The invention relates to a criticality accident dosimeter that provides accurate and personal absorbed doses following an accident. More specifically, this invention relates generally to multi-element alanine dosimeter holder with filters.
Personal dosimeter that is capable of providing timely information is critical for absorbed dose assessment and individual medical treatment following an accident. The Health Physics Society Standards Committee (HPSSC) notes in the current Dosimetry for Criticality Accidents Standard (ANSUHPS N13.3-2013), that “rapid and accurate assessment of personal absorbed doses resulting from a criticality accident may be of the utmost importance for exposed individuals and assisting with their medical treatment.”
Existing Nuclear Accident dosimetry (NAD) or Criticality Accident Dosimetry are based on the activity measurements of the activation products. Dose measurements often require the use of sensitive but expensive counting equipment. While gamma spectrometers are used for indium, copper and gold, and beta counters are used for sulfur. The necessary counting equipment is usually not easily transportable due to the significant weight of the shielding materials used, and delicacy of the counters.
The measuring process can be both time and labor intensive. For example, in order to measure neutron dose in a broad energy range, several different foils need be measured, some of them with a special cover (e.g. cadmium). These time and labor consuming measurements need to be carried out by specially trained and experienced personnel. The typical time required for such dose measurements is about an hour per dosimeter. Moreover the results obtained in terms of activity require a number of corrections, e.g. time since the accident, sample geometry in order to calculate absorbed dose.
Another significant limitation of existing accident dosimeters is that they need to be analyzed within a very short time following an accident. This is due to the short half-life of the activated products:
Sulfur pellets are sensitive to neutrons with energies greater than 3.0 MeV by the reaction: 32S+n=32P+β, 32P→T1/2=14.29 days, beta-emitter with E=1.17 MeV
Indium foils are sensitive to neutrons with energies greater than 1.0 MeV.
There are several activation products from thermal neutron activation of indium. Only the 115mIn has a half-life greater than a few seconds. The reaction is: 115In+n=115mIn+γ; T1/2=0.188 days; gamma-emitter with E=0.336 MeV
Gold foil (bare and Cd-covered). The reaction is: 197Au(n−γ)198Au→T1/2=2.697 days, beta-emitter with E=0.411 MeV
This means that existing criticality dosimeters can be analyzed only once (due to the time constraint), and they are completely useless if not analyzed during the first week following the occurrence of an accident.
Therefore, it is highly desirable to have an inexpensive NAD, which can be read several times during at least one year following an accident, and only requires simple, easily transportable, and inexpensive equipment to read.
Alanine dosimetry is an internationally approved technique for dose measurement in various radiation fields. Alanine produces radicals (unpaired electrons) upon irritation. The number of the radicals is proportional to the radiation dose absorbed over a wide dose range. Crystalline L-α-alanine is a well-known material for Electron Paramagnetic Resonance (EPR) dosimetry, which is used in radiation laboratories in both reference and transfer dosimetry (Regulla, 2005; Baffa and Kinoshita, 2014). Because it is inconvenient to utilize a powder as dosimeter, alanine pellets, made from L-α-alanine powder mixed a binder (such as 10-20% of paraffin), are used for dosimetry. Typical standard alanine pellets have a diameter of 4.5 mm, and a height of 3.5 mm. The ISO/ASTM 51607-2013, Standard Practice for Use of the Alanine-EPR Dosimetry System, provides official guidance for its use.
Alanine dosimeters have several advantages over other dosimeter products. They are small, compact and easy to handle and are characterized by low influence of temperature, humidity and dose rate. Alanine dosimeters also offer a wide measuring range from 2 Gy to 200 kGy, which makes them applicable for radiation therapy, blood components irradiation as well as industrial irradiation.
The L-α-alanine's superior dosimetry properties over other dosimeter products include:
Despite the many advantages of Alanine dosimetry, its application is still limited by a few problems. Hayes et al., (2000) reported an accuracy of 10% for 100 mGy dose measured in alanine pellets in a blind intercomparison. Irradiated alanine dosimeters, which were stored, exhibited compound spectral EPR signal fading of ca 3% over 9 months. While the report is encouraging, the tests have to be carried out in a complex method, which utilize multiple techniques, such as polynomial filtration of the EPR spectrum, dosimeter rotation during scanning, subtraction of all non-radiogenic signals. The method also requires the use of an EPR standard, which is inserted into the resonator during measurement.
In 2008, Trompier et al., reported results of alanine dosimeters measurements of neutron doses in a criticality accident exercise at the CALIBAN irradiation facility. In this dosimetry study, photon contribution was measured by TLD in Al2O3 powder, which was subtracted from the total dose measured by EPR spectrometry in Alanine pellet. Table 1 demonstrates that alanine dosimeters were able to provide results for neutron dose measurements that is comparable to other dosimetric techniques.
However, an additional independent dosimeter and processing equipment (TLD) must be used to measure photon dose before the accurate neutron readings can be produced. Furthermore, alanine dosimeters has relatively low sensitivity to neutrons, e.g. especially to thermal neutrons.
In order to increase its neutron sensitivity it was proposed to add 5% of Gd2O3 to the composition of alanine pellets. Gd2O3 doped alanine pellets were found to increase the EPR signal by a factor of 3.45 in case of PMMA phantom (Marrale et al., 2015). Having two types of alanine pellets with different sensitivity to neutrons gives an opportunity to build a new type of criticality dosimeters based on the same dosimetric material (alanine) and the same method of readout, e.g. EPR. However, because Gd2O3 doped alanine pellets is not commercially available, its application as NAD is significantly limited.
The present invention aims to improve criticality accident dosimetry. The criticality accident dosimeter of present invention provides better neutron sensitivity, and is capable of discriminate photon and neutron dose contributions without requiring special Gd2O3 doped alanine pellets or additional photon dosimeter.
Instead of using two types of alanine pellets with different composition (e.g. with and without Gd2O3), this invention proposes a new design of criticality accident dosimeter based on the same dosimetric material (alanine) and the same method of readout, e.g. EPR. In order to enhance the photon-neutron differentiation of alanine, filters made of material that is capable of improving alanine's neutron sensitivity are placed in front of standard alanine pellets.
It is well known that some materials, such as cadmium and 6Li, can convert neutrons into other types of particles to which alanine has higher sensitivity. A number of materials exist with high neutron-capture cross sections. The capture of neutron then directly or indirectly provides particles that subsequently produce radiation-induced radicals in alanine. A partial list of these types of nuclear reactions is given below:
n+
6Li→α+3H (1)
n+
113Cd→114Cd*→114Cd+γ (2)
n+
157Gd→158Cd*→158Cd+γ (3)
In case of a 6Li filter, the neutron irradiation will generate a particles and tritium ions as a result of the reaction (1), which will produce radiation-induced radicals in alanine pellets placed behind the filter. In case of a cadmium filter, neutrons will produce a photon component (see nuclear reactions (2) and (3)) contributing to the dose measured by the alanine pellet behind the cadimium filter. Although reactions (1-3) are well known in the field. No one has applied these reactions in NAD design. Without building a prototype, and experimentally measuring the effect of the neutron sensitivity enhancement, it was unclear if this dosimetry design is feasible or sensitive enough for NAD application.
A criticality accident dosimeter of the present invention, comprises at least four alanine pellets, of which at least two of the alanine dosimeter pellets are placed behind a filter; wherein said filter enhances the sensitivities of said alanine dosimeter pellets covered by the filter. The filter may be made of 6Li or cadmium. The personal criticality dosimeter of the present invention upon exposure to ionizing radiation, can produces radicals that remain stable for at least a year.
In one embodiment, a personal criticality accident dosimeter of present invention for ascertaining radiation dosage comprising: at least four alanine dosimeter pellets, and a dosimeter holder, which comprises a plurality of supports, each designed to hold one said alanine dosimeter pellet and a 6Li filter or a cadmium filter, wherein said 6Li filter or a cadmium filter covers at least two of said alanine pellets.
Referring to
In another embodiment, a personal criticality accident dosimeter of present invention for ascertaining radiation dosage comprises: at least two standard alanine dosimeter pellets 24, and at least two enhanced alanine dosimeter pellets 28, wherein said enhanced dosimeter pellets is made by adding one or more filter chip/pellets 27 to an alanine dosimeter pellet as shown in
Two types of dosimeter holder have been designed and built (as shown in
Type 1 dosimeter holder is designed to hold four standard alanine pellets (size 4×2.4 mm, AERIAL®, Illkirch—France) without any filtration and another four standard alanine pellets placed behind a 6LiF filter when the holder is closed. Standard 6LiF pellets (size 3.6×0.015 mm) were used as 6LiF filter. These 6LiF pellets were purchased from Thermo Eberline LLC (Franklin, Mass.). In order to check the effect of 6LiF filter thickness on sensitivities of dosimeter, 6LiF filter thickness (e.g. three, two and one 6LiF chips) are ted.
Type 2 dosimeter holder is designed to hold four alanine pellets without any filtration and another four alanine pellets behind a cadmium filter (44×15×0.5 mm).
Neutron Irradiation: 20 MW research reactor of the National Institute of Standards and Technology (NIST) was utilized for the testing of the prototype holders. The reactor is D2O cooled and moderated. The core is comprised of thirty enriched-uranium fuel elements of a unique, split-core design. It utilizes low-energy neutrons, which are often described as thermal and cold. Reactor neutron imaging station BT2 was used for the holders' irradiation. The irradiation was done on the standard ANSI PMMA phantom (as shown in
Gamma Irradiation: an AFRRI Co60 source was utilized for the testing of the prototype holders with similar set up.
A Bruker ELEXSYS 500 (Bruker BioSpin, Billerica, Mass.) spectrometer equipped with a super-high-Q resonator ER 4123 SHQE in the X-band (9-10 GHz) was used for the measurements. All four pellets irradiated under the same conditions were put together into a sample tube and measured. Table 3 shows the recorded settings. The EPR measurement (dose evaluation) takes only 3.5 minutes (Table 3). For statistical purposes, the measurement of each sample was performed for five times.
According to Trompier et al., 2008 the total EPR radiation response of alanine at mixed neutron-photon irradiation in terms of its sensitivity to 60Co gamma rays, R can be generally described by the following formula:
R=kD
n
+hD
γ (1)
Where k is the sensitivity of alanine to neutrons relative to 60Co gamma rays, h is alanine sensitivity to the photons relative to 60Co gamma rays. Both sensitivities are measured in terms of the EPR radiation response per dose unit. Dn and Dγ are the neutron and photon absorbed doses in tissue. In case of alanine use without different filtration, it is impossible to determine photon and neutron doses separately. Therefore 2008 Trompier et al. 2008 additionally used thermoluminescent dosimetry (Al2O3) to measure photon dose alone. If there is a holder with alanine pellets behind different filters then Eq. (1) can be written for each filtration separately and neutron and photon doses can be determined without the use of additional dosimeters, e.g. TLD. In case of holder prototype using a cadmium filter the system of two equations can be written in the following way:
Dγ in the first equation can be substituted by the second equitation:
This equation can be solved relatively to Dn:
Eqs. (8) and (9) allow to calculate neutron and gamma absorbed doses if the proposed prototype with a cadmium filter was used. Data (k, h, and R) from Tables 3 and 4 allow to verify the correctness of the proposed equations i.e. that the calculated neutron and photon doses are equal to the actually delivered neutron and photon doses.
In the case of the prototype with a 6LiF filter similar equations (with the change of Cd to Li) can be proposed for neutron and gamma dose calculations, as follows:
The simulated neutron flux spectrum, neutron dose rate spectrum, core gamma flux spectrum, and core gamma dose rate spectrum (with the cooled 10 cm bismuth filter in the beam) are shown in
Thus neutron and photon doses for any photon-neutron mixture can be calculated by measuring the EPR response of alanine pellets irradiated in the proposed holders and using the determined parameters h and k.
The experiments on prototype dosimeter holders demonstrated that the proposed cadmium and 6LiF filters (convertors) increase the sensitivity of alanine to neutron irradiation by almost a factor of five. The latter makes alanine even more sensitive to neutrons than to photons. Normally its sensitivity to neutrons is significantly lower than to photons.
Proposed and tested holder designs in combination with the developed dose algorithm allow to measure neutron and photon doses separately using only EPR measurements in alanine. This makes the entire dose measurement process fast (<10 min) and requiring only one type of dose readout equipment (EPR).
A method for determining the radiation dose by Electron Paramagnetic Resonance (EPR) dosimetry using alanine criticality accident dosimeter, comprises of 1) providing a subject with a criticality accident dosimeter holder containing at least two alanine pellets and at least two alanine pellets covered by a cadmium filter or a 6Li filter; 2) measuring the EPR spectrum of alanine pellets contained in said holder after a radiation exposure; and c) determining neutron and photon radiation doses using EPR measurements from step 2; c) calculating radiation dose exposed to said subject.
This application claims priority from U.S. provisional application No. 63/082,511, filed Sep. 24, 2020, the content of which is incorporated herein by reference.
Number | Date | Country | |
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63082511 | Sep 2020 | US |