealing for fading time correction (e. g. Ref. Walbersloh in the analysis of glow curves.
and Busch (2015)) results in a significant loss of dosimetric information
due to the preheating process involved. 2. Glow curve model
In this publication, we present a first approach to irradiation dose
estimation using artificial neural networks. The study is based on Glow curves from LiF:Mg, Ti dosemeters in the range from 270 K to
measurements conducted with thin-layer LiF:Mg, Ti thermoluminescent 570 K comprise of five glow peaks, P1 to P5, with individual half-lives
(TL) dosemeters of the TL-DOS system, first described in Ref. ranging from minutes to years and they are typically modeled in tem-
Walbersloh and Busch (2015). The experimental setting and the data perature space, see e.g. Ref. Harvey et al. (2010) and references therein.


Corresponding author.
E-mail address: florian.mentzel@tu-dortmund.de (F. Mentzel).

https://doi.org/10.1016/j.radmeas.2019.02.015
Received 26 September 2018; Received in revised form 30 January 2019; Accepted 19 February 2019
Available online 26 February 2019
1350-4487/ © 2019 Elsevier Ltd. All rights reserved.
K. Kröninger, et al. Radiation Measurements 125 (2019) 34–39

Fig. 2. The measured average relative values of Im for P3 are shown as a


function of the fading time for irradiation doses between 1 mSv and 10 mSv.
Fig. 1. A typical glow curve for a dosemeter irradiated with 15 mSv and a Also indicated is the parameterization with the corresponding uncertainty
fading time of less than 2 h. The individual peaks identified by a fit of the model band.
to the measurement data are also indicated. The bottom plot shows the dif-
ference between the measurement data and the fitted glow curve. A 5%-un-
certainty band is also shown.

As P1 has decayed completely for essentially all practical purposes, the


glow curve is represented by the sum of peaks P2 to P5. The photon
intensity of the individual peaks in our model are described as a
function of the temperature by Equation (25) of Ref. Kitis et al. (2006).
This function is based on Ref. Randall and Wilkins (1945), modified to
take into account an exponential heating function and characterized by
a well-defined set of kinetic parameters according to Ref. Kitis et al.
(2006). These are the maximal peak intensity, Im , the temperature of
the peak maximum, Tm , and the parameter E which represents the width
of the peak. The background is modeled by the sum of an exponential
and a reciprocal term. Fig. 1 shows the fitted glow curve from a dose-
meter irradiated with a dose of 15 mSv and read out after a fading time
of less than 2 h. The figure also shows the individual peaks P2 to P5 and
the difference between the measurement data and the fitted glow curve.
A 5%-uncertainty band is shown to guide the eye and to give an im- Fig. 3. Simulated glow curves for different fading times without background
pression about the agreement between the measurement data and the contributions.
model.
times of zero days, three days and 25 days. As expected, the peak
heights change significantly with the fading time and with different
3. Effective simulation of glow curves
half-lives associated with the peaks. P2 vanishes over a time of 25 days.
P3 increases first and then decreases. The increase can be interpreted as
A first approach towards glow curve simulation is developed as an
clear sign of re-trapping being involved in the fading process. P4 and P5
effective simulation based on a parameterization of the kinetic para-
increase monotonically over that time span.
meters: First, all glow curve data are fitted with the model described in
In order to take into account background and detector effects, the
the previous section. Then the kinetic parameters Im , Tm and E for each
predicted glow curves are transformed into the time regime by in-
peak are parameterized as a function of the irradiation dose and the
tegrating the photon counts between discrete time points. Using fixed-
fading time. Linear functions are used for the parameterization of Im as
width time intervals, the temperatures are computed using an ex-
a function of the dose, the parameters Tm and E are kept constant.
ponential heating function. After the transformation, each bin is
In contrast to that, all kinetic parameters, including E and Tm , were
smeared by a Poisson term with an expected number of occurrences (λ)
found to show a fading time dependence. This fading time dependence
set equal to the integrated bin content. The re-transformation into the
is parametrized using exponential functions with polynomial correction
temperature space is done in the same form as for measurement data.
terms for all kinetic parameters. As an example, Fig. 2 shows the
The necessary steps are presented in detail in Ref. Theinert et al.
measured average relative values of Im for P3 as a function of the fading
(2017). Fig. 4 shows an example for glow curves from the simulation
time from a batch of dosemeters irradiated with doses between 1 mSv
and the average measurement data set for an irradiation dose of 5 mSv
and 10 mSv. Also indicated is the parameterization with the corre-
and a fading time of 24 h. The uncertainty band shows the standard
sponding uncertainty band. The agreement between the parameteriza-
deviation of the measurement data and the Poisson-smeared simulation
tion and the measurement data is reasonable for all kinetic parameters.
per temperature bin. The simulation and average measurement data
In this effective model, the kinetic parameters are now purely a
curve show a reasonably good agreement, the maximum deviation
function of the irradiation dose and the fading time, and these two
observed is about 10%. The comparison in Fig. 4 is exemplified, the
effects are assumed to be independent. For each such pair of values, a
simulation shows a very similar agreement for both the whole irra-
glow curve can be predicted. The glow curves are binned with bin
diation dose and fading time range included in the measurement data.
widths of 2.5 K. Fig. 3 shows three simulated glow curves for fading

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K. Kröninger, et al. Radiation Measurements 125 (2019) 34–39

Fig. 4. Glow curves from the simulation and the average data set for an irra-
diation dose of 5 mSv and a fading time of 24 h. The uncertainty bands show the Fig. 7. Illustration of the temperature-space features.
standard deviation of the measurement data and the simulated data per tem-
perature bin.

Fig. 8. Linear correlation coefficients between the different features.

an example of a quantity derived from measured and simulated glow


Fig. 5. A measured peak ratio Im3/ Im4 as a function of the fading time compared curves, namely the intensity of P3 divided by that of P4 . The agreement
to the simulation results. between simulation and measurement data is reasonable.

4. Data sets and simulations

The measurement data set used comprises of glow curves from


1,600 measurements for which the TL dosemeters have been irradiated
with doses ranging from 0.5 mSv to 10 mSv and with fading times be-
tween 30 min and 41 d. The dosemeters were not individually cali-
brated, but batch-wise. Details of the experimental setup and the
measurement data set can be found in Ref. Theinert et al. (2018).
For the simulated data set, a total of 100,000 glow curves have been
simulated. The dose values and fading times for which the glow curves
are calculated are randomly distributed between 1 mSv and 15 mSv and
between 0 d and 41 d, respectively.

5. Machine learning

Machine learning algorithms are known since decades and have


Fig. 6. Illustration of the time-domain features. been applied in a variety of scientific fields. With the ever-increasing
computational power of modern computer systems, the development
The statistical fluctuations of the simulated glow curves including de- and application of machine learning algorithms also outside the sci-
tector effects are smaller than the standard deviation observed for the entific realm has recently experienced a very strong boost. Artificial
data. This is the case for the majority of data sets because the dose- neural networks are one such class of algorithms. They are character-
meters were not calibrated individually and the intrinsic variation of ized by a set of input variables (features), one or several output nodes
the sensitivity is less than 5% for doses larger than 1 mSv. Fig. 5 shows and a set of hidden layers with a variable number of nodes connecting
the input and output layers. The simplest variant of an artificial neural

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K. Kröninger, et al. Radiation Measurements 125 (2019) 34–39

Fig. 9. Two-dimensional scatter plot of two features illustrating the sensitivity of the approach to the fading time.

Fig. 10. Predicted fading time as a function of the true fading time for the Fig. 11. Estimated total uncertainty of the reconstructed fading time (red line).
measurement data (blue markers) and for the simulation data (red line) in- Also shown are the uncertainty from non-linearities (dashed green line) and the
cluding the uncertainty band. (For interpretation of the references to colour in statistical uncertainties (dashed blue line and markers). The uncertainty esti-
this figure legend, the reader is referred to the Web version of this article.) mate from our previous studies (dashed orange line) is also shown, together
with the 50% and 100% uncertainty ranges. (For interpretation of the refer-
ences to colour in this figure legend, the reader is referred to the Web version of
network is a perceptron introduced in the 1950's (Rosenblatt, 1958) to this article.)
model information processing of the brain.
For the current study, we use the Multilayer-Perception im-
target result, in our case the fading time and the irradiation dose.
plementation of fully connected neural networks from the scikit-learn
During training, the weights are updated iteratively with a technique
package (Pedregosa et al., 2011) to infer on the irradiation dose and the
known as backpropagation that is most commonly used for the training
fading time. A fully connected neural network consists of layers of
of neural networks (Hecht-Nielsen, 1989). In each training iteration, a
neurons where every neuron is connected with all neurons in both the
loss is computed as measure of the deviation of the predicted to the real
previous and in the following layer. The first layer consists of the input
target values. We use the mean squared error as loss function. The al-
features. The output of each node is a function, the so-called activation
gorithm used to minimize the cost function during training is the
function, of its total input. A weighted linear combination of the out-
Limited-Memory BFGS optimizer (Liu and Nocedal, 1989).
puts of the nodes of a layer is the input for the next layer of neurons.
The large amount of neuronal interconnections results in a large
The weights of those linear combinations are randomly initialized and
amount of trainable parameters. Neural network trained on too few
need to be adjusted to match the given data set to predict new data.
input samples are analogous to a high order polynomial fit to few data
This adjustment process is called training and uses data with a known

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K. Kröninger, et al. Radiation Measurements 125 (2019) 34–39

Additionally, feature engineering is used for this study to reduce the


number of input parameters while keeping a maximum of information
about the glow curve. Using all available features like the time or
temperature resolved photon counts results in a large amount of
trainable features and is not necessary. Instead, a lower number of
features which are highly correlated to the irradiation dose and the
fading time is derived from the glow curve using the presented glow
curve model. The extracted features are presented in the next para-
graph.
The variables used as input to the neural network are calculated
from two sources, the recorded glow curve in the time domain and the
fitted glow curve in temperature space. For the former glow curve they
include three time intervals t(i/4)N with i = [1,2,3]. They denote the time
points up to which 25%, 50% and 75% of the total photon count N
within the region of interest (RoI), in which the signal is significantly
larger than the background, has been recorded. Also, the time point
Fig. 12. Predicted irradiation dose as a function of the true dose for the mea- tmax , at which the global mode of photon counts Imax occurs, is used as
surement data (orange markers) and for the simulation data(blue markers). The feature. All these time points are normalized to the length of the RoI
bottom plot shows the relative difference between the prediction and the true
tRoI = tRoI;up − tRoI;low . The four respective photon intensities I(i/4)N and
dose. (For interpretation of the references to colour in this figure legend, the
Imax are also used as input features.
reader is referred to the Web version of this article.)
For the latter glow curve they include the fit parameters Tm, i , Ei and
Im, i with i = [2,3,4,5] for the observed glow peaks as well as the peak
integrals Ni and several peak ratios. Figs. 6 and 7 illustrate these two
feature sets, respectively. These variables characterize the glow curves.
The features are preprocessed by scaling the individual feature dis-
tributions to mean values of 0 and standard deviations of 1. The scaled
variables are then decorrelated using principal-component analysis
(Jolliffe and Cadima, 2016).

6. Fading time estimation

The three features with the largest sensitivity to the fading time are
the peak ratio (Im2 + Im3)/(Im4 + Im5) , the 25%-quantile of the glow
curve, t(1/4N )/ IRoI and the peak ratio Im3/ Im5 . Some of the features used
show a correlation, e.g. the different peak heights and the total number
of photons recorded. Fig. 8 shows a matrix of the linear correlation
coefficients of the input features used and the network output predic-
tion. This linear correlation with the predicted values can be inter-
Fig. 13. Estimated total uncertainty of the reconstructed dose (black line). Also preted as a measure of a single feature's importance for the prediction.
shown are the systematic and statistical uncertainty as well as the 5% and 10% The coefficients can be positive and negative and their absolute values
uncertainty ranges. can range from small values (|ρ| = 0.05) to rather large values
(|ρ| = 0.89). The feature space is thus decorrelated to help the shallow
points. The excess of model complexity results in precise reproduction neural network distinguish between different fading times.
of known data but fails to generalize on unseen, new data. This is called The sensitivity of the features chosen can be demonstrated by two-
over-fitting (Piotrowski and Napiorkowski, 2013) and its monitoring is dimensional scatter plots. Fig. 9 shows such scatter plots for four dif-
of high importance in machine learning. ferent fading times of zero days, two days, 16 days and 41 days. While
As a first step to reduce the probability of over-fitting considering the projections onto the individual variables (diagonal plots) already
the size of our data set being relatively small in terms of machine shows a reasonable discrimination power, the two-dimensional scatter
leaning, we choose a neural network accordingly. We minimize the plots (off-diagonal plots) make the potential of these features to dis-
training parameters by using a shallow neural network that features one criminate between different fading times even more visible.
hidden layer with one more node than there are input nodes, and it only The output of the neural network is a single figure that is an esti-
has one output node. mate of the true fading time and which shows no residual dependence
Another method to observe generalization of the trained network is on the irradiation dose. Fig. 10 shows the predicted fading time as a
called cross-validation and is a commonly used tool (Stone, 1974). For function of the true fading time for the measurement data and for the
this technique, the training data is split up into n equally sized folds, simulation data including the corresponding uncertainty band. The data
n = 8 folds are used in our study, resulting in training and validation are averaged over all doses and the same neural network is used for
data set fractions of 87.5% and 12.5%, respectively. The weight-ad- both measurement and simulated data. Measurement and simulated
justment is performed on n − 1 folds. The last fold is used as validation data up to true fading times of about 32 days are consistent with a
data set. The average performance of n individually trained networks linear trend with a slope of unity. A negative bias is observed for larger
on each of the validation sets respectively, is used to provide a more fading times is visible and accounted for as systematic uncertainty.
reliable measure of the network performance on new data. A final Fig. 11 shows the estimated uncertainty of the reconstructed fading
evaluation is performed on an additional test set that was not part of the time. The method of uncertainty calculation is presented in detail in
training process. Simulated data are used for the training and testing Ref. Theinert et al. (2018). The measurement data is used only for the
process for the estimation of the irradiation dose, and they are solely uncertainty calculation, no simulation data is included. The latter are
used for comparison for the estimation of the fading time. only used to test the linearity of the estimator.
The total uncertainty of the fading time estimation (red line)

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K. Kröninger, et al. Radiation Measurements 125 (2019) 34–39

increases almost linearly and ranges up to three days for a true fading particular shallow neural networks, for the analysis of glow curve data
time of 30 days. It is computed as the squared sum of a statistical from LiF thermoluminescent dosemeters. The data set used was com-
(dashed blue line) and a systematic uncertainty(dashed green line). The posed of measured data from irradiated dosemeters and simulated data
statistical uncertainty is estimated with a quadratic fit to the standard based on an effective glow curve model and a parameterization of the
deviations of the results (blue markers). In the given measurement data kinetic parameters. We have demonstrated that it is possible to estimate
set, they are largest for the measurement data with an irradiation dose the fading time in the clinically relevant time interval of 30 days with
of 0.5 mSv. The shown systematic uncertainties in Fig. 11 represent an uncertainty of up to 10% and to estimate the irradiation dose for
therefore an upper limit for the whole irradiation dose range. doses larger than 1 mSv with an uncertainty of less than 10%. The study
The systematical uncertainty is estimated using the fit of a quadratic thus shows that it is possible to overcome the problem of fading without
function as well but to the absolute value of the difference of predicted using an additional preheating step (Walbersloh and Busch, 2015; Lee
and true fading time. The 50% and 100% uncertainty ranges are in- et al., 2015), and that information about the time of the irradiation can
dicated to guide the eye. The result from our previous studies using a be estimated. This is a significant advantage over other passive dose-
single peak ratio feature for fading time estimation (Ref. Theinert et al., meters, e.g. film-badge dosemeters.
2018) is included (orange dashed) for a comparison of methods. It is The applicability of the approach followed here for the clinical
clearly shown that the uncertainties are significantly reduced with the routine will be investigated in field tests. This includes an individual
neural network method presented within this study. Especially the di- calibration of the dosemeters. In further studies, we will also exploit the
vergence of uncertainties for longer fading times described in Ref. potential of machine learning algorithms to give further information
Theinert et al. (2018) can be eliminated with the new approach. about the irradiation, e.g. the type of radiation and the distinction be-
tween a single irradiation (accident scenario) and continuous irradia-
7. Irradiation dose estimation tion (missing radiation protection scenario).

Neural networks, as well as other machine learning algorithms, can References


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8. Conclusions and outlook

We have presented a study of using machine learning algorithms, in

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