Beyond the energy gap law: the influence of selection rules and host compound effects on nonradiative transition rates in boltzmann thermometers

Philip Netzsch, Matthias Hämmer, Erich Turgunbajew, Thomas P. van Swieten, Andries Meijerink*, Henning A. Höppe*, Markus Suta*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

11 Citations (Scopus)

Abstract

Apart from the energy gap law, control parameters over nonradiative transitions are so far only scarcely regarded. In this work, the impact of both covalence of the lanthanoid–ligand bond and varying bond distance on the magnitude of the intrinsic nonradiative decay rate between the excited 6P5/2 and 6P7/2 spin–orbit levels of Gd3+ is investigated in the chemically related compounds Y2[B2(SO4)6] and LaBO3. Analysis of the temperature-dependent luminescence spectra reveals that the intrinsic nonradiative transition rates between the excited 6PJ (  J = 5/2, 7/2) levels are of the order of only 10 ms−1 (Y2[B2(SO4)6]:Gd3+: 8.9 ms−1; LaBO3:Gd3+: 10.5 ms−1) and differ due to the different degree of covalence of the Gd—O bonds in the two compounds. Comparison to the established luminescent Boltzmann thermometer Er3+ reveals, however, that the nonradiative transition rates between the excited levels of Gd3+ are over three orders of magnitude slower despite a similar energy gap and the presence of a single resonant phonon mode. This hints to a fundamental magnetic dipolar character of the nonradiative coupling in Gd3+. These findings can pave a way to control nonradiative transition rates and how to tune the dynamic range of luminescent Boltzmann thermometers.
Original languageEnglish
Article number2200059
Number of pages9
JournalAdvanced Optical Materials
Volume10
Issue number11
Early online date7 Apr 2022
DOIs
Publication statusPublished - 3 Jun 2022

Keywords

  • Borates
  • Borosulfates
  • Gd3+
  • Luminescence thermometry
  • Nonradiative transitions
  • Structure–property relationship

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