Optical properties of some fluoride compounds and their application to dosimetry

Effects of β, X and VUV irradiation on the optical properties have been studied in various simple and complex fluoride crystals by using optical absorption, X- and UV-excited luminescence (XL and PL), thermoluminescence (TL) and photo-transferred TL (PTTL) techniques. In most tested crystals, the main TL peaks with the same thermal activation energies appear after VUV as well as after X or β irradiation, thus indicating that the same traps are induced by the different types of radiation. The TL excitation spectra generally show absorption maxima on the long wavelengths tail of the fundamental absorption. Within this study, various dosimetric properties, as well as the possible application of the crystals as sensitive radiation detectors and dosimeters for the VUV have also been investigated. The TL sensitivities of the various studied materials have been compared to that of the classic dosimeter TLD-100 (LiF:Mg,Ti). For example, the sensitivity of SrF₂:Pr³⁺ has been found to be the highest among the examined crystals and at a dose of 90 Gy its response is higher by a factor of ～3 than that of TLD-100. The sensitivity of CsGd₂F₇:Pr³⁺ and KYF₄:Pr³⁺ are slightly higher than that of TLD-100, whereas that of nanostructured CaF₂:ZnO crystals is about twice that of TLD-100, but the sensitivity of LiF:Eu is much lower. The SrF₂:Pr³⁺ crystals also showed some important dosimetric properties.     

Spectroscopy of the gamma and X ray leakage radiation from the built-in sources of a Risø TL/OSL reader

In this work we evaluate the intensity and the spectral shape of the leakage radiation from the built-in beta and alpha sources of a Risø TL/OSL reader. LiF (TLD-100), fluorite-based pellets and Al₂O₃:C detectors were used in order to determine the dose rate delivered to the dosimeters when the sources are closed. The leakage spectra under both alpha and beta sources were registered with a CdTe semiconductor detector. The spectrum measured under the beta source shows the X-ray beam generated by the interaction of the beta particles with the lead used to shield the source. Besides, the 59.4 keV gamma ray from ²⁴¹Am was registered under the alpha source. Dose rates from 50 to 100 μGy/h were obtained for the dosimeter positions in the turntable under the beta and the alpha sources with the luminescent dosimeters.     

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.     

Color center production by femtosecond-pulse laser irradiation in fluoride crystals

Color centers are lattice vacancy defects trapping electrons or holes. They are easily created in single crystals by irradiation with ionizing radiation. We report the production of color centers in LiF and LiYF₄ single crystals by ultrashort high-intensity laser pulses (60 fs, 12.5 GW). An intensity threshold for color center creation of 1.9 and 2 TW/cm² was determined in YLF and LiF, respectively, which is slightly smaller than the continuum generation threshold. Due to the high energy density of the coherent radiation of the focused laser beam, we were able to identify a large amount of F centers, which gave rise to aggregates such as F₂, F ₂ ⁺ , and F ₃ ⁺ . The proposed mechanism of formation is based on multiphoton excitation, which also produces short-lived F ₂ ⁺ centers. It is also shown that it is possible to write tracks in the LiF crystals with dimensional control.     

Thermoluminescence and photoluminescence characteristics of K2YF5: Tb3++PTFE irradiated with 90Sr/90Y beta particles

This article presents results of thermoluminescence (TL) and photoluminescence (PL) measurements performed on beta-irradiated K ₂YF ₅:Tb ³⁺+PTFE pellets. K ₂YF ₅ crystals doped with 0.1% of trivalent optically active Tb ³⁺ ions in pellets form were investigated. The TL glow curve of K ₂YF ₅:Tb ³⁺+PTFE has a simple structure with two well-defined peaks centered at 170 and 307 °C. The TL sensitivity of the K ₂YF ₅:Tb ³⁺+PTFE irradiated with beta radiation was found to be higher than that of commercial phosphor TLD-100 (LiF:Mg,Ti), at the same conditions of irradiation and readout. Moreover, PL measurements performed on the terbium doped material show the presence of Terbium as Tb ³⁺ in the material.     

Radioluminescence of ionized electron color centers in LiF crystals

Photoluminescence (PL) and temporal variation of optical absorption and radioluminescence (RL) of LiF crystals after irradiation with an electron impulse are investigated by pulse spectrometry methods using different irradiation regimes and different degrees of initial radiation damage. The difference in the RL and PL characteristics of ionized F ₂ ⁺ and F ₃ ⁺ centers is revealed. Several mechanisms for inducing these centers by irradiation, which differ in energy and kinetic parameters and in temperature dependence, are proposed. It is established that the ionized centers in the radiation active state are created due to the interaction of the respective neutral centers with holes of different thermalization extent. A mechanism for the excitation of these radiation-active centers is proposed.     

Dose response of thermoluminescence emission spectra of LiF:Mg,Ti with different Mg, Ti impurity concentrations

The dose response of the TL emission spectra of an LiF:Mg,Ti (TLD-100) sample and three LiF:Mg,Ti samples with different impurity concentrations (0–6 ppm Ti and 80–100 ppm Mg) have been measured. At a dose less than 22 Gy the emission spectrum of the TLD-100 sample comprises one emission band at 420 nm. The sample without Ti shows also one emission band but now at 620 nm. The spectra of the other two samples comprises two emission bands at 420 nm and 620 nm of which the intensity of the 420 nm band increases with increasing Ti concentration. The dose response of the glow peaks is different for peaks at different temperatures and emission bands. From these observations it can be concluded than in LiF:Mg,Ti at least some of the traps and luminescent centers are coupled.     

Nanostructured layers of anion-defective gamma–alumina – New perspective TL and OSL materials for skin dosimetry. Preliminary results

Thin- layer material based on nanostructured Al₂O₃ of the surface density 5 mg/cm² was obtained. The material is characterized by high OSL and TL yields comparable with those for TLD-500 which is one of the leaders among the TL and OSL detectors. The dose response, fading and dependence of TL yield on heating rate was studied. It is established that high luminescence yield of the samples under study correlates with the content of anion vacancies and γ-phase of Al₂O₃. The data for time-resolved luminescent spectroscopy are presented, which evidence for possible correlation between high TL and OSL activity and the F-type centers. It is noted that the material needs to be modified for successful use in dosimetry. In addition further studies to decrease the contribution of unstable (at 300 К) components to OSL and TL yields are required.     

Thermoluminescence of corundum containing anion defects following ultraviolet laser and x irradiation

The thermoluminescence of single crystals of corundum containing anion defects following x-ray and laser excitation is investigated. Its features in the luminescence bands of F, F⁺, and Cr³⁺ centers are studied. Synchronous measurements of the thermoluminescence and thermally stimulated exoelectron emission are performed by the fractional glow technique following x-ray and laser excitation of the samples. It follows from the results obtained that several traps are active in the temperature range of the principal dosimetric peak (400–500 K). The spectral sensitivity curve contains maxima corresponding to absorption bands of F, F⁺, and Al _i ⁺ centers. A possible mechanism for the recombination luminescence of F centers is discussed. It is found that the material exhibits high sensitivity to small doses of ultraviolet laser radiation. Zh. Tekh. Fiz. 67, 72–76 (July 1997)     

Comparative investigations of TL and OSL in KCI:Eu2+ crystals irradiated with UV and X-rays

Abstract

We present thermoluminescence (TL) glow curves and optical stimulated luminescence (OSL) response from both KCl:Eu²⁺ crystals irradiated with soft X-rays (20 KV, 80 μA) and ultraviolet light (230 nm). Two situations take place. First, we observed that for long time F-light bleaching (560 nm) the typical TL glow curve of X-rays irradiated KCl:Eu²⁺ resembles the TL glow curve of UV-irradiated samples. Second, along with OSL measurements, we have performed a thermal bleaching and we have addressed F and F_z participation in OSL. These results provide us a supportable correlation between F and F_z as responsible centers for OSL and TL processes.     

Photon dosimetry methods outside the target volume in radiation therapy: Optically stimulated luminescence (OSL), thermoluminescence (TL) and radiophotoluminescence (RPL) dosimetry

Dosimetry methods outside the target volume are still not well established in radiotherapy. Luminescence detectors due to their small dimensions, very good sensitivity, well known dose and energy response are considered as an interesting approach in verification of doses outside the treated region. The physical processes of thermoluminescence (TL), radiophotoluminescence (RPL) and optically stimulated luminescence (OSL) are very similar and can be described in terms of the energy band model of electron-hole production following irradiation.This work is a review of the main dosimetric characteristics of luminescence detectors which were used in experiments performed by EURADOS Working Group 9 for in-phantom measurements of secondary radiation (scattered and leakage photons). TL LiF:Mg,Ti detectors type MTS-7 (IFJ PAN, Poland), types TLD-100 and TLD-700 (Harshaw), OSL Al₂O₃:C detectors type nanoDot™ (Landauer Inc.) and RPL rod glass elements type GD-352M (Asahi Techno Glass Coorporation) are described. The main characteristics are discussed, together with the readout and calibration procedures which lead to a determination of absorbed dose to water.All dosimeter types used show very good uniformity, batch reproducibility and homogeneity. For improved accuracy, individual sensitivity correction factors should be applied for TL and OSL dosimeters while for RPL dosimeters there is no need for individual sensitivity corrections.The dose response of all dosimeters is linear for a wide range of doses.The energy response of GD-352M type dosimeters (with Sn filter) used for out-of-field measurements is flat for medium and low energy X-rays.The energy dependence for TLDs is low across the range of photon energies used and the energy correction was neglected. A significant over response of Al₂O₃:C OSLDs irradiated in kilovoltage photon beams was taken into account. The energy correction factor f_en was calculated by using the 2006 PENELOPE Monte Carlo code.With suitable calibration, all dosimeter types are appropriate for out-of-field dose measurements as well as for the in-phantom measurements of radiotherapy MV X-rays beams.     

Control of radiation spatial coherence under synchronous amplification in crystalline LiF:F 2 − amplifier

A technique of spatial coherence control, based on the synchronous amplification of a radiation in LiF crystals with F ₂ ^? color centers, is demonstrated. Spatial radiation distributions of stimulated Raman scattering (SRS) in oxide crystals were investigated under picosecond laser excitation. Low spatial radiation coherence was revealed for both the transient and quasi-stationary SRS. Spatially incoherent SRS was transformed to spatially coherent radiation as a result of phase—locked picosecond synchronous laser pumping of nonlinear Raman and LiF: F ₂ ^? crystals and the Stokes radiation amplification in the color center crystal.     

Features of OSL and TL properties of anion-defective corundum crystals exposed to thermo-optical treatment

The results of systematic investigation of the mechanisms and role of phototransfer in TL and OSL processes in α-Al₂O_3−δ crystals under controlled filling of the main and deep traps depleted at 450 and 720 K, respectively, are presented.Optical depletion spectra of the main and deep traps were measured and compared. It was found that green light stimulation only depletes the main trap, while blue light depletes both the main and deep traps. Optical depletion of the deep trap results in phototransfer of charges that can be realized by 2 mechanisms: either through the main trap to recombination centers or directly to the latter. However, the dominant contribution to the OSL signal is provided by phototransfer through the main trap. It is also found that UV emission at 3.7 eV dominates over F-emission at 3.0 eV in the phototransferred TL spectrum. It is assumed that this UV emission is not related to the F⁺ centers.     

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.     

Conversion of ultraviolet and infrared to visible light in Er3+ and Dy3+ co-doped CsGd2F7

The CsGd₂F₇ crystal co-doped with 1 at% Er³⁺ and 0.2 at% Dy³⁺ ions was studied using the excitation of both synchrotron radiation and 355 nm laser. All the emission bands were assigned by using the Dieke diagram together with the conclusions from relaxation kinetics studies. The onset of the 4f–5d transition bands and the centers of charge transfer bands were also calculated for the lanthanide series CsLn₂F₇ and the results were used to assign the bands and peaks in the excitation spectra. The energy transfer and relaxation processes in CsGd₂F₇ were thoroughly analyzed. Quantum cutting downconversion of one vacuum ultraviolet to two visible photons was realized under 154 nm excitation. Upconverted green emission was observed under 980 nm excitation.     

Dosimetric properties of rare earth doped LiCaBO3 thermoluminescence phosphors

Lithium Calcium borate (LiCaBO₃) polycrystalline thermoluminescence (TL) phosphor doped with rare earth (RE³⁺) elements has been synthesized by high temperature solid state diffusion reaction. The reaction has produced a very stable crystalline LiCaBO₃:RE³⁺ phosphors. Among these RE³⁺ doped phosphors thulium doped material showed maximum TL sensitivity with favorable glow curve shape. TL glow curve of gamma irradiated LiCaBO₃:Tm³⁺ samples had shown two major well-separated glow peaks at 230 and 430 °C. The glow peak at 430 °C is almost thrice the intensity of the glow peak at 230 °C. The TL sensitivity of the phosphor to gamma radiation was about eight times that of TLD-100 (LiF). Photoluminescence and TL emission spectra showed the characteristic Tm³⁺ peaks. TL response to gamma radiation dose was linear up to 10³ Gy. Post-irradiation TL fading on storage in room temperature and elevated temperatures was studied in LiCaBO₃:Tm³⁺ phosphor.     

Photoluminescence properties of SHI induced F2 and F3 color centers in nano-granular LiF thin films

Photoluminescence (PL) properties of swift heavy ions-induced F₂ and F₃⁺ color centers in nano-granular lithium fluoride (LiF) thin film were studied. LiF films were deposited on glass and silica substrates and irradiated with various ion species (Ag, Ni and Au) at different irradiation temperatures. The role of ion species, their fluence and the irradiation temperature on the PL intensity of color centers induced in LiF thin films is discussed.     

Thermoluminescence and opitical absorption of BaF2 crystals

Abstract

Nominally pure and Dy-doped BaF₂ crystals were investigated concerning their optical absorption (OA) and thermoluminescence (TL) properties. Peaks at 120—150 and 200°C were observed for a heating rate of 1.7°C/s. The TL response for γ-rays and the TL emission spectra were obtained for these peaks. Except for the purest crystal, all BaF₂ crystals produced OA bands before irradiation typical of Ce³⁺ ions. After irradiation, Dy doped crystals showed bands due to Dy²⁺ ions. A nominally pure sample gave bands related to Ce²⁺ ions and photochromic centers of Ce³⁺ ions. and photochromic centres of Ce³⁺ ions. The correlation between some OA bands and TL peaks is discussed.     

The response of thermally and optically stimulated luminescence from Al2O3:C to high-energy heavy charged particles

The thermoluminescence (TL) and optically stimulated luminescence (OSL) response of Al₂O₃ dosimeters to high-energy heavy charged particles (HCP) has been studied using the heavy ion medical accelarator at Chiba, Japan. The samples were Al₂O₃ single-crystal chips, of the type usually known as TLD-500, and Luxel^TM dosimeters (Al₂O₃:C powder in plastic) from Landauer Inc. The samples were exposed to ⁴He (150 MeV/u), ¹²C (400 MeV/u), ²⁸Si (490 MeV/u) and ⁵⁶Fe (500 MeV/u) ions, with linear energy transfer values covering the range from 2.26 to 189 keV/μm in water and doses from 1 to 100 mGy (to water). A ⁹⁰Sr/⁹⁰Y beta source, calibrated against a ⁶⁰Co secondary standard, was used for calibration purposes. For OSL, we used both continuous-wave OSL measurements (CW-OSL, using green light stimulation at 525 nm) and pulsed OSL measurements (POSL, using 532 nm stimulation from a Nd:YAG Q-switched laser). The efficiencies (η_HCP,γ) of the different HCPs at producing OSL or TL were observed to depend not only upon the linear energy transfer (LET) of the HCP, but also upon the sample type (single crystal chip or Luxel^TM) and the luminescence method used to define the signal—i.e. TL, CW-OSL initial intensity, CW-OSL total area, or POSL. Observed changes in shape of the decay curve lead to potential methods for extracting LET information of unknown radiation fields. A discussion of the results is given, including the potential use of OSL from Al₂O₃ in the areas of space radiation dosimetry and radiation oncology.     

Synthesis, photoluminescence, thermoluminescence and dosimetry properties of novel phosphor Zn(BO2)2:Tb

Polycrystalline powder samples of terbium doped Zn(BO₂)₂ phosphors were prepared by solid state reaction in the thermal carbon reducing atmosphere at high temperature. The photoluminescence (PL), three-dimensional (3D) TL emission spectrum and dosimetric characteristics following ⁶⁰Co gamma-rays irradiation were studied. Characteristic emission bands of Tb³⁺ at about 490, 543, 584 and 620 nm, attributed to the ⁵D₄→⁷F_J (J=3, 4, 5, 6) transitions of Tb³⁺ ions, were observed in the TL and PL emission spectrum. No emission from Tb⁴⁺ ions was observed in the TL emission spectrum. The TL-dose response of the powder samples Zn(BO₂)₂:Tb to ⁶⁰Co gamma-rays radiation in the dose range from 1 to 100 Gy for clinical dose levels was almost linear. The experiment results showed that Zn(BO₂)₂:Tb has potential use as the materials of gamma-rays thermoluminescence dosimeter (TLD) for clinical dosimetry.