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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Efficient Pr3+ laser material excitation by three-for-one cross-relaxation

Larry D. Merkle, Mark A. DUBINSKII

Published May 1, 2017• 0 citations
Publisher

Abstract

Pr3+ has three excited manifolds with the right energy spacings for emission between 3.5 and 5.5 microns, and can be excited efficiently using laser diodes developed for telecommunications. In the potential laser crystal Pr:RbPb2Cl5, we have observed strikingly strong fluorescence in this wavelength range following 1.53-micron excitation. Careful analysis indicates this must be due to two cross-relaxation processes that, together, efficiently convert one Pr3+ initially excited to the 3F3 manifold into three ions excited to the 3H5 manifold. This newly discovered “three-for-one” crossrelaxation process in Pr3+ may greatly enhance its utility as a mid-infrared laser ion.

DOI
10.1117/12.2264840

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Pr3+ has three excited manifolds with the right energy spacings for emission between 3.5 and 5.5 microns, and can be excited efficiently using laser diodes developed for telecommunications. In the potential laser crystal Pr:RbPb2Cl5, we have observed strikingly strong fluorescence in this wavelength range following 1.53-micron excitation. Careful analysis indicates this must be due to two cross-relaxation processes that, together, efficiently convert one Pr3+ initially excited to the 3F3 manifold into three ions excited to the 3H5 manifold. This newly discovered “three-for-one” crossrelaxation process in Pr3+ may greatly enhance its utility as a mid-infrared laser ion.
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.
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.
High resolution spectroscopy of quantum systems is a key point in the quantum information field. Rare earth ions in crystals are interesting candidates for this application because of the long coherence lifetime of some of their transitions. These ions can also be manipulated by optical excitation which has, however, to be produced by ultra-stable laser sources. This proves to be a very difficult task in the case of dye lasers which are necessary to excite Pr3+ doped crystals and especially Pr3+:Y2SiO5. This compound is by far the most used host in rare earth based quantum information studies. In this paper, we discuss the use of Pr3+,Yb3+ codoped materials to build an infrared pumped solid state laser suitable to excite Pr3+:Y2SiO5 around 606 nm. We show by the analysis of a rate equation model that avalanche upconversion is not very efficient to obtain a high power laser. This is more easily obtained if a second laser is set to pump resonantly Yb3+ ions. The spectroscopic properties of a new matrix Pr3+,Yb3+:PbF2 are also investigated. We found that this compound emits at 606.18 nm with a width of 5 nm and would be therefore suitable to excite Pr3+:Y2SiO5. Moreover, it can be excited at 857 nm and 975 nm, i.e. in the range of high power laser diodes.
In a Y2SiO5:Pr3+ crystal characterized by two non-equivalent Pr3+ optical centers, the interaction mechanisms between Pr3+ ions as well as between Pr3+ ions and a crystal lattice have been studied. It has been shown that along with the electron-phonon interaction, the interaction between Pr3+ ions and two-level systems made an additional contribution to the homogeneous linewidth of the 3H4↔3P0 optical transition. Two different mechanisms of the Pr3+ interionic coupling have been found. The first mechanism is associated with a dipole-dipole interaction between non-equivalent Pr3+ optical centers, while the other one is governed by a cooperative cross relaxation of the excitation energy among the same type Pr3+ optical centers.