Influence of Dy 3+ and Tb 3+ doping on 13 C dynamic nuclear polarization

Niedbalski, Peter; Parish, Christopher  (ORCID:0000000223546298); Kiswandhi, Andhika; Fidelino, Leila; Khemtong, Chalermchai; Hayati, Zahra; Song, Likai; Martins, André; Sherry, A. Dean; Lumata, Lloyd

doi:10.1063/1.4973317

Erbium lanthanum titanate glasses were prepared by levitation melting for the spectroscopic study of ways to promote the mid-infrared fluorescence. Two series of heavily erbium doped glasses (15 wt%) were prepared with the addition of either Pr³⁺or Nd³⁺in amounts relative to Er³⁺of 0.05, 0.1, and 0.2. Both ions quench the lower Er³⁺laser level with the Pr³⁺doing so more rapidly. Although high co-dopant concentrations result in higher energy transfer, as clearly evidenced in upconversion and downconversion fluorescence measurements, the mid-infrared lifetime also suffers a reduction and, therefore, a balance must be struck in the co-dopant concentration. Lifetime and spectral measurements indicate that, at a fixed relative co-dopant amount, Pr³⁺is more effective than Nd³⁺at removing the bottleneck of the Er³⁺ ⁴I_13/2level. Moreover, consideration of the lifetimes alongside the absorption data of the individual ions indicates that despite the large absorption cross-section of Nd³⁺at 808 nm, the concentration needed to yield more absorbed power than utilizing direct 976 nm excitation of Er³⁺results in unfavorable lifetimes of the mid-infrared transition. In the end, Pr³⁺prevails as the superior co-dopant in terms of the effects on fluorescence lifetimes as well as potential laser system design considerations. In a unique self-doping approach, a reducing melt atmosphere of Ar instead of O₂creates a small fraction of Ti³⁺. In 5Er₂O₃-12La₂O₃-83TiO₂glass, the presence of Ti³⁺quenches the⁴I_13/2emission about 2.6 times more than the⁴I_11/2when lifetimes are compared to an O₂melt environment. As an additional means of increasing the mid-infrared emission, the effect of temperature on the mid- and near- infrared lifetimes of a lightly doped lanthanum titanate composition is investigated between 77-300 K. The mid-infrared lifetime increases by ∼30% while the near-infrared lifetime increases by ∼10%, which suggests in addition to co-doping, active cooling of the gain media will further enhance performance.

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