Radioluminescence of LiF:Mg,Ti induced by 4 MeV electrons

This paper reports on the radioluminescence characteristics of LiF:Mg,Ti induced by 4 MeV linear accelerator electrons. The main emission peak of the luminescence is found at 410 nm, but weaker emission occurs around 320, 360, 460, 520 and 560 nm as well. The relative intensities of the emission bands show a strong dependence on the Mg concentration of the sample. The radioluminescence signal reaches its maximum typically 1.5 ms after the irradiation pulse, and decays with a half-life of 4–6 ms. Both the build-up time and the half-life decreases with increasing Mg concentration. The luminescence yield shows a strong dependence on the irradiation dose.     

LiF:Mg,Ti (MTT) TL detectors optimised for high-LET radiation dosimetry

The properties of LiF:Mg,Ti (distributed as, e.g., TLD-100 or MTS-N), the most frequently used thermoluminescent detector, have been optimised for measurements of sparsely ionising radiation (gamma rays), typically encountered in radiation protection or clinical dosimetry. However, these detectors need also to be applied in conditions of mixed-field dosimetry with a high-LET component, such as those encountered in heavy ion beams or in space.

At the Institute of Nuclear Physics in Kraków a new type of LiF:Mg,Ti detector (named MTT) has been recently developed through modification of its dopant composition. This composition is intended to increase the detection efficiency after a dose of high-LET radiation. The concentration of dopants in the MTT material is: C_Mg=50 ppm, and C_Ti=120 ppm, i.e. about a three times less of magnesium and about 10 times more of titanium content, compared with the standard MTS-N. The MTT TL detectors feature an increased relative efficiency to high-LET radiation, which for 5 MeV alpha-particles is about twice that of standard LiF:Mg,Ti. The response of MTT detectors has been studied in charged particle beams of the HIMAC accelerator in Chiba, Japan and in Dubna, Russia. The main foreseen application of MTT detectors are dose measurements in space. The dose after high-LET exposure can be estimated from the difference of the response of MTS and MTT detectors. In the near future MTT detectors will be applied in the “Matroshka” experiment. Within this experiment a specially constructed human phantom will be exposed in free space (outside the International Space Station) for 1 year. The phantom will incorporate a few thousand measuring points enabling radiation doses to particular organs to be determined.     

Spectral characteristic of high-dose high-temperature emission from LiF:Mg,Cu,P (MCP-N) TL detectors

High-temperature emission spectra of LiF:Mg,Cu,P (MCP-N) TL detectors, irradiated above the nominal saturation level, up to the hundreds of kGy, have been measured. Emission spectra integrated over the whole temperature range, as well as the spectra recorded at the temperatures corresponding to the TL peaks maxima, were analyzed. With increasing dose of γ-radiation no significant changes were observed in the short wavelength emission range (220–450 nm) of the measured spectra. For doses of 4 kGy and higher the long wavelength emission (450–800 nm) started to be visible. All recorded spectra have been expressed in a form of the sum of several Gaussian-shape bands in the energy domain, which parameters remain in a general agreement with the measurements of Mandowska et al. (2010). Spectra of the low-temperature, main, high-temperature and “B” TL peaks were investigated. In the ranges of the low-temperature and the main dosimetric peaks, that is 100–125 and 210–230 °C, respectively, the short wavelength emission disappeared with increasing dose and for the highest doses the long wavelength emission became dominant. Both the high-temperature (290–320 °C) and the “B” (370–425 °C) peaks emission spectra exhibited somewhat different behavior with increasing dose. Initially, an even growth of the whole spectrum was observed and for doses higher than 16 kGy the intensity of the spectrum decreased, but the short wavelength emission band fell significantly faster, in case of the high-temperature TL peaks. In case of the “B” peak emission spectra the long wavelength emission did not play any role in the analyzed dose range. The spectra measured at the TL peaks maxima were also fitted with several Gaussian-shape bands. Dose-intensity dependences for all Gaussian-shape bands fitted to the measured spectra are also included in this paper.     

Kinetic modeling of thermoluminescence,optical absorption and bleaching in LiF:Mg,Ti

In this paper we describe some aspects of our recent work which treats via kinetic simulations the experimentally observed linear/supralinear/saturating dose response of the thermoluminescence, optical absorption and behavior of optical bleaching at various photon energies in irradiated LiF:Mg,Ti (TLD-100) system in a physically realistic scenario. The results of the simulations are in good agreement with the experimental observations and this can be considered as a validation of the details of the proposed models.     

Optical and dosimetric properties of variously doped SrF2 crystals

Optical properties and irradiation effects of Nd³⁺-, Pr³⁺-, Tb³⁺- and Tm³⁺-doped SrF₂ crystals and their possible application to solid-state dosimetry were studied and compared to those induced in pure SrF₂ crystals. Optical absorption, thermoluminescence (TL), X- and light-induced luminescence (XL and PL) as well as optically stimulated luminescence and phototransferred TL (OSL and PTTL) were measured in the various samples. Special attention was given to effects of monochromatic vacuum ultraviolet (VUV) radiation. TL was excited in the pure and doped samples by X and β rays as well as by VUV radiation. TL peaks appeared after VUV irradiation at the same temperatures and with the same thermal activation energies as after X or β irradiation, indicating that they are due to the same processes. The VUV excitation spectra showed two maxima at about 145 and 130 nm. Comparison of the TL sensitivities of the various TL materials, showed that the sensitivity of SrF₂:Pr³⁺ was by more than an order of magnitude higher than that of the known LiF:Mg,Ti (TLD-100) phosphor. The sensitivity of pure and of the Nd, and Tb-doped SrF₂ were by a factor of 2–4 higher than that of the TLD-100 and that of SrF₂:Tm was slightly lower. The main emission bands of SrF₂:Pr³⁺ are located in a convenient spectral region between 460 and 640 nm, where most of the standard photomultipliers are sensitive. The dose dependence of the 460 K TL peak in SrF₂:Pr³⁺ is nearly linear in a wide range up to above 27 000 Gy.     

微波法合成红色长余辉发光材料Gd2O2S:Eu,Mg,Ti及其发光特性

用微波辐射法首次合成了Gd2O2S:Eu,Mg,Ti红色磷光化合物,用X射线粉末衍射(XRD)、扫描电镜(SEM)、荧光分光光度计等对合成产物进行了分析和表征.结果表明:材料的晶体结构为六方晶系,与Gd2O2S的相同.颗粒的形貌为类球形,分散性较好,尺寸在1～2 μm之间.Gd2O2S:Eu,Mg,Ti的激发光谱呈带状,激发光谱主峰位于360 nm,另外在400,422,472 nm等处也有激发峰存在;发射光谱为线状光谱,归属于Eu3 的5DJ(J=0,1,2)到7FJ(J=O,1,2,3,4)的跃迁.随着Eu浓度的增加,位于蓝绿区的586,557,541,513,498,471,468 nm处的发射峰逐渐减弱,而主峰位于627 nm处的红光发射明显增强.当Eu浓度为6 mol%时,红光发射最强.Mg,Ti共掺杂可显著改善其余辉性质.     

Kinetic simulation of charge transfer following 5.08 eV (F band) optical excitation of irradiated LiF:Mg,Ti (TLD-100): Participation of holes released via V3-VK transformation

Kinetic simulations of charge transfer in the framework of the conduction band/valence band model are described which investigate the effect of 5.08 eV photon bleaching on the optical absorption spectrum of irradiated LiF:Mg,Ti (TLD-100). The decrease in intensity of the 3.8 eV and 4.3 eV bands, newly discovered sub-entities of the 4.0 eV composite band, is interpreted as arising from the participation of holes released by capture of electrons at V₃ two-hole-centers. The simulations also require highly efficient electron transfer from the excited state of the F center to the V₃ center which is necessary to guarantee an adequate supply of released holes following the V₃-V_k transformation.     

Investigation of the optical absorption characteristics of slow-cooled LiF:Mg,Ti (TLD-100)

The optical absorption (OA) spectrum of LiF:Mg,Ti has been studied as a function of dose at two different cooling rates following the 400 °C pre-irradiation anneal in order to further investigate the role of cooling rate in the thermoluminescence (TL) mechanisms of this material. “Slow-cooling” following the pre-irradiation 400 °C anneal substantially decreases the OA bands at 3.25 eV and 4.0 eV, in agreement with the overall loss in TL peaks 2–5 intensity using slow-cooling routines. Slow-cooling appears to shift the maximum intensity of peak 5 to lower temperatures (a behaviour which has been attributed to an enhanced intensity of peak 5a), however, no difference in the shape of the 4.0 eV OA band is detected following “slow-cooling”. Apparently the OA band related to peak 5a is too close in energy to the peak 5 OA band to be observed due to lack of sufficient resolution and spectral deconvolution process or it is not present at room temperature (RT) and formed during heating of the sample. The intensity of the 4.0 eV OA band does not change if the sample (prior to irradiation to a standard dose of 200 Gy) is irradiated to 4 kGy followed by a 500 °C/1 h post-irradiation anneal. This result demonstrates that the loss of intensity at high levels of dose (so-called radiation damage) of TL glow peak 5 results from alteration of the LCs or to the creation of additional competitive centers and is not correlated with the dose behaviour of the TCs.     

Eu3+摩尔浓度对Y2O2S:Eu3+,Mg2+,Ti4+红色长余辉材料光谱的影响

用高温固相法制备了Y2O2S：Eu^3 ,Mg^2 ,Ti^4 红色长余辉材料。测量了该材料的余辉曲线,余辉时间为1h以上;由X射线衍射得到晶体结构为Y2O2S.测量了不同Eu^3 摩尔浓度下的激发光谱和发射光谱,得到从^5DJ(J=0,1,2,3)^-7FJ(J=0,1,2,3,4,5)的发射谱线,并得到位于260,345,468和540nm激发峰。由于激活剂饱和效应,Y2O2S：Eu^3 ,Mg^2 ,Ti^4 发射光谱中513．6,540．1,556．4,587．3和589．3nm属于从^5D2,^5D1到^7FJ(J=0,1,2,3,4)跃迁的发射峰随Eu^3 摩尔浓度的增加相对削弱;激发谱包括位于350nm左右属于电荷转移态吸收(Eu^3 -O^2-,Eu^3 -S^2 )的激发主峰和在可见光区位于468,520和540nm属于Eu^3 离子4f-4厂吸收的激发峰。随着Eu^3 摩尔浓度的增加,位于468,520和540nm的激发峰相对增强。     

Dose response of F center optical absorption in LiF:Mg,Ti (TLD-100)

Optical absorption (OA) of nominally pure single crystal LiF following beta irradiation was measured in order to estimate, the energy and width of the dominant F-band with minimum interference from dopant-related bands. The OA dose response of LiF:Mg,Ti was measured to 30,000 Gy, a level of dose sufficiently high to observe total saturation of the F band, which, we believe, reduces uncertainty in the estimation of the dose filling constant. The dose filling constants for the OA bands associated with the trapping center (4 eV) and competitive center (5.45 eV) responsible for the major dosimetric TL glow peak 5 were also determined. The results of these studies will be used in the framework of a kinetic model which includes the effects of radiation created defects and which will aid in the investigation of the capability of Track Structure Theory to predict OA heavy charged particle (HCP) relative efficiencies.     

Thermoluminescence of nanocrystalline LiF:Mg, Cu, P

Nanocrystalline LiF:Mg, Cu, P of rod shape (about 30-40 nm in diameter and 0.3-0.5 μm in length) has been prepared by the chemical co-precipitation method. Thermoluminescence (TL) and dosimetric characteristics of the nanocrystalline phosphor are studied and presented here. The formation of the material was confirmed by the X-ray diffraction (XRD). Its shape and size were also observed by transmission electron microscope (TEM). The TL glow curve of the nanocrystalline powder shows a single peak at 410 K along with four overlapping peaks of lesser intensities at around 570, 609, 638 and 663 K. The observed TL sensitivity of the prepared nanocrystalline powder is less than that of the commercially available “Harshaw TLD-700H hot-pressed chips” at low doses but it still around three times more than that of LiF:Mg, Ti (TLD-100) phosphor. The 410 K peak of the nanomaterial phosphor shows a very linear response with exposures increasing up to very high values (as high as 10 kGy), where all the other thermoluminesent dosimeters (TLD) phosphors show saturation. This linear response over a large span of exposures (0.1 Gy-10 kGy) along with negligible fading and its insensitivity to heating treatments makes the nanocrystalline phosphor useful for its application to estimate high exposures of γ-rays. The ‘tissue equivalence’ property of this material also makes it useful over a wide range of high-energy radiation.     

Newly developed highly sensitive LiF:Mg,Cu,Si TL discs with good stability to heat treatment

The preparation method and some dosimetric properties of the new LiF:Mg,Cu,Si discs are presented. The effect of heat treatments on LiF:Mg,Cu,Si was investigated. The shape of the glow curve for LiF:Mg,Cu,Si is similar to that for standard LiF:Mg,Cu,P (GR-200A), and shows minimal differences when annealed in the range from 260 °C to 290 °C for 10 min. The TL sensitivity for LiF:Mg,Cu,Si is much lower than that for GR-200A, but is 35 times larger than that for TLD-100 and is slightly higher than that for HMCP. The height of the high-temperature peaks for LiF:Mg,Cu,Si is not only lower than that for GR-200A, but also lower than that for HMCP. The glow curve shape of LiF:Mg,Cu,Si annealed at 260 °C for different times shows minimal differences and TL response remains stable. These results indicate that the new LiF:Mg,Cu,Si disc has a good stability to thermal treatments and a lower residual TL signal.     

Radio-photoluminescence of highly irradiated Lif:Mg,Ti and Lif:Mg,Cu,P detectors

The radio-photoluminescent (RPL) characteristics of LiF:Mg,Ti (MTS) and LiF:Mg,Cu,P (MCP) thermoluminescent detectors, routinely used in radiation protection dosimetry, were investigated after irradiation with ultra-high electron doses ranging up to 1 MGy. The photoluminescence of both types of LiF detectors was stimulated by a blue light (460 nm) and measured within a spectral window around 530 nm. The RPL dose response was found to be linear up to 50 kGy and sublinear in the range of 50 kGy to 1 MGy for MCP detectors and linear up to 3 kGy and next sublinear in the range from 5 kGy to 1 MGy for MTS detectors. For both type of LiF detectors RPL signal is saturated for doses higher than 100 kGy. The observed differences between MCP and MTS may suggest, that the RPL effect in LiF is not entirely governed by intrinsic defects (F₂ and F₃⁺ centers), but dopants may also have a significant influence. Due to the non-destructive character of the RPL measurement, it is suggested to apply combined RPL/TL readouts, what should improve accuracy of high-dose dosimetry.     

OSL and TL in TLD-100 following alpha and beta irradiation: Application to mixed-field radiation dosimetry

The optically stimulated luminescence (OSL) of LiF:Mg,Ti (TLD-100) following irradiation by beta and alpha particles was investigated by measurement of the excitation and emission spectra of OSL and comparison with thermoluminescence (TL) characteristics. The OSL excitation spectra of all the samples following both beta and alpha irradiation are very similar.Identical emission bands with very similar relative intensities following both beta irradiation and alpha particle irradiation have been recorded in the OSL induced in nominally pure LiF mono and TLD-100 polycrystals. The identical excitation and emission bands in the doped and pure crystals are strong evidence indicating that the observed OSL is due to an intrinsic trapping structure. The OSL has indeed been previously attributed to F₂ centers and F₃⁺ centers.The preferential excitation of OSL compared to TL following high ionisation density (HID) alpha irradiation is naturally explained via the identification of OSL with the “two-hit” F₂ or F₃⁺ center, whereas the major component of composite TL glow peak 5 is believed to arise from a “one-hit” complex defect. This discovery allows near-total discrimination between HID radiation and low ionisation density (LID) radiation and may have significant potential in mixed-field radiation dosimetry.     

Influence of sintering temperatures on LiF:Mg,Cu,P with various magnesium concentrations

The dependence of LiF:Mg,Cu,P samples with various concentrations of Mg on sintering temperatures was investigated to find a new dosimeter. The influence of high sintering temperatures on LiF:Mg,Cu,P chips depends strongly on Mg concentrations. The height of the main peak versus the sintering temperatures exhibits a maximum, the position of which varies between 690 °C and 750 °C, depending on the Mg concentration in the range studied. The high temperature peaks of LiF:Mg,Cu,P for various Mg concentrations reduce basically when the sintering temperature is increased. LiF:Mg,Cu,P is much less sensitive than LiF:Mg,Cu,Si to sintering temperature. LiF:Mg,Cu,P with 0.6 mol% of Mg can be re-used at annealing temperature of 260 °C, regardless of the sintering temperature. It was found that the optimum concentration is Mg: 0.6 mol%, the optimum sintering temperature is 750 °C, considering that LiF:Mg,Cu,P with a low residual signal and good sensitivity can be re-used at annealing temperature of 260 °C and produced in a large scale. The new optimum LiF:Mg,Cu,P formation has 52 times higher than that of the TLD-100, and an extremely low residual signal of 0.07% without an initialization readout procedure.     

Radioluminescence (RL) behaviour of Al2O3:C-potential for dosimetric applications

The radioluminescence (RL) of carbon doped aluminium oxide (Al₂O₃:C) TL dosimeter material (TLD-500) was investigated using a ¹³⁷Cs conversion electron source (which also emits β and γ) for simultaneous irradiation and luminescence excitation. Furthermore, RL dosimetry characteristics of this material were studied. The main RL emission occurs at 420 nm. That matches the known main TL and OSL emissions for this material as well as an emission that was investigated in earlier RL studies, excited at higher energies (4 MeV electrons) and very high pulse delivered doses (≈800 kGy·s⁻¹). Furthermore, the saturation dose for the main peak is reached at the dose level of ≈80 Gy as known from TL and earlier RL investigations. Other peaks at 700 and 790 nm and broad emission bands at photon energies higher than 3.00 eV and others between 2.00 and 2.50 eV were observed. The 700 nm emission shows growth also at higher dose levels, and saturates at an estimated dose of ≈800 Gy. The 790 nm emission reaches its maximum intensity at ≈10 Gy absorbed dose. The reported results give an outlook to the usability and the potential of Al₂O₃:C combined with RL measurements for radiation dosimetry as well as for beta source calibration, using radioluminescence.     

Effects of type of radiation on glow curve and thermoluminescence emission spectrum of CaF2:Tm

Thermoluminescence emission spectra of CaF₂:Tm (TLD-300) samples irradiated with 48 keV X-rays ⁶⁰Co gamma rays, 4.5 MeV alpha particles and 15 MeV neutrons were measured in the 300–650 K temperature region. Seven emission bands were observed of which the one in the infrared (at 803 nm) is very intense. The emission bands can be assigned to ¹D, ¹G, ³F and ³H levels characteristic for Tm³⁺ de-excitation in a cubic field. All observed lines in the spectrum are due to 4f-4f transitions. The spectra undergo remarkable changes in intensity when the temperature is raised from room temperature up to 350°C, while the number of the emission bands remains constant. The glow curve structure is both dependent on emission wavelength and the type of radiation. Evidence has been found that the trapping structures responsible for glow peaks 2 and 3 alter under the influence of high LET () radiation. For glow peaks 4–6 the filling of the traps alters with the type of radiation. The observations can be explained assuming a TL process involving several hole trapping centres but with only one luminescent centre (Tm³⁺) active at all temperatures.     

Nanodosimetric kinetic model incorporating localized and delocalized recombination: Application to the prediction of the electron dose response of the peak 5a/5 ratio in the glow curve of LiF:Mg,Ti (TLD-100)

A kinetic model combining both localized and delocalized recombination is described which is based on different filling rates as a function of irradiation electron energy of a spatially correlated trapping center/luminescent center (TC/LC) complex. Following irradiation and thermal de-trapping the locally trapped electron-hole configuration is assumed to give rise to peak 5a and the e-only configuration to peak 5 in the glow curve of LiF:Mg,Ti (TLD-100). The model is capable of simulating the linear/supralinear dose response of composite peak 5, the dependence of the supralinearity on photon energy and the ratio of the intensities of peak 5a to peak 5 as a function of dose. However, this is achieved only by invoking the presence of band-tail states which allow thermally induced hopping leading to semi-localized recombination in the recombination mechanism of the e-only configuration.     

Behaviour of LiF:Mg,Cu,P and LiF:Mg,Ti thermoluminescent detectors for electron doses up to 1 MGy

The behaviour of LiF:Mg,Cu,P and LiF:Mg,Ti detectors at ultra-high doses up to 1 MGy, has been investigated. The presence of the ultra-high-temperature peak (450 °C) of reproducible properties was observed in various batches of LiF:Mg,Cu,P, confirming earlier findings. The results indicate that this peak is not an effect of random impurities nor intrinsic effects of LiF, but it is rather connected with the doping.A parameter called ultra-high temperature ratio (UHTR) was defined in order to quantify the observed changes of LiF:Mg,Cu,P glow-curve shape at very high doses and very high temperatures. The use of this parameter allows to determine an absorbed dose in the range from 1 kGy to 1 MGy. This new method of high-dose dosimetry makes LiF:Mg,Cu,P a unique dosimeter, which is capable to cover at least 12 orders of magnitude of dose range: from a microgray to a megagray.