Optimized Scintillator YAG:Pr Nanoparticles for X-ray Inducible Photodynamic Therapy.

We describe a sol-gel synthetic method for the production of praseodymium-doped yttrium aluminum garnet (YAG) nanoparticles suitable for X-ray inducible photodynamic therapy (X-PDT). Our sol-gel based approach was optimized by varying temperature and time of calcination, resulting in nanoparticles that were smooth, spherical, and 50-200 nm in crystallite size. The powders were uniformly coated with a thin (10 nm) layer of silica to facilitate surface conjugation with functional moieties. Measurements of photon flux revealed that coated and uncoated powders emitted a similar photon emission spectrum in response to 50 keVp X-rays. We also determined that the presence of silica did not significantly reduce flux and the emission peak had a maximum at approximately 320 nm. Thus, these YAG:Pr powders are suitable candidates for future in vivo X-PDT studies.

Monte Carlo simulations of time-of-flight PET with double-ended readout: calibration, coincidence resolving times and statistical lower bounds.

This paper demonstrates through Monte Carlo simulations that a practical positron emission tomograph with (1) deep scintillators for efficient detection, (2) double-ended readout for depth-of-interaction information, (3) fixed-level analog triggering, and (4) accurate calibration and timing data corrections can achieve a coincidence resolving time (CRT) that is not far above the statistical lower bound. One Monte Carlo algorithm simulates a calibration procedure that uses data from a positron point source. Annihilation events with an interaction near the entrance surface of one scintillator are selected, and data from the two photodetectors on the other scintillator provide depth-dependent timing corrections. Another Monte Carlo algorithm simulates normal operation using these corrections and determines the CRT. A third Monte Carlo algorithm determines the CRT statistical lower bound by generating a series of random interaction depths, and for each interaction a set of random photoelectron times for each of the two photodetectors. The most likely interaction times are determined by shifting the depth-dependent probability density function to maximize the joint likelihood for all the photoelectron times in each set. Example calculations are tabulated for different numbers of photoelectrons and photodetector time jitters for three 3 × 3 × 30 mm3 scintillators: Lu2SiO5:Ce,Ca (LSO), LaBr3:Ce, and a hypothetical ultra-fast scintillator. To isolate the factors that depend on the scintillator length and the ability to estimate the DOI, CRT values are tabulated for perfect scintillator-photodetectors. For LSO with 4000 photoelectrons and single photoelectron time jitter of the photodetector J = 0.2 ns (FWHM), the CRT value using the statistically weighted average of corrected trigger times is 0.098 ns FWHM and the statistical lower bound is 0.091 ns FWHM. For LaBr3:Ce with 8000 photoelectrons and J = 0.2 ns FWHM, the CRT values are 0.070 and 0.063 ns FWHM, respectively. For the ultra-fast scintillator with 1 ns decay time, 4000 photoelectrons, and J = 0.2 ns FWHM, the CRT values are 0.021 and 0.017 ns FWHM, respectively. The examples also show that calibration and correction for depth-dependent variations in pulse height and in annihilation and optical photon transit times are necessary to achieve these CRT values.

Bright and ultra-fast scintillation from a semiconductor?

Semiconductor scintillators are worth studying because they include both the highest luminosities and shortest decay times of all known scintillators. Moreover, many semiconductors have the heaviest stable elements (Tl, Hg, Pb, Bi) as a major constituent and a high ion pair yield that is proportional to the energy deposited. We review the scintillation properties of semiconductors activated by native defects, isoelectronic impurities, donors and acceptors with special emphasis on those that have exceptionally high luminosities (e.g. ZnO:Zn, ZnS:Ag,Cl, CdS:Ag,Cl) and those that have ultra-fast decay times (e.g. ZnO:Ga; CdS:In). We discuss underlying mechanisms that are consistent with these properties and the possibilities for achieving (1) 200,000 photons/MeV and 1% fwhm energy resolution for 662 keV gamma rays, (2) ultra-fast (ns) decay times and coincident resolving times of 30 ps fwhm for time-of-flight positron emission tomography, and (3) both a high luminosity and an ultra-fast decay time from the same scintillator at cryogenic temperatures.

Monte Carlo calculations of PET coincidence timing: single and double-ended readout.

We present Monte Carlo computational methods for estimating the coincidence resolving time (CRT) of scintillator detector pairs in positron emission tomography (PET) and present results for Lu2SiO5 : Ce (LSO), LaBr3 : Ce, and a hypothetical ultra-fast scintillator with a 1 ns decay time. The calculations were applied to both single-ended and double-ended photodetector readout with constant-fraction triggering. They explicitly include (1) the intrinsic scintillator properties (luminosity, rise time, decay time, and index of refraction), (2) the exponentially distributed depths of interaction, (3) the optical photon transport efficiency, delay, and time dispersion, (4) the photodetector properties (fill factor, quantum efficiency, transit time jitter, and single electron response), and (5) the determination of the constant fraction trigger level that minimizes the CRT. The calculations for single-ended readout include the delayed photons from the opposite reflective surface. The calculations for double-ended readout include (1) the simple average of the two photodetector trigger times, (2) more accurate estimators of the annihilation photon entrance time using the pulse height ratio to estimate the depth of interaction and correct for annihilation photon, optical photon, and trigger delays, and (3) the statistical lower bound for interactions at the center of the crystal. For time-of-flight (TOF) PET we combine stopping power and TOF information in a figure of merit equal to the sensitivity gain relative to whole-body non-TOF PET using LSO. For LSO crystals 3 mm × 3 mm × 30 mm, a decay time of 37 ns, a total photoelectron count of 4000, and a photodetector with 0.2 ns full-width at half-maximum (fwhm) timing jitter, single-ended readout has a CRT of 0.16 ns fwhm and double-ended readout has a CRT of 0.111 ns fwhm. For LaBr3 : Ce crystals 3 mm × 3 mm × 30 mm, a rise time of 0.2 ns, a decay time of 18 ns, and a total of 7600 photoelectrons the CRT numbers are 0.14 ns and 0.072 ns fwhm, respectively. For a hypothetical ultra-fast scintillator 3 mm × 3 mm × 30 mm, a decay time of 1 ns, and a total of 4000 photoelectrons, the CRT numbers are 0.070 and 0.020 ns fwhm, respectively. Over a range of examples, values for double-ended readout are about 10% larger than the statistical lower bound.

Fundamental limits of scintillation detector timing precision.

In this paper we review the primary factors that affect the timing precision of a scintillation detector. Monte Carlo calculations were performed to explore the dependence of the timing precision on the number of photoelectrons, the scintillator decay and rise times, the depth of interaction uncertainty, the time dispersion of the optical photons (modeled as an exponential decay), the photodetector rise time and transit time jitter, the leading-edge trigger level, and electronic noise. The Monte Carlo code was used to estimate the practical limits on the timing precision for an energy deposition of 511 keV in 3 mm × 3 mm × 30 mm Lu2SiO5:Ce and LaBr3:Ce crystals. The calculated timing precisions are consistent with the best experimental literature values. We then calculated the timing precision for 820 cases that sampled scintillator rise times from 0 to 1.0 ns, photon dispersion times from 0 to 0.2 ns, photodetector time jitters from 0 to 0.5 ns fwhm, and A from 10 to 10,000 photoelectrons per ns decay time. Since the timing precision R was found to depend on A(-1/2) more than any other factor, we tabulated the parameter B, where R = BA(-1/2). An empirical analytical formula was found that fit the tabulated values of B with an rms deviation of 2.2% of the value of B. The theoretical lower bound of the timing precision was calculated for the example of 0.5 ns rise time, 0.1 ns photon dispersion, and 0.2 ns fwhm photodetector time jitter. The lower bound was at most 15% lower than leading-edge timing discrimination for A from 10 to 10,000 photoelectrons ns(-1). A timing precision of 8 ps fwhm should be possible for an energy deposition of 511 keV using currently available photodetectors if a theoretically possible scintillator were developed that could produce 10,000 photoelectrons ns(-1).

Shallow impurity level calculations in semiconductors using ab initio methods.

An ab initio method is presented to calculate shallow impurity levels in bulk semiconductors. This method combines the GW calculation for the treatment of the central-cell potential with a potential patching method for large systems (with 64,000 atoms) to describe the impurity state wave functions. The calculated acceptor levels in Si, GaAs, and an isovalent bound state of GaP are in excellent agreement with experiments with a root-mean-square error of 8.4 meV.

Ba(11)La(4)Br(34): a new barium lanthanum bromide.

The structure of the title compound, barium lanthanum bromide (11/4/34), can be derived from the fluorite structure. The asymmetric unit contains two Ba sites (one with site symmetry 4/m..), one La site (site symmetry 4..), one mixed-occupied Ba and La site (ratio 1:1, site symmetry m..) and six Br sites (one with site symmetry \=4.., one with 2.., one with m.., the latter being disordered over two positions with a 0.86:0.14 ratio). The fundamental building units of the structure are edge-sharing polyhedral clusters made up of Ba and La bromide clusters inter-connected to BaBr(8) square prisms and BaBr(10) groups.

A retrospective on the LBNL PEM project.

We present a retrospective on the LBNL Positron Emission Mammography (PEM) project, looking back on our design and experiences. The LBNL PEM camera utilizes detector modules that are capable of measuring depth of interaction (DOI) and places them into 4 detector banks in a rectangular geometry. In order to build this camera, we had to develop the DOI detector module, LSO etching, Lumirror-epoxy reflector for the LSO array (to achieve optimal DOI), photodiode array, custom IC, rigid-flex readout board, packaging, DOI calibration and reconstruction algorithms for the rectangular camera geometry. We will discuss the high-lights (good and bad) of these developments.