Scintillation timing characteristics of (La,Gd)2Si2O7:Ce and Gd2SiO5:Ce single crystal scintillators: A comparative study

The scintillation timing characteristics of (La,Gd)₂Si₂O₇:Ce (GPSLa23.5%:Ce) single crystal were studied and compared with Gd₂SiO₅:Ce (GSO:Ce) single crystal. The photoelectron yield, scintillation decay times and coincidence time resolution were measured. At 511 keV γ-rays, the photoelectron yield of 10,770 ± 500 phe MeV⁻¹ and energy resolution of 5.4 ± 0.2% obtained for GPSLa23.5%:Ce are much better than those of 3350 ± 160 phe MeV⁻¹ and 7.8 ± 0.3% obtained for GSO:Ce. The scintillation decay time profile was measured by the time-correlated single photon counting technique using a fast-slow coincidence setup. In both materials the comparable rise times of several nanoseconds are present. The fast component decay time of 56 ns with relative intensity of 49% obtained for GPSLa23.5%:Ce is inferior to that of 32 ns(88%) obtained for GSO:Ce. Consequently, the coincidence time resolution of GPSLa23.5%:Ce is slightly worse than that of GSO:Ce. The normalized time resolution was also discussed in terms of a number of photoelectrons and decay time of the scintillation pulse.     

Luminescence and scintillation properties of advanced Lu3Al5O12:Pr3+ single crystal scintillators

In this paper we present the luminescence and scintillation properties of Lu₃Al₅O₁₂:Pr (LuAG:Pr) single crystals with Pr³⁺ concentration of 0.13 wt %, grown by the Czochralski method. The light yield and energy resolution were measured under 662 keV γ-ray excitation. The dominant emission band peaking at 310 nm with a shoulder at 370 nm was observed in the photoluminescence spectrum. High light yield of 24,500 ph/MeV and an energy resolution of 5.3 % were obtained for a 6 × 6 × 2 mm³ LuAG:Pr sample. Light yield dependence on sample height and shaping time was measured. The estimated photofraction in pulse height spectrum and total mass attenuation coefficient at 662 keV γ-rays were also determined and compared with the theoretical ones calculated using the WinXCom program.     

Timing characteristics of the scintillation response of Gd3Al2Ga3O12:Ce and Gd3Al2.6Ga2.4O12:Ce single crystal scintillators

The timing characteristics of scintillation response of Czochralski-grown Gd₃Al₂Ga₃O₁₂:Ce and Gd₃Al_2.6Ga_2.4O₁₂:Ce single crystals were compared. The photoelectron yield, scintillation decay times, and coincidence time resolution were measured. At 662 keV γ-rays, the photoelectron yield of 6200 phe MeV⁻¹ obtained for Gd₃Al₂Ga₃O₁₂:Ce is higher than that of 4970 phe MeV⁻¹ obtained for Gd₃Al_2.6Ga_2.4O₁₂:Ce, while an inferior energy resolution of the former (7.2% vs. 5.6%) is observed. Scintillation decays are approximated by sum of exponentials with the dominant fast component decay time and its relative intensity of 89 ns (73%) for Gd₃Al₂Ga₃O₁₂:Ce and 136 ns (69%) for Gd₃Al_2.6Ga_2.4O₁₂:Ce. The coincidence time resolution obtained for Gd₃Al₂Ga₃O₁₂:Ce is superior than that of Gd₃Al_2.6Ga_2.4O₁₂:Ce. The normalized time resolution was also discussed in terms of a number of photoelectrons and decay characteristics of the light pulse.     

Scintillation response of Y3Al5O12:Pr3+ single crystal scintillators

In this paper we present the photoluminescence (PL) and scintillation response of Pr³⁺-doped Y₃Al₅O₁₂ (YAG:Pr) single crystals grown by the Czochralski method with different Pr³⁺ concentrations of 0.16, 0.33, and 0.65 mol%. PL spectra and decay curves were measured for both the fast 5d → 4f and slow 4f → 4f emissions. The PL decay times were evaluated which evidence concentration quenching especially in ¹D₂ → ³H₄ emission for the highest Pr³⁺ concentration. Light yield (LY) of 15,600 photons per MeV and energy resolution of 6.4% at 662 keV γ-rays were obtained with the YAG:Pr (0.33%) crystal. The LY non-proportionality and energy resolution versus γ-ray energy were measured and the intrinsic resolution was calculated. A good proportionality of the LY was found within 7% over the energy range from 1274.5 keV down to 32 keV. The estimated photofraction in the pulse height spectra of 320 and 662 keV γ-rays was also determined and compared with the theoretical one calculated using WinXCom program.     

Improvement of the scintillation properties of Gd3Ga3Al2O12:Ce,B single crystals having tailored defect structure

A novel approach is reported to minimize various defect centers in Ce doped Gd₃Ga₃Al₂O₁₂ single crystals to improve the scintillation properties. The crystals of Gd₃Ga₃Al₂O₁₂ codoped with 0.2 at% Ce and B (GGAG:Ce,B) have been grown in air and argon ambient using the Czochralski technique. The scintillation light output of crystals grown in Ar ambient was significantly increased after annealing the crystals in air. The measured light output of 60000 ph/MeV for annealed crystals is the highest value reported among this class of materials. As a consequence, the energy resolution at 662 keV gamma‐rays from a ¹³⁷Cs source was improved from 8% for the crystals grown in air to 6% for crystals grown in Ar and subsequently annealed in air. Further, the thermal quenching energy of photoluminescence (PL) emission was increased to be 470 meV for the annealed crystals. The thermoluminescence (TL) measurements suggest that the crystals grown in Ar ambient and post‐growth annealed in air may have a lesser concentration of trap centers which subsequently lead to the improvement in optical and scintillation properties leading to a superior detector performance. (© 2015 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

Lu2SiO5:Ce and Y2SiO5:Ce single crystals and single crystalline film scintillators: Comparison of the luminescent and scintillation properties

The paper is dedicated to development of scintillators based on the single crystalline films of Ce³⁺ doped Lu₂SiO₅ (LSO:Ce) and Y₂SiO₅ (YSO:Ce) orthosilicates grown by Liquid Phase Epitaxy method onto YSO substrates from melt-solutions based on the PbO–B₂O₃ flux. We also compare the luminescent and scintillation properties of Ce doped LSO:Ce and YSO:Ce single crystalline films with those of their single crystal counterparts, grown by the Czochralski method.     

X-ray excited luminescence of Ce:Li2CaSiO4, Ce:CaBPO5 and Ce:LiCaPO4

Three materials Ce:Li₂CaSiO₄, Ce:CaBPO₅ and Ce:LiCaPO₄ were synthesized as polycrystalline samples for scintillation application in neutron detection. Ce³⁺ optical spectroscopy was investigated. Then, under X-rays excitation, Ce:Li₂CaSiO₄ and Ce:LiCaPO₄ present light yields about 7800 ph/MeV and 5900 ph/MeV, respectively. A self trapped exciton loss mechanism has been evidenced and competes with the cerium emission.     

Luminescence and Scintillation Characterization of Cs2NaGdBr6: Ce3+ Single Crystal

Luminescence and scintillation properties of newly discovered bromo-elpasolites Cs₂NaGdBr₆: Ce³⁺ (CNGB: Ce³⁺) are presented. Single crystals of CNGB: Ce³⁺ with dimensions up to Ø7×10 mm³ are successfully grown by the Bridgman technique. X-ray excited luminescence measurements of the grown samples showed a broad emission band in the wavelength range from 365 to 470 nm. It offered an energy resolution of 5.1% (FWHM) at 662 keV for 10% Ce sample. The light output of the investigated samples increases along with cerium concentration. A maximum light yield of ～36,800 ph/MeV is measured for the 10% Ce sample crystal. Under γ-ray excitation, CNGB: Ce³⁺ crystals showed three exponential decay time components. The scintillation mechanism in the sample crystal is presented.     

Gadolinium pyrosilicate single crystals for gamma ray and thermal neutron monitoring

Bulk Gd₂Si₂O₇:Ce (GPS:Ce) single crystals obtained by Czochralski method demonstrate a high light output at γ-irradiation (3.8 times higher in comparison with Bi₄Ge₃O₁₂ (BGO)), energy resolution 13% (137Cs, 662 KeV), fast decay time (41.7 ns), and good thermal stability of light output (up to 425 K). This combination of characteristics makes this scintillator very attractive for medical imaging and high-temperature applications. Light output at thermal neutron monitoring is evaluated as twice higher in comparison with Gd₂SiO₅:Ce (GSO). The observed rather high afterglow level (0.2% after 20 ms) and moderate energy resolution (13%) certifies a room for improvement of these parameters by further optimization of crystal quality.     

The nature of activation centers in Y2SiO5:Pr3+, Gd2SiO5:Pr3+, and Lu2SiO5:Pr3+ crystals

A complex study of the energy spectra and relaxation channels for the excitation energy of activation centers in Y₂SiO₅:Pr³⁺, Lu₂SiO₅:Pr³⁺, and Gd₂SiO₅:Pr³⁺ was performed. An analysis of the low-temperature optical spectra showed that the energy parameters and the character of field splitting of the ¹ D ₂ and ³ H ₄ activator ion terms were substantially different in crystals of different crystallographic types. The pseudosymmetry effect was observed in splitting of the ¹ D ₂ and ³ H ₄ terms of Pr³⁺ ions situated in nonequivalent crystal lattice cation sites of Y₂SiO₅ and Lu₂SiO₅. Activator ions nonuniformly populated nonequivalent cation sites of the Y₂SiO₅ crystal lattice. At high activator ion concentrations (>1 at %), luminescence decay in Y₂SiO₅ could not be described by a simple exponential time dependence. The complex luminescence decay law was caused by activator ion excitation energy migration and capture by acceptors. The role of energy acceptors was played by activator ion dimers.     

Comparison of Lu3Al5O12:Pr and Bi4Ge3O12 scintillators for gamma-ray detection

The scintillation properties of Lu₃Al₅O₁₂:Pr³⁺ (LuAG:Pr) single crystal grown by the Czochralski method with praseodymium concentration of 0.19 mol% were investigated. For a comparison, a good quality Bi₄Ge₃O₁₂ (BGO) single crystal grown by Bridgman method was also studied. The light yield and energy resolution were measured using photomultiplier tube (XP5200B PMT) readout. Moderate light yield of 15,900 photons per MeV was measured for the LuAG:Pr(0.19%) crystal. For 662 keV gamma rays (¹³⁷Cs source), an energy resolution of 6.5% obtained for LuAG:Pr(0.19%) is much better than that of 9.0% obtained for BGO. The light yield non-proportionality and energy resolution versus energy of gamma rays were measured and the intrinsic resolution of the crystals was determined after correcting the measured energy resolution for PMT statistics. The LuAG:Pr(0.19%) showed a good proportionality of the light yield within 5% over the energy range from 1274.5 keV down to 32 keV, which is much better than that of 14% for BGO. The photofraction was determined at 320 and 662 keV for both crystals and compared with the ratio of the cross-sections for the photoelectric effect to the total one calculated using WinXCOM program.     

Electron paramagnetic resonance study of exchange coupled Ce3+ ions in Lu2SiO5 single crystal scintillator

The Ce³⁺ ions incorporation inside lutetium oxyorthosilicate (Lu₂SiO₅) single crystals was studied by electron paramagnetic resonance. Already known Ce1 and Ce2 centers originating from the lattice peculiarity allowing two lutetium sites coordinated by different number of the oxygen ions were detected. Remarkably, for the Ce2 center, the determined g² tensor is asymmetric and could not be diagonalized as compared to the Ce1 center, for which the three principal values and corresponding axes orientation have been determined and reported previously. Besides, the much weaker resonance lines found in spectra close to those coming from the Ce1 and Ce2, and following them under crystal rotation with respect to the direction of an external magnetic field, have been revealed as well. They were classified as doublets produced by the exchange coupled Ce³⁺ ions, creating the Ce1–Ce1, Ce2–Ce2 and Ce1–Ce2-like dimers. The corresponding spin–spin coupling constants were estimated. They are in the range 0.04–0.4 cm⁻¹. The Ce1, Ce2 and total dimer centers populations were calculated as 89%, 4.5% and 6.5%, comparing integral intensities of corresponding resonance lines.     

Gamma-ray emission from 134Ce and levels in 134La

The decay of ¹³⁴Ce to doubly odd ¹³⁴La has been studied using Ge(Li) and Si(Li) photon detectors. Samples of the ¹³⁴Ce(75.9 h)- ¹³⁴La(6.67 min) have been produced by ≈ 800 MeV proton bombardment of Pr foils in LAMPF, followed by chemical and mass separation. To increase the sensitivity (by up to a factor ≈ 50) for detection of ¹³⁴Ce γ-rays in the presence of the interfering ¹³⁴La activity, the ¹³⁴Ce-¹³⁴La samples were loaded onto a HDEHP column and the ¹³⁴La eluted off continuously. Gamma-ray singles and γ-γ coincidence measurements were made using the ¹³⁴Ce activity remaining on the column as the source. Some 32 γ-rays, ranging in energy up to 355 keV, are observed to be associated with this decay. Approximately 30 of these have been fitted into a level scheme for ¹³⁴La with excited states at energies of 31, 54, 93, 136 or 148, 162, 187, 150 or 205, 252, 294 and 355 keV. Only limits can be set for the spin and parity values of each of these states. The observation of γ-rays with energies up to 355 keV indicates that the previously reported values of ≈ 0.1 MeV for the ¹³⁴Ce electron-capture decay energy, inferred from the K-electron capture probability, are incorrect.     

The radiation induced color centers of the LaBr3:Ce crystal

This paper presents study of the gamma-rays induced radiation damage in the LaBr₃:Ce crystal. The light output and transmittance are measured before and after γ-rays irradiations with an integrated dose up to 10⁶ rad for two LaBr₃:Ce samples. After γ-rays irradiation, LaBr₃:Ce crystal shows very slow recovery process or has no recover under room temperature, indicating that the radiation damage in LaBr₃:Ce crystal is not dose date dependent. Meanwhile, it's found that the radiation induced color centers are respectively peaked at the wavelength of 448 nm, 512 nm and 590 nm. Those color centers should be ascribed to the V_k, V_F and F center respectively.     

Intrinsic ultraviolet luminescence from Lu2O3, Lu2SiO5 and Lu2SiO5:Ce

Radioluminescence and thermally stimulated luminescence measurements on Lu₂O₃, Lu₂SiO₅ (LSO) and Lu₂SiO₅:Ce³⁺ (LSO:Ce) reveal the presence of intrinsic ultraviolet luminescence bands. Characteristic emission with maximum at 256 nm occurs in each specimen and is attributed to radiative recombination of self-trapped excitons. Thermal quenching of this band obeys the Mott-Seitz relation yielding quenching energies 24, 38 and 13 meV for Lu₂O₃, LSO and LSO:Ce, respectively. A second intrinsic band appears at 315 nm in LSO and LSO:Ce, and at 368 nm in Lu₂O₃. Quenching curves for these bands show an initial increase in peak intensity followed by a decrease. Similarity in spectral peak position and quenching behavior indicate that this band has a common origin in each of the samples and is attributed to radiative recombination of self-trapped holes, in agreement with previous work on similar specimens. Comparison of glow curves and emission spectra show that the lowest temperature glow peaks in each specimen are associated with thermal decay of self-trapped excitons and self-trapped holes. Interplay between the intrinsic defects and extrinsic Ce³⁺ emission in LSO:Ce is strongly indicated.     

Imaging performance and light emission efficiency of Lu<Subscript>2</Subscript> SiO<Subscript>5</Subscript>:Ce (LSO:Ce) powder scintillator under X-ray mammographic conditions

The aim of the present study was to measure the imaging transfer characteristics and the luminescence efficiency (XLE) of a Lu₂SiO₅:Ce (LSO:Ce) powder scintillator for use in X-ray mammography detectors. An LSO:Ce powder scintillating screen, with a coating thickness of 25 mg/cm², was prepared in our laboratory. The imaging performance of the screen was assessed by experimental determination of the modulation transfer function (MTF) and the detective quantum efficiency (DQE) as well as single index image quality parameters such as noise equivalent pass band (Ne) and informational efficiency (n _I). A theoretical model, describing radiation and light transfer, was fitted to experimental MTF values in order to estimate optical properties of the scintillator. Screen irradiation was performed under exposure conditions employed in mammographic applications (27 kVp, 63 mAs). MTF was determined by the square wave response function (SWRF) method. Results showed that LSO:Ce exhibits high MTF and DQE values, which are comparable to those of the commercially used Gd₂O₂S:Tb. Considering our image quality parameters and luminescence efficiency results as well as the fast response of the LSO:Ce scintillator screen (40 ns), this material can be considered for use in X-ray mammographic detectors.     

Dopant concentration dependence of radiation-induced positive hysteresis of Ce:GSO and Ce:GSOZ

Positive hysteresis and radiation tolerance to high-dose radiation exposure were investigated for Ce 0.5, 1, and 1.5%-doped Gd₂SiO₅ (GSO) and for Zr co-doped GSO with the same Ce concentrations (GSOZ). When they were irradiated by 200–800 Gy ⁶⁰Co in 200 Gy steps, all Ce-doped GSO samples exhibited light yield enhancement (positive hysteresis). On the other hand, the light yield of GSOZ decreased greatly. Ce 0.5%-doped GSO showed the highest positive hysteresis, with ∼20% light yield enhancement. When the Ce concentration was increased, the positive hysteresis became weaker.     

5d–4f luminescence of Ce3+, Gd3+ and Lu3+ in LiCaAlF6

The emission and excitation spectra as well as decay kinetics of luminescence due to 5d–4f transitions in Ce³⁺, Gd³⁺ and Lu³⁺ ions doped into LiCaAlF₆ crystals have been analyzed with high spectral and time resolution using synchrotron radiation for excitation. The rich fine structure originating from electronic origins of transitions and their phonon replica has been well resolved and identified. Experimental data are compared with the spectra simulated in the framework of the semiphenomenological models of the crystal field and the crystal lattice dynamics.     

Luminescence and origin of lead-related centers in single crystalline films of Y2SiO5 and Lu2SiO5

In the temperature range 4.2–350 K, the steady-state and time-resolved emission and excitation spectra and luminescence decay kinetics are studied for the undoped Y₂SiO₅ and Lu₂SiO₅ single crystalline films grown by liquid phase epitaxy method from the PbO-based flux and, owing to that, containing lead ions substituting for Y³⁺ or Lu³⁺ ions. Luminescence characteristics of Pb-related centers of different types are identified. On the basis of the results obtained, we suggest that the ultraviolet emission of Pb-related centers arises from the Pb²⁺ ions substituting for Y³⁺ or Lu³⁺ ions in the Y1 and Lu1 lattice sites of the X₂ structure. Possible hypotheses on the origin of the intense complex lead-related blue emission are discussed. We propose phenomenological models describing the excited-state dynamics of the studied luminescence centers. We also determine characteristic parameters of the corresponding relaxed excited states, in particular, the energy separations between the excited states and the rates of the radiative and non-radiative transitions from these states.     

Anti-ferromagnetic ordering and crystal electric field in Ce:GSAG and Ce:LLGG garnets

The magnetic susceptibility of Ce:Gd₃Sc₃Al₃O₁₂ (Ce:GSAG) and Ce:La₃Lu₂Ga₃O₁₂ (Ce:LLGG) has been studied in the temperature range from 15 to 293 K. Both the Ce-doped garnets Ce:GSAG and Ce:LLGG show anti-ferromagnetic ordering at 18 and 27 K, respectively. Crystal electric field split energy levels have been used to calculate the magnetic susceptibility following Van Vleck's model. The calculated susceptibility values reasonably agree with the experimental susceptibility data of Ce:LLGG but differ for that of Ce:GSAG system. Contribution from long-range ordering between Ce and Gd ions for anomaly in Ce:GSAG system is speculated.