Research Article |
Corresponding author: Vladimir A. Stepanov ( stepanov@iate.obninsk.ru ) Academic editor: Sergey Ulin
© 2022 Pyotr B. Baskov, Gleb V. Marichev, Vyacheslav V. Sakharov, Vladimir A. Stepanov.
This is an open access article distributed under the terms of the Creative Commons Attribution License (CC BY 4.0), which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.
Citation:
Baskov PB, Marichev GV, Sakharov VV, Stepanov VA (2022) Nuclear-optical converters for detecting intense neutron. Nuclear Energy and Technology 8(1): 31-36. https://doi.org/10.3897/nucet.8.82558
|
In the design of nuclear-optical converters (NOC) for detecting intense neutron fields (fluxes over 1015 cm–2·s–1), it is proposed to use hybrid gas ionization chambers (IC), in which electrical and optical neutron detecting methods are combined. For hybrid ICs, a technology is proposed for obtaining radiation-resistant and mechanically strong radiator materials capable of operating at temperatures of up to 1000 °C. This technology is based on solid-phase boron diffusion saturation of steel. It is shown that, at thermal neutron fluxes of 1×1010 n/(cm2·s) and higher, the integral intensity of argon luminescence as a result of ionization by α-particles and 7Li ions from layers of boride phases is sufficient for detection.
The combination of optical and radiation properties of multicomponent fluoride glasses makes it possible to use them as condensed active substances of NOCs. Choosing the elemental and isotopic composition, it becomes possible to use fluoride glasses for multichannel neutron detection as well as to significantly simplify the procedure for separating gamma and neutron components of radiation under conditions of intense radiation fluxes. It has been experimentally shown that in irradiation with a neutron flux of 1×1017 n/(cm2·s), the intensity of Nd IR luminescence in glasses based on zirconium fluoride (ZBLAN) increases in the presence of Gd, which interacts with neutrons.
Neutron detectors, gamma detectors, nuclear-optical converter, ionization chamber, scintillator, fluoride glass, intense neutron field
The need to improve the existing and build new neutron detectors is explained by the changing conditions of operation for radiation devices. Thus, temperatures of up to 700 °C, neutron fluxes of up to 1×1017 cm–2·s–1, gamma dose rates of up to 1×102 Gy/s and vibrations of up to 200 Hz are already reached in the reactor core. Providing neutron diagnostics in reactors with such characteristics requires extending the capabilities of neutron detectors based on an electrical principle of operation via combinations with radiation luminescent detection or by switching altogether to radiation photonics systems. As small noise as possible can be achieved in radiation photonics systems under high temperature while persevering proportional detection of high-rate radiation fluxes.
Evolution of neutron detection optics is associated with the development of the nuclear-optical converter (NOC) intended to provide an autonomous neutron monitoring channel. The NOC has the following key functional components:
Development of each NOC component is a pending issue. Alternate solutions for the structural micro- and nanoscale arrangement of the NOC fiber-optic translators with the required operating strength under extreme external impacts can be found in (
Neutron diagnostics in current control and protection systems of the reactors in operation is based on 3He counter tubes and ICs using 235U, 232Th and 10B isotopes, the principle of action for which was developed as long ago as in the 1970s. An IC is a gas-filled pressure vessel with two electrodes to which an electrical potential difference is applied. Materials containing neutron-interacting isotopes are used as the IC radiator. Reactions with neutrons result in the working gas ionization by nuclear transformation products, and the ionization charge gets on the chamber’s electrodes and is transmitted to the external electric circuit (
A detection system, based on radiation photonics technologies but using common fission chambers for detection, is developed in a hybrid chamber (
Apart from electrical signals from a traditional IC, such system detects the working gas bursts and glows which accompany nuclear reactions, this improving the reliability of detection and extends the neutron flux detection range. An optic fiber is used as the channel for transmission of optical signals from the fission chamber working gas scintillations. The problem of the radiation and temperature stability of the functional components and these to be joined into a single sensitive element needs to be addressed in the hybrid fission chamber. The problem of the thermomechanical stability of radiators is resolved by forming a stable boron-containing coating on stainless steel.
Natural boron consists of two stable isotopes: 10B (19.57%) and 11B (80.43%). The characteristics of the stable boron isotope interaction with thermal neutrons are presented in Table
Characteristics of the stable boron isotope interaction with thermal neutrons (
Isotope | % of content in natural material | (n,α)-reaction cross-section with 0.025 eV, barn | (n,γ)-reaction cross-section with 0.025 eV, barn | Reaction of interaction with neutrons |
---|---|---|---|---|
10B | 19.57 | 3840 | 0.5 | 1) 10B(n,α) → Li7*+ α+2.31 |
2) 10B(n, α) → Li7+ α+2.79 | ||||
3) 10B(n,γ) → 11B | ||||
11B | 80.43 | 0.005 | 50·10–3 | 11B(n,γ) → 12B |
(T1/2 = 0.019 s) |
Unlike uranium, thorium and lithium isotopes used in radiators, boron, along with a large thermal neutron absorption cross-section, forms highly radiation- and heat-resistant compounds. Surface boration, e.g. for iron, cast iron and steel, is known to lead to coatings with formation of iron borides with a high surface hardness, wear resistance, heat resistance and corrosion stability (
Stainless steel was selected in this study as the basis for saturating the 84% В4С+16% Na2B4O7 paste and the BF-4 glue in acetone. The saturation took place at 1000 °C with a protective layer composed of 50%B2O3+50%SiO2. It was shown using an X-ray phase analysis that such chemicothermal treatment leads to a solid layer of Fe2B and FeB borides formed on the surface. The microstructure of the radiator sample section is shown in Fig.
To estimate the efficiency of such radiator, we shall assume that, as shown in Table
10B + n0 → 6Li* + α → 7Li (0.83 MeV) + α (1.47 MeV) + γ (0.48 MeV) (93%);
→ 7Li (1.0 MeV) + α (1.8 MeV) (7%).
The ion fraction, f (x), escaping into the gas from depth x from the electrode surface is
f (x) = 1/[2(1 – x/R)],
and the overall fraction of the ions escaping into the gas is obtained with coating thickness s being larger than ion range R
.
The results of calculating the He and Li ion fluxes from borated steel layers are shown in Table
Phase | ρ, g/cm3 | Neutron absorption factor, cm–1 | α (1.47 MeV) | 7Li (0.87 MeV) | ||||
---|---|---|---|---|---|---|---|---|
Range R, μm | f | Flux q, 1010 ion/(cm2s) | Range R, μm | f | Flux q, 1010 ion/(cm2s) | |||
FeB | 5.1080 | 34.64 | 2.96 | 0.1850 | 6.41 | 1.82 | 0.1138 | 3.94 |
Fe2B | 6.0273 | 22.24 | 2.71 | 0.1694 | 3.77 | 1.39 | 0.0869 | 1.93 |
Argon suits best for the hybrid chamber working medium. This is explained by the fact that the arc and spark spectra of argon consist of many lines (about 900) situated in the spectral region between 400 and 706 nm (
Results of calculating the luminous intensity of the hybrid chamber argon during thermal neutron irradiation of 1×1010 n/cm2s
Ion | FeB | Fe2B | ||||
---|---|---|---|---|---|---|
Eav, MeV | Ion energy flux, 1010 MeV/(cm2s) | Luminous intensity I, mW/cm2 | Eav, MeV | Ion energy flux, 1010 MeV/(cm2s) | Luminous intensity I, mW/cm2 | |
α | 0.818 | 5.243 | 0.251 | 0.752 | 2.835 | 0.136 |
7Li | 0.492 | 1.938 | 0.093 | 0.195 | 0.376 | 0.018 |
The full solid angle luminous intensity will be up to 0.3 mW. Even with the inevitable loss in the course of the radiation fiber interception in the hybrid chamber, such intensity will allow confident neutron flux detection starting with 1×1010 n/cm2s.
Condensed oscillators have long been used as the NOC working medium (
Table
Material | Density, g/cm3 | Luminescence time, 10–9 s | Wavelength in spectrum maximum, nm | Energy conversion efficiency, % (for electrons) |
---|---|---|---|---|
Anthracene, C14 H10 | 1.25 | 30 | 445 | 4 |
Stilbene, C14H12 | 1.16 | 6 | 410 | 3 |
NaI (Tl) | 3.67 | 250 | 410 | 6 |
ZnS (Ag) | 4.09 | 11 | 450 | 10 |
CsI (Tl) | 4.5 | 700 | 560 | 2 |
CaF2(Eu) | 3.18 | 940 | 435 | 3 |
Bi4Ge3O12 | 7.13 | 350 | 480 | 0.6 |
CdWO4 | 7.90 | 1000 | 530 | 1.2 |
Glass, SiO2(Ce)-Li | 2.2 | 200 | 480 | 5 |
HBLAN (Ce) | 6 | 25 | 320 | ~1 |
With gamma radiation and neutron components being simultaneously detected, the optical scintillations caused by neutrons and gamma quanta are separated as the result of processing statistically the amplitudes and time responses of individual scintillations. They differ during the interactions of gamma quanta and neutrons with the material (
Such detection method often leads to major uncertainties, specifically in high neutron fields with fluxes of over 1×1015 cm–2·s–1. First, to implement a statistical analysis of scintillations, representative luminescence times shall not exceed a few to tens of nanoseconds to avoid the signal interferences. However, individual, even short oscillations coalesce to form a solid background in high radiation fields, this making it completely impossible to investigate their shape and duration. Second, short scintillations of optically active impurities in materials turn out to be in visible and ultraviolet bands, in which major optical degradation of the materials as such takes place with the growth in the radiation exposure dose (
The above issues are coped with by using multicomponent glasses and by giving up the method of counting and analyzing individual scintillations from radiation fluxes (
Glasses based on hafnium and zirconium fluorides were studied for using fluoride glasses as the NOC working medium (
HBLAN – 54%HfF424%BaF23%AlF318%NaF1%InF3, ZBLAN – 52%ZrF420%BaF24%LaF34%AlF320%NaF.
Nuclei of hafnium and zirconium elements differ greatly in terms of the neutron interaction cross-section but glasses based on these have similar optical properties. Fig.
With ionizing irradiation, fluoride glasses luminesce in the UV and visible spectrum ranges (Fig.
Fluoride glasses in conditions of radiation effects are transparent in a broader wavelength range than crystals and glasses based otherwise. Irradiated fluoride glasses restore their optical properties in the process of photoelectric annealing. Photoelectric restoration of the optical properties of gamma irradiated fluoride glasses is effective with light intensities of just 1 mW/cm2 (
Isotopes with a high (n, α) reaction cross-section (6Li, 10B) or a high probability of the (n, γ) radiative capture reaction (Hf, Cd, Gd, ,I and others) may be chosen when selecting the elemental composition for detection of radiation fluxes as interacting with neutrons of the glass components. Radiative capture involves nearly instantaneous liberation of energy of about 7.5 MeV in the form of gamma radiation that is absorbed and ionizes the glass. Fig.
Fig.
The NOC luminescence spectra are the Nd luminous spectra with a band with the maximum of 900 nm and a narrow line at 1050 nm. The luminescence from the ZBLAN(Nd) element is associated only with the reactor gamma radiation. The neutron component of the radiation field is another contributor to the ZBLAN(Nd,Gd) luminous intensity. This is clearly seen when comparing the luminous intensity of glasses with and without Gd, as well as during irradiation with fast and thermal neutrons for which the Gd (n,γ) reaction cross-section differs by several orders of magnitude (see Fig.
Hybrid gas ICs, which combine electrical and optical methods of neutron detection, are proposed in developing a NOC for detection of high neutron fields (fluxes of over 1×1015 cm–2·s–1). A technology for producing radiation-resistant radiator materials fit for service at temperatures of up to 1000 °С is proposed for hybrid ICs. Solid-phase diffusive boron saturation of 12Kh18N10T steel makes it possible to produce IC radiators with FeB and Fe2B phase layers with a thickness of up to 50 μm and a microhardness of up to 9.1 GPa. It has been shown that with a thermal neutron flux of 1×1010 n/cm2·s, the integral luminous intensity of argon from ionization with alpha particles and 7Li ions is 0.35 mW/cm2 from FeB phase layers and 0.15 mW/cm2 from Fe2B phase layers.
Combining the optical and radiation properties of multicomponent fluoride glasses enables their use as the condensed NOC working media and in integral neutron and gamma flux detectors. Major variations of the elemental and isotope compositions can be used to increase the sensitivity to the neutron and gamma components of high-rate radiation fluxes and optimize the energy conversion efficiency of glasses. It has been shown experimentally that the luminous intensity of Nd (900 and 1050 nm) in ZBLAN glasses with the addition of a Gd impurity, which is active to neutrons, increases during neutron irradiation of 1×1017 n/(cm2·s) and gamma quanta irradiation of 1×105 Gy/s. The neutron spectrum degradation leads to an increased luminous intensity of the ZBLAN glass with Gd thanks to an increased cross-section of interaction with neutrons.