Production of NaCl pellets
The study examined three different salts (NaCl) (Table 1) compressed to pellets (Waldner and Bernhardsson 2018). Salt 1 was a commercially available rock salt while Salt 2 was a commercially available sea salt, both bought in Swedish supermarkets. Salt 3 was an analytical grade salt used for laboratory purposes (Scharlab, 99.5%). The NaCl pellets were produced using a specially-made tool (Promech, Sweden) and a hydraulic hand press (Hamron, Sweden) with a pressure of 0.8 tons per pellet. The pellets were 4 mm in diameter and about 0.8 mm thick, made from about 20 mg of NaCl with grain sizes between 100 and 400 µm. The pellets were produced at least 24 h before they were exposed to ionising radiation unless an exception is noted for the different experiments. After manufacturing the pellets were kept at room temperature in a laboratory with a combination of natural and artificial lighting. No additional optical or thermal bleaching was needed to zero potential background OSL signals. The produced pellets were visually identical and no additional controls were made to ensure that they were physically and dosimetrically identical beyond the properties previously investigated in Waldner and Bernhardsson (2018). In addition, any difference in dosimetric properties between pellets was corrected by the use of the calibration dose.
Table 1 Three types of salt used in the current study: Salts 1 and 2 were ordinary table salts bought in supermarkets, while Salt 3 was an analytical grade NaCl for laboratory purposes OSL signal readout
Readout of the OSL signal from NaCl pellets was performed using a Risø TL/OSL reader (TL/OSL-DA-15, DTU Nutech, Denmark), described in detail by Thomsen (2004). The reader was equipped with an internal 90Sr/90Y irradiation source (20 MBq as of 9 April 2009) with an absorbed dose rate of 0.77 ± 0.02 mGy s−1 (as of 1 February 2019) to quartz (calibration quartz, DTU Nutech, Batch 101). The dose rate to NaCl was 0.72 mGy s−1, calculated using a stopping power ratio of 0.938 (Berger et al. 2005) between NaCl and SiO2. Light stimulation was performed using continuous wave (CW) stimulation by means of blue (λ = 470 nm) LEDs. The photomultiplier tube used to detect the luminescence photons was equipped with a 7.5 mm thick Hoya U-340 filter, resulting in a detection window with maximum transmission at 340 nm.
Typically, the first minutes after irradiation the OSL signal decreases rapidly before it starts to stabilise after about 1 h (Waldner and Bernhardsson 2018), due to the emptying of the more shallow and unstable impurity traps in the NaCl. It is desirable to avoid any signal contributions of these shallow traps, which means that the unstable traps need to be emptied before readout of the OSL signal. This can be achieved by either waiting for the signal to stabilise on its own at room temperature or by heating the sample to remove the unstable part of the signal.
To investigate the optimal use of either a preheat or a pause, the readout protocol in Table 2 was used for OSL signal readout. The preheat temperature was kept the same in Steps 2.1 and 5.1 in Table 2 to ensure a reproducible fraction of emptied energy state traps in the crystal lattice after each irradiation.
Table 2 The protocol for OSL-signal readouts of NaCl pellets using the Risø TL/OSL reader Pellets of the three types of salt presented in Table 1 were subjected to the two readout protocols described in Table 2. In the assessment of the unknown signal, Su, no background correction was performed as the background signal was assumed negligible (all NaCl pellets had been pre-bleached in daylight). After the 1 h pause or preheat after exposure, the radiation-induced signal from each pellet was defined as the integrated number of luminescence counts registered during the first 5 s of the 20-s OSL signal readout with blue light stimulation. The OSL signal decreased rapidly during the first seconds of readout to a background which then decreased slowly. The integrated luminescence during the last 5 s of the recorded OSL signal decay curve was used as a background correction when further irradiations and readouts were performed on the same pellet since any additional induced signal will be added to the remaining background from the former readout. The calibration signal, Sc, was thus defined as the integrated OSL signal between 0 and 5 s of readout corrected for the background of the previous OSL signal readout between 15 and 20 s.
For some experiments, only Steps 1–3 of the readout protocol in Table 2 were used, and the signal was compared to the pre-established signal-dose response curve described in Waldner and Bernhardsson (2018). This curve shows the mean OSL signal from 10 NaCl pellets, read using Steps 1–3 of the protocol in Table 2, for several different increasing absorbed doses up to 300 mGy. Using such a curve provides a quick estimation of the absorbed dose, with uncertainties of about 10% (Waldner and Bernhardsson 2018) in the absorbed dose determination.
The procedure of using only the readout Steps 1–3 in Table 2 was also used to determine the calibration dose when the full readout protocol in Table 2 was used (Section “OSL signal fading and its dependence on preheating conditions”). According to previous work (Waldner and Bernhardsson 2018), a Dc twice the size of Du gives a good estimation of the absorbed dose for all salts at the absorbed dose levels used in the present investigation (< 50 mGy).
When using the full protocol in Table 2, the absorbed dose to the NaCl pellets was calculated according to Eq. 1.
$${D}_{u}=\frac{{S}_{u}}{{S}_{c}}\cdot {D}_{c},$$
(1)
where Du is the unknown dose, Dc is the calibration dose, Su is the signal after exposure to an unknown dose, and Sc is the calibration signal.
Optimisation of preheat temperature for NaCl pellets
The preheat temperature was optimised in two steps: first, it was determined whether heating the NaCl pellet affected its dosimetric properties, and second, it was investigated whether the chosen temperature was sufficient to empty the unstable electron traps in the crystal lattice.
Effects of preheating the NaCl pellet
When using a calibration dose to determine an unknown dose, it is important that the OSL signal per unit dose is the same for both the unknown exposure and the administered calibration dose (or that the relationship between the responses is known and constant). If the dosimetric properties change between the two irradiations, the unknown dose, Du in Eq. 1, will not be estimated correctly.
To investigate if the heating of NaCl before readout affects the dosimetric properties, and if so, at what temperature, several measurements were performed using the protocol in Table 2. The preheat was varied between 25 and 225 ºC in steps of 25 ºC, with all other parameters remained unchanged. The preheat temperature in Step 2.1 was kept the same as that in Step 5.1 (Table 2). For this investigation, the two given doses, Du and Dc, had the same value (21.6 mGy); hence, the corresponding signals Su and Sc were expected to be similar. The ratio of the unknown signal Su and the calibration signal Sc was calculated and compared for the different preheat temperatures. Any deviation from a value of 1 for this ratio was then interpreted as a change in sensitivity.
Time delay between preheat and readout
To investigate if the selected preheat was sufficient to empty the unstable traps in the NaCl, the OSL signal was read at several instances after the preheat. If the signal did not continue to decrease after preheat, then the chosen preheat temperature was considered to be sufficient. Five NaCl pellets were irradiated with an absorbed dose of 21.6 mGy and then preheated. After a pause following the preheat, the OSL signal was read. This was repeated nine times, with pauses between 0 and 400 s introduced between the preheat and readout steps, i.e., between Steps 2.1 and 3 in the readout protocol in Table 2.
OSL signal fading and its dependence on preheating conditions
In the present study, fading is defined as the decrease in the read OSL signal, Su, and estimated dose, Du, over time. To investigate the fading, the OSL signal was read on multiple occasions from different pellets after exposure to the same absorbed dose. For this, 100 NaCl pellets were irradiated by a 60Co gamma radiation source (Gammatron 3, Siemens, Germany) 24 h after production. The NaCl pellets were positioned in a PMMA phantom with a 5 mm build-up layer and then irradiated with an absorbed dose, Du, corresponding to 5 mGy to water. After this exposure, the pellets were kept in a light sealed plastic container intended for photographic films, to keep the signal from optical bleaching.
The OSL signal from the irradiated pellets was read at various times, from 1 h to 4 weeks after irradiation. Ten pellets were read on each occasion: five at room temperature after being preheated to the temperature determined in Section “Production of NaCl pellets” and five at room temperature without any preheat. After readout, the signal was compared to a pre-established signal-dose calibration curve (Waldner and Bernhardsson 2018) to estimate the absorbed dose from the 60Co source. Based on the estimated absorbed dose, a calibration dose, Dc, was determined and administrated to the pellets. For all three salts, Dc was set twice as high as the administered dose, Du. The calibration signal, Sc, was read after a preheat of 100 ºC for the first five pellets and after a 1-h pause for the other five pellets. The estimated absorbed dose was calculated using Eq. 1.
OSL signal yield over time
To investigate the OSL signal yield over time, NaCl pellets were irradiated, and the OSL signal read, on several occasions between one hour and one month after production of the pellets. The internal 90Sr/90Y source of the TL/OSL reader was used for the irradiations. After the pellets were manufactured they were kept in a transparent plastic container at ambient conditions. The Du administered to the NaCl pellets was at the same level (28.8 mGy) for each exposure. Two types of readout (Table 2) were used after irradiation: first, five pellets were read after a preheat (Step 2.1 in Table 2) at a temperature determined in Section “Production of NaCl pellets”, and second, five pellets were read after a pause of one hour using no preheat (Step 2.2 in Table 2). In this way, the OSL signal yield, or radiation sensitivity, of the NaCl pellets was determined as a function of time after pellet production for two types of signal acquisition.
Acute versus chronic irradiation
To investigate any potential effects of long-term irradiation and the influence of exposure with varying dose rates, NaCl pellets made from Salt 1 were placed in opaque packages on styrofoam blocks at different distances (40, 60 and 80 cm) from a 20 MBq 137Cs point source (Fig. 1). The use of varying distances from the point source was intended to mimic free air exposure with different ambient dose equivalent rates 4, 7, and 13 µSv/h, respectively, as determined using a handheld radiation detector (identiFINDER, FLIR, United States). These dose rates resulted in cumulated doses of around 3–10 mGy to the NaCl pellets after 5 weeks which is well above the detection limits of the NaCl pellets but in the relevant range for personal dosimetry. At each distance from the radiation source, five packages of pellets, each containing five NaCl pellets, were placed on individual styrofoam blocks. One package per distance was removed for readout (full readout protocol with pause, Table 2) after 1, 2, 3, 4, and 5 weeks of exposure to achieve five different total absorbed doses with three different dose rates. The dose rate effects were expected to be the same for the three salts (Table 1), which is why only one salt (Salt 1) was investigated. Scattering effects were not considered as the aim was only to have a constant dose rate at each styrofoam block for the 5 weeks of measurements.
Uncertainty calculations
Uncertainties were calculated using error propagation (Eq. 2). When irradiating and reading the OSL signal twice from the same NaCl pellet, i.e., twice repeating Steps 1–3 in Table 2, all dosimetric properties were assumed to be unchanged. This means that the unknown signal and calibration signal were not independent of each other but were likely correlated. Thus, their covariance needed to be accounted for in the uncertainty estimate.
$${\left(\frac{{\sigma D}_{NaCl}}{{D}_{NaCl}}\right)}^{2}=\left({\left(\frac{\sigma {S}_{u}}{{S}_{u}}\right)}^{2}+{\left(\frac{\sigma {S}_{c}}{{S}_{c}}\right)}^{2}+{\left(\frac{\sigma {D}_{c}}{{D}_{c}}\right)}^{2}-2\cdot r\cdot \frac{\sigma {S}_{u}}{{S}_{u}}\cdot \frac{\sigma {S}_{c}}{{S}_{c}}\right),$$
(2)
where σ denotes the uncertainty of the previously described variables and r is the correlation factor.
Figure 2 shows a graph of Su as a function of Sc, read from the same NaCl pellet after two exposures with the same dose, repeated for different absorbed doses. The correlation, r, between Su and Sc is obtained as the square root of the Pearson R2 value in Fig. 2. For these data, the correlation was 0.9996, and the uncertainty contribution from Su and Sc thus became very small.