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The Journal of Chemical Physics

Site-selected luminescence of atomic europium in the solid rare gases

Owen Byrne, John G. McCaffrey

Published Jul 12, 2011• 5 citations
Publisher

Abstract

Site-selective excitation has been used to simplify complex emission recorded in the visible spectral region for atomic europium isolated in the solid rare gases. In addition to y(8)P resonance fluorescence, excitation of the y(8)P state produces emission from the z(6)P state and the metastable a(10)D state. Very weak emission at 690 nm is tentatively assigned to the J = 9/2 level of the z(10)P state. Eu atoms isolated in the red and blue sites exhibit very different temperature dependence both spectrally and temporally. For the y(8)P state emission the red site atoms exhibit small Stokes shifts and yield radiative lifetimes while the emission from the blue site loses intensity and the temporal profiles shorten dramatically between 10 and 16 K indicating very efficient non-radiative relaxation in this site. An analysis of the Stokes shifts exhibited for the y(8)P state in each site supports the attributions made in a previous publication [O. Byrne and J.G. McCaffrey, J. Chem. Phys. 134, 124501 (2011)] that the smaller blue tetravacancy site has a greater repulsive interaction with the guest. With the exception of the y(8)P state resonance fluorescence, the recorded decay profiles of all the other emissions exhibit multiple components. This behaviour has been attributed to the existence of multiple crystal field levels arising from the splitting of the distinct spin-orbit levels from which emission occurs.

DOI
10.1063/1.3609116

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Site-selective excitation has been used to simplify complex emission recorded in the visible spectral region for atomic europium isolated in the solid rare gases. In addition to y(8)P resonance fluorescence, excitation of the y(8)P state produces emission from the z(6)P state and the metastable a(10)D state. Very weak emission at 690 nm is tentatively assigned to the J = 9/2 level of the z(10)P state. Eu atoms isolated in the red and blue sites exhibit very different temperature dependence both spectrally and temporally. For the y(8)P state emission the red site atoms exhibit small Stokes shifts and yield radiative lifetimes while the emission from the blue site loses intensity and the temporal profiles shorten dramatically between 10 and 16 K indicating very efficient non-radiative relaxation in this site. An analysis of the Stokes shifts exhibited for the y(8)P state in each site supports the attributions made in a previous publication [O. Byrne and J.G. McCaffrey, J. Chem. Phys. 134, 124501 (2011)] that the smaller blue tetravacancy site has a greater repulsive interaction with the guest. With the exception of the y(8)P state resonance fluorescence, the recorded decay profiles of all the other emissions exhibit multiple components. This behaviour has been attributed to the existence of multiple crystal field levels arising from the splitting of the distinct spin-orbit levels from which emission occurs.
The electronic transitions of ytterbium atoms in a solid Xe matrix grown at 4.8 K are investigated. Absorption bands are detected in the regions of the gas-phase 6s2 1S0 → 4f135d6s2 and 6s2 1S0 → 6s6p 1P1 transitions. Both bands indicate that Yb atoms occupy multiple trapping sites, of which three are identified. Emission induced by the 6s2 1S0 → 6s6p 1P1 excitation is found to be concentrated entirely in the region of the 6s6p 3PJ → 6s2 1S0 decay, whereas the singlet emission is completely quenched. Multiple emission peaks are observed and the effects of annealing and prolonged irradiation on their amplitudes are found to be significant and are interpreted as a consequence of Yb population transfer from one type of site to another. Modeling of the ground-state site structure and stability predicts three Yb/Xe occupation types, substitutional (ss), tetravacancy (tv) and hexavacancy (hv), in order of decreasing stability. Their tentative associations with observed absorption and emission features are discussed. Time correlated single photon spectroscopy is used to determine the lifetimes of the individual emission bands. They are found to be different from each other with indications of a mixture of short- and long- lived 6s6p 3PJ fine-structure components and demonstrate distinct temperature dependencies. A dramatic decrease in the lifetime of the emission peak tentatively assigned to the most stable site with temperature is explained by a competition between the radiative and non-radiative decay paths of the 6s6p 3P1 state. The mechanism of the latter can be attributed to electron–phonon coupling as confirmed by a model of the temperature-dependence of the lifetime.
The low-lying electronic states of Yb isolated in a solid Ar matrix grown at 4.2 K are characterized through absorption and emission spectroscopy. Yb atoms are found to occupy three distinct thermally stable trapping sites labeled "red," "blue," and "violet" according to the relative positions of the absorption features they produce. Classical simulations of the site structure and relative stability broadly reproduced the experimentally observed matrix-induced frequency shifts and thus identified the red, blue, and violet sites as due to respective single substitutional (ss), tetravacancy (Tv), and hexavacancy (Hv) occupation. Prolonged excitation of the (1)S → (1)P transition was found to transfer the Yb population from hv sites into Tv and ss sites. The process showed reversibility in that annealing to 24 K predominantly transferred the Tv population back into Hv sites. Population kinetics were used to deduce the effective rate parameters for the site transformation processes. Experimental observations indicate that the blue and violet sites lie close in energy, whereas the red one is much less stable. Classical simulations identify the blue site as the most stable one.
Rare-earth (RE) atoms, such as erbium (Er), have inner-shell optical transitions in the near-infrared, some of which are in the telecom bands. These transitions are largely insensitive to the host environment due to effective shielding by the filled outer shells. Cryogenic rare-gas (RG) solids, such as solid neon (Ne) and argon (Ar), combine high chemical purity with a nearly nuclear-spin-free environment, making them attractive solid hosts for preserving optical and spin coherence. In this work, we isolate neutral Er atoms in solid Ne and Ar at 6 K and characterize their emission by steady-state and time-resolved photoluminescence (PL) spectroscopy. In both hosts, we observe several near-infrared transitions between 1000--1500 nm, including inner-shell emission in the telecom O and E bands. The 4f→5d4f \rightarrow 5d4f→5d transition near 1299 nm forms a multiplet of narrow components, consistent with crystal-field splitting, and decays on a microsecond timescale. The 4f→4f4f \rightarrow 4f4f→4f transition near 1437 nm shows a matrix shift below 1 cm−1^{-1}−1 in both hosts. In solid Ne, its inhomogeneous linewidth is bounded by the spectrometer resolution to < 22 GHz, and its PL lifetime reaches up to 78.9 ms, close to the estimated radiative limit. Thermal annealing extends the 1437 nm lifetime in Ne and suppresses the phonon sidebands relative to the zero-phonon lines in Ar. These results identify RG solids as promising hosts for long-lived telecom-band Er emission and provide a foundation for future spin-photon interfaces and hybrid quantum architectures.
Even-parity highly excited states of an europium (Eu) atom have been investigated by employing the three-colour stepwise resonant excitation technique. Seventy-eight even-parity states of the Eu atom have been detected in the energy region between 43 500 and 45 200 cm −1 with two different excitation schemes. With a detailed analysis of the experimental data, this work not only confirms or improves the previous results by determining their level energy, J assignment, but also reports 21 new states of the Eu atom with a unique J assignment. In addition, the information about relative line intensities of these 78 related transitions are also provided for the first time.
Abstract The luminescence of Ne* centers in solid Ne is investigated. The samples are excited with synchrotron radiation in the excitonic range. By an appropriate selection of the excitation energy and by time correlated measurement of the emission spectra, overlapping luminescence bands are separated and assigned to Ne* centers in different electronic states (1P1, 3P1, 3P2) and different environments in the bulk and at the surface of the solid. Lifetime measurements and excitation spectra of spectrally selected luminescence bands support the assignments, Electronic relaxation from n ≧ 2 free excitons to the n = 1 state is found to be less effective than exciton trapping into Ne* centers. Resonance fluorescence of free Ne* atoms indicates a close connection between exciton trapping and desorption.
A series of Yb3+-doped yttrium aluminum monoclinic Y4Al2O9 (Yb:YAM) single crystals with Yb3+ ion concentrations of 0.1, 1, 5 and 10 at.% was grown by means of micro pulling down method. Blue emission was observed in Yb3+ activated YAM crystals under infrared site-selective laser excitation. Through the excitation and emission spectra, decay time measurements and excitation intensity dependence the process responsible for this anti-Stokes emission was assigned to the cooperative deexcitation of two Yb3+ ions. The results show that at 10% Yb3+ dopant concentration investigated system could be considered as single-site system in which cooperative luminescence is dominated by the energetically lowest Yb3+ site. Theoretical cooperative emission spectrum and the cooperative luminescence rate of Yb3+:YAM were calculated.