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

Cooperative optical phenomena in praseodymium doped CsCdBr 3

Johann Heber, Sergey I. Nikitin, R. Demirbilek, A.G. Papashvili, Ivan N. Vorob'ev, Olimkhon K. Alimov, Yu.V. Orlovskii, E.O. Orlovskaya

Published Jul 12, 2002• 2 citations
Publisher

Abstract

In CsCdBr3 the trivalent Rare-Earth (RE) ions substitute for the divalent Cd ions. For reasons of charge compensation and the specific crystal structure, RE centers of the form RE3+ - (Cd vacancy) - RE3+ are preferentially formed. These symmetric pair centers are very suitable for studying cooperative effects of RE ions. These include processes between the ions of the pair as well as processes between the coupled pair and the electronic excitations of the host lattice. Experiments will be shown and discussed on: (i) cross relaxation and up-conversion by direct ion-ion interaction; (ii) cooperative cross relaxation of the Pr3+ pairs with the host lattice; and (iii) cooperative vibronic emission of the Pr3+ pairs with high phonon progressions.

DOI
10.1117/12.475336

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In CsCdBr3 the trivalent Rare-Earth (RE) ions substitute for the divalent Cd ions. For reasons of charge compensation and the specific crystal structure, RE centers of the form RE3+ - (Cd vacancy) - RE3+ are preferentially formed. These symmetric pair centers are very suitable for studying cooperative effects of RE ions. These include processes between the ions of the pair as well as processes between the coupled pair and the electronic excitations of the host lattice. Experiments will be shown and discussed on: (i) cross relaxation and up-conversion by direct ion-ion interaction; (ii) cooperative cross relaxation of the Pr3+ pairs with the host lattice; and (iii) cooperative vibronic emission of the Pr3+ pairs with high phonon progressions.
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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.
Electron paramagnetic resonance spectra of Yb 3+ ions in the optically bistable compound Yb:CsCdBr 3 are presented. The features observed are assigned to the symmetrically coupled pair complexes of the type Yb 3+ -V Cd -Yb 3+ (V Cd being a cadmium vacancy) whose axis is parallel to the crystallographic c -axis. There are no asymmetric pairs of the type Yb 3+ -Yb 3+ -V Cd . It is shown that simulation of the spectra is possible only if an exchange interaction is taken into account in the spin Hamiltonian. The value of J = -0.0016 cm -1 shows that the exchange interaction is antiferromagnetic but extremely weak. It is also found that there is a significant relaxation (about 12%) of Yb 3+ ions toward the Cd vacancy. From the experimental g -tensor values, it is established that the lower ground state of Yb 3+ ions in CsCdBr 3 is mainly composed of 4f ϕ (63%) and 4f δ (32%) ytterbium orbitals. It has been previously proposed that optical bistability is due to asymmetric pairs of the type Yb 3+ -Yb 3+ -V Cd . On the basis of the present work, this now appears unlikely.
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.
Rare-Earth (RE) atoms possess a unique atomic energy level structure, leading to excellent electronic and spin coherence properties [1]. Consequently, RE-ion-doped materials are promising candidates for implementing light-matter interfaces for photonic quantum technologies, such as quantum memories. To exploit these properties in quantum technologies, the REs must be hosted in a solid-state material [1]. RE organic molecular crystals offer advantages over the well-known RE-doped inorganic crystals. In organic molecular crystals, RE ions are integral parts of the molecular structure, unlike in inorganic crystals, in which the RE ions are distributed randomly into the crystal lattice structure. This can potentially lead to narrower inhomogeneous broadening. These crystals provide unmatched flexibility in combining with photonic structures and in material composition, allowing the choice of different ligands and point group symmetries around the RE ion [2], [10], [4]. Our research focuses on crystals formed from a molecular complex hosting erbium ions⌈Er(C5H7O2)3(C12H8N2)⌉\lceil{E}r(C_{5}H_{7}O_{2})_{3}(C_{12}H_{8}N_{2})\rceil⌈Er(C5​H7​O2​)3​(C12​H8​N2​)⌉. As these crystals have not yet been studied for quantum information purposes, we conducted a series of optical spectroscopy measurements to characterize the platform. We performed absorption measurements and obtained the absorption profiles at room and cryogenic temperatures. The results show a narrow inhomogeneous broadening in samples with different relative concentrations, even at 100%, for which all molecules contain an erbium ion. We measured the lifetime of the second lowest crystal field level of the ground state manifold(30 cm−1(\boldsymbol{30}\ cm^{-1}(30 cm−1above ground state) to be 1.759 seconds. Additionally, we measured the inhomogeneous broadening of the lowest crystal field level versus temperature to investigate the effects of phonon processes. Finally, under an external magnetic field, we observed Zeeman splitting and determined the g-factor to be 3.23 for erbium ions in this molecular complex.