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Journal of the Optical Society of America B

Pr^3+ cluster management in CaF_2 by codoping with Lu^3+ or Yb^3+ for visible lasers and quantum down-converters

Diana Serrano, Alain Braud, J.L. Doualan, Patrice Camy, R. Moncorgé

Published Jul 3, 2012• 30 citations
Publisher

Abstract

The codoping of CaF2:Pr3+ with Yb3+ or Lu3+ ions is shown to avoid the clustering of Pr3+ ions, which otherwise prevent Pr3+ doped CaF2 to be used for various photonic applications. The breaking of Pr3+ clusters by Lu3+ ions paves the way towards the development of a Pr3+ doped CaF2 visible laser. On the other hand, the formation of Pr3+-Yb3+ clusters in place of Pr3+ clusters leads to extremely efficient energy transfers between Pr3+ and Yb3+ which could be used for quantum cutting applications. Two types of clusters are observed for both types of codopings. Pr3+ to Yb3+ energy transfer analysis shows that for one of the clusters an ultrafast energy transfer takes place with a rate of 5×107 s−1, which is likely due to exchange interaction.

DOI
10.1364/josab.29.001854

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The codoping of CaF2:Pr3+ with Yb3+ or Lu3+ ions is shown to avoid the clustering of Pr3+ ions, which otherwise prevent Pr3+ doped CaF2 to be used for various photonic applications. The breaking of Pr3+ clusters by Lu3+ ions paves the way towards the development of a Pr3+ doped CaF2 visible laser. On the other hand, the formation of Pr3+-Yb3+ clusters in place of Pr3+ clusters leads to extremely efficient energy transfers between Pr3+ and Yb3+ which could be used for quantum cutting applications. Two types of clusters are observed for both types of codopings. Pr3+ to Yb3+ energy transfer analysis shows that for one of the clusters an ultrafast energy transfer takes place with a rate of 5×107 s−1, which is likely due to exchange interaction.
The deposition of a thin layer of a quantum-cutter material on top of silicon-based solar cells seems to be a promising solution to reduce the thermalization losses. This mechanism has been reported in materials codoped with Pr3+-Yb3+, where Pr3+ can sensitize two Yb3+ ions for one absorbed blue photon. In the present Letter, we analyze precisely energy transfers between Pr3+ and Yb3+ in CaYAlO4, and we measure a quantum-cutting rate of 145%. We show that a very efficient back transfer from Yb3+ toward the (1)G4 level of Pr3+ ion leads to a strong reduction of the quantum yield.
Abstract Quantum cutting (QC) is a process that can split one high-energy photon into two or more low-energy photons.1-4 As an attractive mechanism, it has been extensively explored for acquiring high quantum efficiency (QE) of more than 100%.5-8 Here, we report the first experimental observation of multiphoton QC with ultrahigh QEs in CaF2:Yb polycrystalline. Under 266 nm excitation, an internal quantum efficiency as high as ~285% was achieved, indicating that one ultraviolet (UV) photon was split into more than two ~1000 nm near infrared (NIR) photons. Photovoltaic experiments demonstrated that the polycrystalline increased the output power of a polycrystalline silicon solar cell by more than 200% in the case of 266 nm irradiation. Spectral analysis confirmed that the ultrahigh QE originated from efficient cooperative absorptions of Yb-tetramers and Yb-trimers and individual emission of single Yb3+ ions. This study provides a promising approach for improving spectral response of silicon solar cells and detectors in the UV region.
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.