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Journal of Luminescence

Temporal dynamics of the frequency non-degenerate transient photoluminescence enhancement observed following excitation of inter-configurational f→d transitions in CaF2:Yb2+

Pubudu S. Senanayake, Jon‐Paul R. Wells, Michael F. Reid, Rosa B. Hughes-Currie, Giel Berden, Roger J. Reeves, Andries Meijerink

Published Jul 28, 2017• 1 citation
Publisher
DOI
10.1016/j.jlumin.2017.07.053

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Impurity trapped excitons (ITEs) occurring in divalent ytterbium doped calcium and strontium fluoride crystals have been investigated by exploiting the radically different radiative decay rates of the lowest exciton state and higher excited states, utilizing a novel two-colour transient photoluminescence enhancement experiment. The ITE energy levels have been directly measured with the observation of sharp transitions occurring from the changes of states of the localized hole and broad bands associated with changes of state of the delocalized electrons. The dynamic behaviour under excitation by time delayed ultra-violet (UV) and infrared (IR) pulses has been observed allowing for the identification of excitation and decay pathways between the ITE states. The position and transition intensities of the sharp lines within the IR excitation spectrum have been successfully matched using a semi-empirical effective Hamiltonian crystal field model. In CaCaF₂:Yb²⁺ the lines occurring at 249 and 1145 cm⁻¹ were matched with the crystal field parameter B4 = 800 cm⁻¹ and the exchange parameter G3(fs) = 5900 cm⁻¹. In SrCaF₂:Yb²⁺ these lines were observed at 178 and 1284 cm⁻¹ and matched with B4 = 600 cm⁻¹ and G3(fs) = 7278 cm⁻¹. Local heating and direct absorption by intra-excitonic transitions are found to be the causes of the broad band observed in the spectrum and have been deconvolved by studying the dynamic behaviour of the monitored emission at different IR excitation frequencies. Through this modeling, higher lying ITE states have been identified occurring at 785 cm⁻¹ in SrCaF₂:Yb²⁺ and in between 740 - 820 cm⁻¹ in CaCaF₂:Yb²⁺. The dynamic model developed successfully simulates the temporal behaviour of the emission under IR excitation under a variety of parameters including IR fluence, excitation frequency, sample temperature and UV - IR pulse delay. Examination of the SrCaF₂:Yb²⁺ dynamic behaviour over a time scale of 100 ms shows UV driven trap population at a rate of approximately 3% per pulse, which are liberated and recycled to the Yb²⁺ ground state by the IR pulse. The two-colour technique is applied to MgCaF₂:Yb²⁺, a candidate for possible ITE emission. Temperature dependent emission spectra obtained under UV excitation indicates the possibility of an ITE state, independently populated from the 5d level of the Yb²⁺. Typical 5d emission is also observed from this system. Under IR excitation, liberation of shallow traps and possible local heating is observed. No ITE emission is conclusively found with IR probing.
We explore an array of quantum emitters as non-equilibrium probes, coupled to a one-dimensional photonic waveguide, aiming to estimate its properties such as wave number which encodes the waveguide frequency and dispersive characteristics. By considering transient dynamics following initial excitation, we show that the quantum Fisher information (QFI) can be significantly enhanced through careful emitter positioning. For two-emitter probes, optimal spacing stabilizes populations and coherences in the single-excitation subspace, suppressing super radiant decay and extending both the magnitude and longevity of QFI. Randomized emitter configurations also reveal that vanishing waveguide-mediated cross decay maximizes both achievable sensitivity and the temporal duration over which information about the parameter remains accessible. Extending to multipartite probes, we demonstrate that the maximum QFI and its temporal integral scale with system size, exceeding the Heisenberg limit for all positioning strategies. Our results highlight the potential of waveguide-coupled emitter arrays as versatile quantum sensors, where collective radiative dynamics can be harnessed to achieve tunable, long-lived, and enhanced precision.