Lithium Niobate Tantalate Solid Solutions Probed by Luminescence Spectroscopy

The polar oxide Lithium Niobate Tantalate is probed using time-resolved luminescence spectroscopy with the goal of revealing an initial structural insight into the solid solution by analyzing the spectral properties and dynamics of radiatively decaying self-localization phenomena. A blue-green luminescence band can be induced by ultraviolet nanosecond laser pulses with a temperature-dependent intensity and spectral width, pointing to the radiative decay of optically generated self-trapped excitons as its origin, i.e., electron–hole pairs with strong coupling to either the NbO6- or TaO6-octahedra. The luminescence decay takes place in the microsecond time range and deviates significantly from a single exponential behavior, so the determined lifetime constants of up to ≈70 μs and stretching factors (1/3–1/5) are validated in more detail using alternative evaluation methods. We discuss our findings, considering the interplay of radiative and non-radiative decay channels, the transition from self-trapped to free excitons, and the presence of a structural disorder of the oxygen octahedra in the solid solutions. Overall, our results suggest self-trapped excitons as local probes for an initial structural elucidation and provide essential information about further experimental and theoretical studies on the atomic structure of Lithium Niobate Tantalate, but also for improving the crystal quality in the framework of applications in photonics and quantum optics.