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Waetzig GR, Horrocks GA, Jude JW, et al. Ligand-Mediated Control of Dopant Oxidation State and X-ray Excited Optical Luminescence in Eu-Doped LaOCl. Inorg Chem. 2018;57(10):5842-5849doi: 10.1021/acs.inorgchem.8b00234.
Waetzig, G. R., Horrocks, G. A., Jude, J. W., Villalpando, G. V., Zuin, L., & Banerjee, S. (2018). Ligand-Mediated Control of Dopant Oxidation State and X-ray Excited Optical Luminescence in Eu-Doped LaOCl. Inorganic chemistry, 57(10), 5842-5849. https://doi.org/10.1021/acs.inorgchem.8b00234
Waetzig, Gregory R, et al. "Ligand-Mediated Control of Dopant Oxidation State and X-ray Excited Optical Luminescence in Eu-Doped LaOCl." Inorganic chemistry vol. 57,10 (2018): 5842-5849. doi: https://doi.org/10.1021/acs.inorgchem.8b00234
Waetzig GR, Horrocks GA, Jude JW, Villalpando GV, Zuin L, Banerjee S. Ligand-Mediated Control of Dopant Oxidation State and X-ray Excited Optical Luminescence in Eu-Doped LaOCl. Inorg Chem. 2018 May 21;57(10):5842-5849. doi: 10.1021/acs.inorgchem.8b00234. Epub 2018 May 10. PMID: 29746109.
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Inorg Chem. 2018 May 21;57(10):5842-5849. doi: 10.1021/acs.inorgchem.8b00234. Epub 2018 May 10.

Ligand-Mediated Control of Dopant Oxidation State and X-ray Excited Optical Luminescence in Eu-Doped LaOCl.

Inorganic chemistry

Gregory R Waetzig, Gregory A Horrocks, Joshua W Jude, Graciela V Villalpando, Lucia Zuin, Sarbajit Banerjee

Affiliations

  1. Department of Chemistry and Department of Materials Science and Engineering , Texas A&M University , College Station , Texas 77845-3012 , United States.
  2. Canadian Light Source , University of Saskatchewan , Saskatoon , Canada.

PMID: 29746109 DOI: 10.1021/acs.inorgchem.8b00234

Abstract

The development of an expanded palette of X-ray phosphors is a critical imperative for applications in medical imaging, radiation detection, and scientific instrumentation. The rational design of X-ray phosphors has been stymied by the absence of fundamental understanding of activation channels, sensitization mechanisms, and recombination pathways induced upon high-energy excitation of luminescent centers. In this article, we describe the preparation of Eu-doped LaOCl nanocrystals based on the condensation of molecular precursors. The synthetic route allows for control of the oxidation state of the incorporated Eu-atoms based on ligand-induced oxidation or reduction of the Eu-precursors. Nanocrystals exhibiting blue and red X-ray excited optical luminescence are developed by tuning the oxidation state of europium ions incorporated within the LaOCl nanocrystal matrix. Pronounced modulation of the intensity of the optical luminescence is evidenced at and near the giant resonance absorption of the host matrix as a result of distinctly divergent recombination channels. Resonant excitation results in recombination via Auger electron ionization and relaxation of a single electron-hole pair, whereas excitation away from the giant resonance results in thermalization of "hot" electron-hole pairs, while launching cascades of energy transfer, excitation, and radiative recombination events at the Eu-luminescent centers. Mechanistic elucidation and the development of a generalizable synthetic route starting from molecular precursors paves the way to an expanded palette of X-ray phosphors.

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