Interpretation of europium(III) spectra

Spectroscopic properties and design of highly luminescent lanthanide coordination complexes

The optical spectra of the lanthanides doped into single crystal LaF3 have been interpreted in terms of transitions within 4f N configurations. Energy matrices combining free‐ion terms with a crystal field for an approximate model which assumes C2v instead of the actual C2 site symmetry were diagonalized. Excellent correlations were obtained between experimental transition energies and the computed level structures. We also report the results of previously unpublished experimental spectroscopic investigations of Nd3+ and Sm3+:LaF3, as well as predicted energy levels for Pm3+:LaF3. The spectroscopic data for each ion were independently interpreted using an effective‐operator model, then the model parameters were intercompared. Systematic trends have been identified, and a comprehensive energy level diagram is presented.

/pdf/a-systematic-analysis-of-the-spectra-of-the-lanthanides-1ozi0k3sof.pdf

A systematic analysis of the spectra of the lanthanides doped into single crystal LaF3

Present technological demands in disparate areas, such as microfluidics and nanofluidics, microelectronics and nanoelectronics, photonics and biomedicine, among others, have reached to a development such that conventional contact thermal probes are not accomplished anymore to perform accurate measurements with submicrometric spatial resolution. The development of novel noncontact thermal probes is, then, mandatory, contributing to an expansionary epoch of luminescence thermometry. Luminescence thermometry based on trivalent lanthanide ions has become very popular since 2010 due to the unique versatility, stability, and narrow emission band profiles of the ions that cover the entire electromagnetic spectrum with relatively high emission quantum yields. Here, a perspective overview on the field is given from the beginnings in the 1950s until the most recent cutting‐edge examples. The current movement toward usage of the technique as a new tool for thermal imaging, early tumor detection, and as a tool for unveiling the properties of the thermometers themselves or of their local neighborhoods is also summarized.

Lanthanide-based thermometers: At the cutting-edge of luminescence thermometry

Lanthanide-doped inorganic nanoparticles possess superior physicochemical features such as long-lived luminescence, large antenna-generated Stokes or anti-Stokes shifts, narrow emission bands, high resistance to photobleaching and low toxicity, and thus are regarded as a new generation of luminescent bioprobes as compared to conventional molecular probes like organic dyes and lanthanide chelates. These functional nanoparticles, although most of their bulk counterparts were well studied previously, have attracted renewed interest for their biomedical applications in areas as diverse as biodetection, bioimaging, and disease diagnosis and therapeutics. In this review, we provide a comprehensive survey of the latest advances made in developing lanthanide-doped inorganic nanoparticles as potential luminescent bioprobes, which covers areas from their fundamental chemical and physical features to bioapplications including controlled synthesis methodology, surface modification chemistry, optical spectroscopy, and their promising applications in diverse fields, with an emphasis on heterogeneous and homogeneous in vitro biodetection of tumor markers and multimodal bioimaging of various tumor tissues. Some future prospects and challenges in this rapidly growing field are also summarized.

Lanthanide-doped luminescent nanoprobes: controlled synthesis, optical spectroscopy, and bioapplications.

Two types of correlations with experimental results are reported. For even-f-electron systems, a center of gravity was computed based on the energies of the observed states, and calculated optimized sets of atomic energy level parameters. For odd-electron systems complete crystal field calculations were performed in which parameters of both the atomic and crystal-field parts of the interaction were adjusted to experimental data. The result is a set of eigenvectors for all the ionic states in each configuration. Spectroscopic results for all lanthanides doped into LaF3 (In³⁺ +/:LaF3) except Pm³⁺ and Eu³⁺ are reported.

/pdf/energy-level-structure-and-transition-probabilities-in-the-gjmbal6l70.pdf

Energy level structure and transition probabilities in the spectra of the trivalent lanthanides in LaF

A parametric model for lanthanide and actinide atomic and crystal energy levels is presented that correlates trends in Hartree–Fock calculations with empirically determined atomic parameters in such a way that predictions for unclassified complex cases can be made from the analysis of simpler ones. When appropriate effective operators, including electrostatic operators up to the third rank for fN configurations and magnetic operators up to the second rank for fN and fNd shells, are used in the parametric Hamiltonian, statistical errors of 10–20 cm−1 are typical for the simpler examples presented.

Parametric model for f-shell configurations. I. The effective-opertor Hamiltonian

New measurements of the optical spectrum of trivalent neodymium in a hexagonal lanthanum chloride host have been made at 4 and 77 K at wavelengths down to 2500 A (40 000 cm−1). Crystal quantum number assignments for new energy levels were derived from these results and for most of the earlier levels not already classified. A least‐squares fit with a mean error of 8.1 cm−1 was carried out for 101 levels, using 20 adjustable parameters in a Hamiltonian containing operators for two‐ and three‐particle electrostatic interactions; spin–orbit, spin–other‐orbit and spin–spin magnetic interactions; two‐particle pseudomagnetic configuration‐mixing interactions; and single‐particle crystal‐field interactions.

The spectrum of Nd3+:LaCl3

The spectrum of U3+:LaCl3 has been analyzed; 53 crystal states of electronic origin have been identified, many of them accompanied by extensive vibronic sidebands having a recognizable structure similar to that for lanthanide‐doped LaCl3. Seventeen energy level parameters were varied simultaneously in a least‐squares adjustment yielding a mean error of 26 cm−1. Values for the crystal field parameters are: B20=260±64 cm−1, B40=−532±139 cm−1, B60=−1438±113 cm−1 and B66=1025±88 cm−1.

Spectrum analysis of U3+:LaCl3

The polarized absorption and fluorescence spectra of 0.01–5% Np3+ doped into single‐crystal LaCl3 were measured at moderate and high resolution in the range to 50 000 cm−1 at 298, 77, and 4 K. The 150 crystal field components identified were fit by a parametrized model which has previously been shown to provide an excellent account of the energy level structures observed for lanthanides doped into LaCl3. This constitutes the first successful evaluation of the crystal field interaction for an actinide ion in LaCl3 in which J mixing effects were explicitly included. The crystal field parameters for Np3+:LaCl3, B20=163, B40=−632, B60=−1625, and B66=1028, all in cm−1, were determined to be approximately twice as large as those for the analogous lanthanide, Pm3+:LaCl3. From analysis of Zeeman patterns in the fluorescence spectra, the ground state was found to be doubly degenerate, having crystal quantum numbers ±2 and a parallel splitting factor 0.17 LU (Lorentz unit).

Energy level analysis of Np3+:LaCl3 and Np3+:LaBr3

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