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The Journal of Chemical Physics

Energy transfer upconversion in LaF3:Pr3+

Denis J. Zalucha, John Curtis Wright, Francis K. Fong

Published Aug 1, 1973• 47 citations
Publisher

Abstract

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.

DOI
10.1063/1.1680232

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Nonlinear Optical Properties of Materials•Jan 1, 1988•0 citations
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.
In this paper, we report the first laser-excited optical double-resonance experiments in rare-earth-doped crystals. Infrared upconversion in LaCl3 : Pr3+ and LaF3 : Pr3+ has been achieved by means of a tunable cw dye laser pump. The quantum efficiency of the upconversion process at 2.03 μ in LaCl3 : Pr3+ is 1.2×10−3, which is an improvement of 4×105 over the highest efficiency found previously with incoherent sources. It is shown that an efficiency of 1 can be easily obtained with higher fluxes and improved crystal quality. Direct excitation of the output fluorescence from the 3P0 level is observed in both LaCl3 : Pr3+ and LaF3 : Pr3+ when the dye laser frequency is resonant with the states of the lower-lying 1D2 manifold in the absence of the infrared input. Detailed assignments of the observed double-resonance transitions have been made from wavelength and polarization measurements.
We excite the (4f2)1s0 state directly through a two photon excited state absorption (from the 1D2 level) and indirectly through excitation of the 4f5d band (using an ArF excimer laser). In Pr3+:LaF3 the 1S0 state lies below the band, and only 1S0 emission is observed. In most hosts examined, it is above the band, and only 4f5d emission is observed. In Pr3+:CaF2 there are sites with each of these properties, and both 1S0 and 4f5d emission are observed, with a relative strength that is concentration dependent.
In this paper, we outline a novel method for the determination of oscillator strengths in rare-earth crystals. This method involves the observation of fluorescence resulting from a sequential two-photon excitation process. The rate equations are analyzed and a simple linear relationship between the laser flux, the fluorescent intensity, and the oscillator strength is derived. The equations are applied to LaCl3:Pr3+ and the resulting oscillator strength measured for the 3H6→3P1 transition is found to be in good agreement with the value measured by conventional absorption techniques. One advantage of the present method is the elimination of the need to determine the dopant concentration.
Short pulse laser-induced fluorescence experiments on the lowest-energy electronic states (υ<10−4 cm−1) of trivalent praseodymium ions are reported. Crystals of lanthanum trichloride with a range of Pr3+ concentrations were examined. We compute cross relaxation and upconversion coefficients for the metastable energy levels using a standard rate equation analysis. The limitations of the rate equation approach are examined with a focus on the underlying dynamics of this rare-earth system. The implications of these results for laser emission in the 1.3–7.2 μm spectral range are discussed.
We report an investigation of a nonlinear optical absorption phenomenon observed in LaCl3 crystals doped with Pr. When these crystals are illuminated with a laser beam of 529 nm wavelength and intensity in excess of a certain critical value, the light is strongly absorbed. The laser radiation is resonant with a Pr3+ transition from the first excited state (3H5) to a high optical state (3P1), and absorption is accompanied by strong fluorescence output from 3p1 and 3p0 to several lower-lying levels. Since the resonant transition does not include the ground state, it is not expected a priori that any absorption should occur (see Fig. 1). This is an example of the so-called photon avalanche phenomenon1.