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Tinsley, James R.

Publications and source records attributed to Tinsley, James R..

Time-Resolved Radioluminescence of the Copper(I) Cluster Cu4I62-. Temporal responses to Photo, X-ray, Beta-ray, and alpha-ray Excitation.

Described are time-resolved radioluminescence (TRRL) properties of the Cu(I) cluster Cu4I62– upon pulsed X-ray, β-ray or α-particle excitation. The longer (>2 μs) TRRL component displayed exponential decay comparable to pulsed UV excitation; however, temporal behavior at shorter times indicates that high local excited state density provides an alternative decay channel.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Time-Resolved Radioluminescence of the Polynuclear Copper(I) Phosphor Cu4I6²–. Different Temporal responses to Photo, X-Ray, β-Ray and α-Particle Excitation

Described for the first time are the time-resolved radioluminescence (TRRL) properties of the highly luminescent copper(I) cluster Cu4I62– using X-ray, b-ray and a-particle excitation. The copper(I) phosphors are two crystalline salts of this anion, [Na2(18-crown-6)2(H2O)3][Cu4I6] (I) and [Li(benzo-15-crown-5)2(H2O)]2[Cu4I6] (II), that had been shown to display strong photoluminescence (PL) when excited with ultraviolet light. The integrated radioluminescence (RL) spectra observed when pulsed X-rays were used as the excitation source are virtually the same as the PL spectra under comparable conditions. These temporal RL spectra are invariant at all observation times indicating that the observed scintillation occurs from a common excited state (or set of excited states). When the TRRL is collected from excitation with a pulsed X-ray source, b-ray decay from 90Sr or a-decay from 244Cm, the longer components (>2 μs) of the TRRL displayed (in each case) lifetimes comparable to those of the strictly exponential PL decays recorded under pulsed laser UV excitation. However, at shorter observation times (< 500 ns), the RL decay deviated from the exponential model, indicating a markedly different temporal luminescence behavior when these materials were excited with pulsed high energy radiation. Furthermore, this effect was the most pronounced for the a-particle excitation. These results suggest that the absorption of a very high energy X-ray photon, b-ray or a-particle at a site within the crystalline solid leads to a high local density of electronic excited states and that coupling between these states provides an alternative channel for excited state decay. Given that the patterns observed

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

End-to-End Simulations of a 3.4-Meter Detector Wall for Neutron-Diagnosed Subcritical Experiments

The Nevada National Security Site, together with Los Alamos National Laboratory and Lawrence Livermore National Laboratory, is developing a novel diagnostic to measure the reactivity of subcritical experiments. This capability is known as neutron-diagnosed subcritical experiments. The decay of the fission gamma rays from the neutron-interrogated subcritical experiment is measured as a function of time with a large (~3-meter diameter) detector wall consisting of 151 individual detector pixels. The data from this current mode measurement inform the neutron multiplication factor, keff, and thus the relative reactivity of the subcritical experiment. The Nevada National Security Site developed the Gamma Array Simulation Toolkit initially to help inform the design of the individual detector pixels and the 3.4-meter diameter detector wall to be fielded as part of neutron-diagnosed subcritical experiments. This toolkit is now being used to simulate and predict the performance of the final design of the individual detector pixels and the aggregate detector wall. Additionally, key detector characteristics evaluated from these simulations include impulse response, pulse height spectrum, number of photoelectrons per MeV, detector efficiency, and cross talk between detector pixels. Collectively, the results of these simulations inform how well the fission gamma ray die-off distribution from a neutron-diagnosed subcritical experiment measurement can be resolved. This is critical to determining the relative reactivity of the experiment. Furthermore, the Gamma Array Simulation Toolkit can be used to aid in the analysis of the experimental data from a neutron-diagnosed subcritical experiment measurement once the simulation has been benchmarked.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗