Quantum information transfer from light to atom ensembles and vice versa has both basic and practical importance. Among the relevant topics let us mention entanglement and decoherence of macroscopic systems, together with applications to quantum memory for long distance quantum cryptography. Although the first experimental demonstrations have been performed in atomic vapors and clouds, rare earth ion doped crystals are also interesting media for such processes. In this paper we address Tm 3+ ions capability to behave as threelevel Λ systems, a key ingredient to convert optical excitation into a spontaneous-emissionfree spin wave. Indeed Tm 3+ falls within reach of light sources that can be stabilized easily to the required degree. In the absence of zero-field hyperfine structure we apply an external magnetic field to lift the nuclear spin degeneracy in Tm 3+ :YAG. We experimentally determine the gyromagnetic tensor components with the help of spectral hole-burning techniques. Then appropriate orientation of the applied field enables us to optimize the transition probability ratio along the two legs of the Λ . The resulting three-level Λ system should suit quantum information processing requirements.

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A three-level Λ system in Tm 3+ doped YAG crystal is experimentally investigated in the prospect of quantum information processing. Zeeman effect is used to lift the nuclear spin degeneracy of this ion. In a previous paper [de Seze et al. Phys. Rev. B, 73, 85112 (2006)] we measured the gyromagnetic tensor components and concluded that adequate magnetic field orientation could optimize the optical connection of both ground state sublevels to each one of the excited state sublevels, thus generating Λ systems. Here we report on the direct measurement of the transition probability ratio along the two legs of the Lambda. Measurement techniques combine frequency selective optical pumping with optical nutation or photon echo processes.