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Journal de Physique IV (Proceedings)

Mechanisms of up-conversion excitation of blue emission in YAG:Tm, Yb

A. KNÜPFER, V. Ostroumov, ERNST HEUMANN, Günter Huber, Voicu Lupei

Published Apr 1, 1994• 4 citations
Publisher

Abstract

Trivalent ytterbium ions were used as sensitizers for the 1D2 and 1G4 blue emitting thulium levels. The evolution of the population of the 1D2, 1G4, 3H4, 3F4 levels of Tm3+ and the 2F5/2 level of Yb3+ were investigated after short resonant excitation into these levels in YAG:Tm, Yb crystals. We observed upconversion fluorescence with a fast cooperative process followed by a slower step-by-step-process.

DOI
10.1051/jp4:19944120

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Trivalent ytterbium ions were used as sensitizers for the 1D2 and 1G4 blue emitting thulium levels. The evolution of the population of the 1D2, 1G4, 3H4, 3F4 levels of Tm3+ and the 2F5/2 level of Yb3+ were investigated after short resonant excitation into these levels in YAG:Tm, Yb crystals. We observed upconversion fluorescence with a fast cooperative process followed by a slower step-by-step-process.
Cooperative luminescence phenomenon of Yb:YAG crystals was studied. Up-converted blue luminescence was obviously observed in Yb:YAG under excitation in the near-infrared region with a wavelength 940 nm. Experimental evidence was provided by the fact that the intensity of 498 nm luminescence shows a quadratic dependence on excitation power, and the intensity of blue luminescence increased with the increase in Yb ion concentration. It is concluded that this luminescence is due to a cooperative process resulting from a strong interaction of Yb ions. The cooperative luminescence is possiblely assigned to the strong interaction of 4f(13) electrons and neighboring Yb3+ ions in a covalent host lattice such as YAG. Theoretical cooperative luminescence spectrum was calculated.
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Studies of infrared quantum counter upconversion in LaF3:Pr3+ and LaCl3:Pr3+ have led to the discovery of a process in which a red excitation photon results in the emission of a blue photon. When the 1D2 level of Pr3+ is excited by a cw rhodamine 6-G dye laser, blue fluorescence from the 3P0 level is observed. From the flux dependence and lifetime of the induced fluorescence, we conclude that the observed phenomenon arises from excitation annihilation involving pairs of ions in the 3H6 and the 1D2 states.
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.
New efficient mechanisms of long-wavelength excitation of short-wavelength luminescence in a system of rare-earth impurity ions are proposed. The model studied involves a multilevel system of electronic states of a rare-earth ion interacting with the long-wavelength emission that is in resonance with one or several transitions between the excited levels. The concentration of impurity ions is assumed to be sufficiently high, so that the interionic cross-relaxation and the up-conversion play a significant role. Moreover, the model includes processes similar to photon avalanche, in which the photoinduced excitation of a single ion is converted into lower-level excitations of several ions, each of them reentering the process after photon absorption. Numerical solutions of the system of balance equations for a multilevel system are obtained with calculated and semiempirical parameters of self-quenching and up-conversion. It is shown that, in a system of Tm 3+ impurity ions, short-wavelength luminescence at λ≥0.29 μm can be efficiently excited by radiation at λ≅1.11 or 0.649 μm with a moderate intensity.
The possibility of using stimulated emission to improve the optical pumping of Tm3+ ions embedded in Tm3+:YAG to the 3F4 level is explored. The oscillator strengths and the frequencies of the transitions between the ground crystal field level of 3H4 to the different crystal field levels of 3F4 are measured at low temperature. Stimulated emission measurements at 1461 nm are performed to evaluate the optical pumping efficiency. Application to the spectral tailoring of Tm3+:YAG for quantum information applications is discussed.