Vacuum ultraviolet silicon photomultipliers applied to BaF2cross-luminescence detection for high-rate ultrafast timing applications.

Inorganic scintillators are widely used for fast timing applications in high-energy physics (HEP) experiments, time-of-flight positron emission tomography and time tagging of soft and hard x-ray photons at advanced light sources. As the best coincidence time resolution (CTR) achievable is proportional to the square root of the scintillation decay time it is worth studying fast cross-luminescence, for example in BaF2which has an intrinsic yield of about 1400 photons/MeV. However, emission bands in BaF2are located in the deep-UV at 195 nm and 220 nm, which sets severe constraints on photodetector selection. Recent developments in dark matter and neutrinoless double beta decay searches have led to silicon photomultipliers (SiPMs) with photon detection efficiencies of 20%-25% at wavelengths of 200 nm. We tested state-of-the-art devices from Fondazione Bruno Kessler and measured a best CTR of 51 ± 5 ps full width at half maximum when coupling 2 mm × 2 mm × 3 mm BaF2crystals excited by 511 keV electron-positron annihilation gammas. Using these vacuum ultraviolet SiPMs we recorded the scintillation kinetics of samples from Epic Crystal under 511 keV excitation, confirming a fast decay time of 855 ps with 12.2% relative light yield and 805 ns with 84.0% abundance, together with a smaller rise time of 4 ps beyond the resolution of our setup. The total intrinsic light yield was determined to be 8500 photons/MeV. We also revealed a faster component with 136 ps decay time and 3.7% light yield contribution, which is extremely interesting for the fastest timing applications. Timing characteristics and CTR results on BaF2samples from different producers and with different dopants (yttrium, cadmium and lanthanum) are given, and clearly show that the the slow 800 ns emission can be effectively suppressed. Such results ultimately pave the way for high-rate ultrafast timing applications in medical diagnosis, range monitoring in proton or heavy ion therapy and HEP.

Cation influence on exciton localization in homologue scheelites.

Homologue scheelite crystals CaWO4, SrWO4, and BaWO4 possess similar crystal and electronic structure, but their luminescence exhibits drastically different thermal stabilities. By measuring the temperature dependence of the decay time of the intrinsic luminescence and fitting it to a three level model, we have qualitatively shown the effective exciton radius to increase in the order CaWO4 → SrWO4 → BaWO4, which explains the differences in the thermal stability. The origin of the variation in the exciton radii is suggested to be related to differences in the excited state dynamics in these crystals. From the decay kinetics measured under conditions of high excitation density, the efficiency of dipole-dipole interaction between excitons is shown to grow with exciton delocalization.

Band tail absorption saturation in CdWO4 with 100 fs laser pulses.

The decay kinetics of the excitonic emission of CdWO4 scintillators was studied under excitation by powerful 100 fs laser pulses in the band tail (Urbach) absorption region. A special imaging technique possessing both spatial and temporal resolution provided a unique insight into the Förster dipole-dipole interaction of self-trapped excitons, which is the main cause of the nonlinear quenching of luminescence in this material. In addition, the saturation of phonon-assisted excitonic absorption due to extremely short excitation pulses was discovered. A model describing the evolution of electronic excitations in the conditions of absorption saturation was developed and an earlier model of decay kinetics based on the Förster interaction was extended to include the saturation effect. Compared to the previous studies, a more accurate calculation yields 3.7 nm as the Förster interaction radius. It was shown that exciton-exciton interaction is the main source of scintillation nonproportionality in CdWO4. A quantitative description using a new model of nonproportionality was presented, making use of the corrected value of the Förster radius.

A luminescence spectroscopy and theoretical study of 4f-5d transitions of Ce3+ ions in SrAlF5 crystals.

This research is focused on the 4f-5d transitions in Ce(3+) centers doped into tetragonal ß-SrAlF(5) single crystals belonging to the I4(1)/a space group. The presence of four non-equivalent Sr(2+) sites in this compound leads to the appearance of three spectroscopically non-equivalent Ce(3+) luminescence centers, which can be well distinguished using a time-resolved laser spectroscopy technique. All 4f-5d transitions have slightly varying excitation and emission energies with characteristic probabilities resulting in several decay times that can be determined experimentally. One of these centers experiences strong perturbation due to a defect nearby, probably the O(2-) impurity ion substituting for the F(-) ion and acting as a charge compensator as well. Identification of these photoluminescence centers is performed using crystal field calculations. The crystal field parameters are calculated for two identified centers using the structural data for SrAlF(5); diagonalization of the crystal field Hamiltonian results in obtaining the splitting of the Ce(3+) 5d states. This method allows 'regular' unperturbed Ce(3+) centers with selected Sr(2+) sites to be assigned.

Resonant inelastic x-ray scattering and UV-VUV luminescence at the Be 1s edge in BeO.

We carried out a combined study of UV-VUV luminescence and resonant x-ray emission from BeO single crystals with incident photon energies in the vicinity of the Be 1s absorption edge. The x-ray emission spectra show that at the Be 1s photoabsorption edge the lattice relaxation processes in the excitation site take place already on the timescale of the radiative decay of the core excitation. Comparison of the x-ray emission and the luminescence spectra indicates that the maximum energy loss of the process of lattice relaxation during the decay of inner-shell holes is similar to the loss that occurs in the self-trapping process of valence excitons. The possible decay channels of core excitations have been discussed and the mechanism for the creation of 5.2 eV luminescence at the photoabsorption resonances has been suggested.

Luminescence properties of undoped LiBaAlF6 single crystals.

This paper presents the results of the study of electronic excitations in undoped LiBaAlF(6) single crystals by means of luminescence spectroscopy and complimentary optical methods. The intrinsic emission at 4.2 eV due to self-trapped excitons was identified. The fast nanosecond defect-related luminescence was revealed at 3.0 eV. Both emissions degrade under electron beam irradiation, the most probable reason of which is defect creation introducing an additional non-radiative relaxation channel prohibiting energy transfer to luminescence centers. These defects can be recovered and luminescence intensity restored at higher temperatures (>200 K). The permanent damage by electron beam irradiation results only in overall growth of the absorption coefficient in the whole 1.5-6.5 eV spectral region studied. The analysis of thermally stimulated luminescence glow curves in the temperature range of 5-410 K revealed two shallow charge carrier traps with the activation energies of 0.22 and 0.33 eV, respectively. The luminescence of an impurity peaked at 2.5 eV was found and tentatively assigned to an oxygen-related emission center.

Luminescence of singlet self-trapped excitons in MgF(2).

Fast (τ∼1.7 ns) broadband (full width at half-maximum = 1.1 eV) vacuum ultraviolet (VUV; hν = 8.4 eV) luminescence from MgF(2) crystals has been detected at low temperature (T<80 K) and analyzed with techniques of cathodoluminescence and time-resolved VUV spectroscopy using synchrotron radiation. The VUV emission discovered has been attributed to the luminescence of spin-singlet self-trapped excitons (STEs). In contrast to the case for alkaline earth fluoride crystals with fluorite structure, the luminescence of the singlet STEs in MgF(2) shows smaller Stokes shift than that of the triplet STEs, which is similar to 'typical' behavior observed for alkali halide crystals.

Triplet luminescence of cadmium centres in alkaline-earth fluoride crystals.

The emission and excitation spectra as well as decay of emissions of alkaline-earth fluoride crystals doped with CdF2 were investigated in the 2-24 eV range at temperatures in the range 8-300 K. Emission bands at 4.2 and 3.5 eV, respectively, were found under excitation into the Cd absorption region in CaF2-Cd and SrF2-Cd crystals at low temperatures. Both emission bands have slow luminescence decay times of microsecond timescale. No Cd-related emission was found in BaF2-Cd crystals. The calculations of the geometrical configurations of excited triplet Cd2+ centres and the Cd-related electron transitions were carried out by using the ab initio Hartree-Fock method. The results of experiments and calculations lead us to the conclusion that the observed Cd2+ emission bands are due to the triplet-singlet transitions from the Cd s-states to the nearest fluorine ions. The calculated energies are in good agreement with experimentally observed ones.