Thermoluminescence due to tunneling in nanodosimetric materials: A Monte Carlo study

Thermoluminescence (TL) signals from nanodosimetric materials have been studied extensively during the past twenty years, especially in the area of nanomaterials doped with rare earths. One of the primary effects being studied experimentally have been possible correlations between the nanocrystal size and the shape and magnitude of TL signals. While there is an abundance of experimental studies attempting to establish such correlations, the underlying mechanism is not well understood. This paper is a Monte Carlo simulation study of the effect of nanocrystal size on the TL signals, for materials in which quantum tunneling is the dominant recombination mechanism. TL signals are simulated for a random distribution of electrons and positive ions, by varying the following parameters in the model: the radius of the crystal R, tunneling length a, and the relative concentrations of electrons and ions. The simulations demonstrate that as the radius of the nanocrystals becomes larger, the peaks of the TL glow curves shift towards lower temperatures and changes occur in both peak intensity and peak width. For large crystals with a constant density of positive ions, the TL glow curves reach the analytical limit expected for bulk materials. The commonly used assumption of nearest neighbor interactions is examined within the model, and simulated examples are given in which this assumption breaks down. It is demonstrated that the Monte Carlo method presented in this paper can also be used for linearly modulated infrared stimulated luminescence (LM-IRSL) signals, which are of importance in luminescence dosimetry and luminescence dating applications. New experimental data are presented for Durango apatite, a material which is known to exhibit strong anomalous fading due to tunneling; the experimental data is compared with the model. The relevance of the simulated results for luminescence dosimetry is discussed.