Origin of resolution enhancement by co-doping of scintillators: Insight from electronic structure calculations

It was recently shown that the energy resolution of Ce-doped LaBr$_3$ scintillator radiation detectors can be crucially improved by co-doping with Sr, Ca, or Ba. Here we outline a mechanism for this enhancement on the basis of electronic structure calculations. We show that (i) Br vacancies are the primary electron traps during the initial stage of thermalization of hot carriers, prior to hole capture by Ce dopants; (ii) isolated Br vacancies are associated with deep levels; (iii) Sr doping increases the Br vacancy concentration by several orders of magnitude; (iv) $\text{Sr}_\text{La}$ binds to $V_\text{Br}$ resulting in a stable neutral complex; and (v) association with Sr causes the deep vacancy level to move toward the conduction band edge. The latter is essential for reducing the effective carrier density available for Auger quenching during thermalization of hot carriers. Subsequent de-trapping of electrons from $\text{Sr}_\text{La}-V_\text{La}$ complexes then can activate Ce dopants that have previously captured a hole leading to luminescence. This mechanism implies an overall reduction of Auger quenching of free carriers, which is expected to improve the linearity of the photon light yield with respect to the energy of incident electron or photon

Energy Transport and Scintillation of Cerium Doped Elpasolite Cs2LiYCl6: Hybrid Density Functional Calculations

Elpasolites are a large family of halides which have recently attracted considerable interest for their potential applications in room-temperature radiation detection. Cs2LiYCl6 is one of the most widely studied elpasolite scintillators. In this paper, we will show hybrid density functional calculations on electronic structure, energetics of small electron and hole polarons and self-trapped excitons, and the excitation of luminescence centers (Ce impurities) in Cs2LiYCl6. The results provide important understanding in energy transport and scintillation mechanisms in Cs2LiYCl6 and rare-earth elpasolites in general

Particle detection through the quantum counter concept in YAG:Er3+^{3+}

We report about a novel scheme for particle detection based on the infrared quantum counter concept. Its operation consists of a two-step excitation process of a four level system, that can be realized in rare earth-doped crystals when a cw pump laser is tuned to the transition from the second to the fourth level. The incident particle raises the atoms of the active material into a low lying, metastable energy state, triggering the absorption of the pump laser to a higher level. Following a rapid non-radiative decay to a fluorescent level, an optical signal is observed with a conventional detectors. In order to demonstrate the feasibility of such a scheme, we have investigated the emission from the fluorescent level $^4$S$_{3/2}$ (540 nm band) in an Er$^{3+}$-doped YAG crystal pumped by a tunable titanium sapphire laser when it is irradiated with 60 keV electrons delivered by an electron gun. We have obtained a clear signature this excitation increases the $^{4}I_{13/2}$ metastable level population that can efficiently be exploited to generate a detectable optical signal

Location of the Energy Levels of the Rare-Earth Ion in BaF2 and CdF2

The location of the energy levels of rare-earth (RE) elements in the energy band diagram of BaF2 and CdF2 crystals is determined. The role of RE3+ and RE2+ ions in the capture of charge carriers, luminescence, and the formation of radiation defects is evaluated. It is shown that the substantial difference in the luminescence properties of BaF2:RE and CdF2:RE is associated with the location of the excited energy levels in the band diagram of the crystals

Novel Scintillation Material - ZnO Transparent Ceramics

ZnO-based scintillation ceramics for application in HENPA LENPA analyzers have been investigated. The following ceramic samples have been prepared: undoped ones (ZnO), an excess of zinc in stoichiometry (ZnO:Zn), doped with gallium (ZnO:Ga) and lithium (ZnO:Li). Optical transmission, x-ray excited emission, scintillation decay and pulse height spectra were measured and analyzed. Ceramics have reasonable transparency in visible range (up to 60% for 0.4 mm thickness) and energy resolution (14.9% at 662 keV Cs137 gamma excitation). Undoped ZnO shows slow (1.6 {\mu}s) luminescence with maximum at 2.37 eV and light yield about 57% of CsI:Tl. ZnO:Ga ceramics show relatively low light yield with ultra fast decay time (1 ns). Lithium doped ceramics ZnO:Li have better decay time than undoped ZnO with fair light yield. ZnO:Li ceramics show good characteristics under alpha-particle excitation and can be applied for the neutral particle analyzers.Comment: 4 pages, 8 figures, research covered in this paper was presented at SCINT2011 conference as a poster, submitted for publication at IEEE Trans. Nucl. Sc

Electronic structure of LaBr3 from quasi-particle self-consistent GW calculations

Rare-earth based scintillators in general and lanthanum bromide (LaBr_3) in particular represent a challenging class of materials due to pronounced spin-orbit coupling and subtle interactions between d and f states that cannot be reproduced by standard density functional theory (DFT). Here a detailed investigation of the electronic band structure of LaBr_3 using the quasi-particle self-consistent GW (QPscGW) method is presented. This parameter-free approach is shown to yield an excellent description of the electronic structure of LaBr_3. Specifically it is able to reproduce the band gap, the correct level ordering and spacing of the 4f and 5d states, as well as the spin-orbit splitting of La-derived states. The QPscGW results are subsequently used to benchmark several computationally less demanding techniques including DFT+U, hybrid exchange-correlation functionals, and the G_0W_0 method. Spin-orbit coupling is included self-consistently at each QPscGW iteration and maximally localized Wannier functions are used to interpolate quasi-particle energies. The QPscGW results provide an excellent starting point for investigating the electronic structure of excited states, charge self-trapping, and activator ions in LaBr_3 and related materials.Comment: 8 pages, 7 figure

Mechanisms for Tuning Engineered Nanomaterials to Enhance Radiation Therapy of Cancer.

Engineered nanomaterials that produce reactive oxygen species on exposure to X- and gamma-rays used in radiation therapy offer promise of novel cancer treatment strategies. Similar to photodynamic therapy but suitable for large and deep tumors, this new approach where nanomaterials acting as sensitizing agents are combined with clinical radiation can be effective at well-tolerated low radiation doses. Suitably engineered nanomaterials can enhance cancer radiotherapy by increasing the tumor selectivity and decreasing side effects. Additionally, the nanomaterial platform offers therapeutically valuable functionalities, including molecular targeting, drug/gene delivery, and adaptive responses to trigger drug release. The potential of such nanomaterials to be combined with radiotherapy is widely recognized. In order for further breakthroughs to be made, and to facilitate clinical translation, the applicable principles and fundamentals should be articulated. This review focuses on mechanisms underpinning rational nanomaterial design to enhance radiation therapy, the understanding of which will enable novel ways to optimize its therapeutic efficacy. A roadmap for designing nanomaterials with optimized anticancer performance is also shown and the potential clinical significance and future translation are discussed