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Preparation, Purification, and Characterization of Lanthanide Complexes for Use as Contrast Agents for Magnetic Resonance Imaging
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Tuning a Lanthanide Complex To Be Responsive to the Environment in Solution.

Ryan T Golkowski1, Nicholas S Settineri1, Xikang Zhao1

  • 1Department of Chemistry, 560 Oval Drive, Purdue University , West Lafayette, Indiana 47907-2084, United States.

The Journal of Physical Chemistry. A
|November 17, 2015
PubMed
Summary

Lanthanide complexes with a pyrrolidinyl substituent show tunable emission. The terbium complex exhibits unique f-f emission sensitive to its environment and oxygen.

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Area of Science:

  • Coordination Chemistry
  • Photophysics
  • Materials Science

Background:

  • Lanthanide ion complexes are known for predictable f-f emissions, crucial for applications.
  • However, their emissive states are typically insensitive to environmental factors.

Purpose of the Study:

  • To investigate ligand- and metal-centered emission in mixed-ligand lanthanide complexes.
  • To explore the impact of a pyrrolidinyl substituent on excited state properties and emission behavior.

Main Methods:

  • Synthesis of mixed-ligand complexes M(X-T)(NO3)3 (M = Eu, Gd, Tb, Lu; X-T = H-T, Ph-T, pyrr-T).
  • Characterization of photophysical properties, including fluorescence and phosphorescence quantum yields.
  • Analysis of excited state dynamics and environmental sensitivity.

Main Results:

  • The pyrrolidinyl substituent induces intraligand charge-transfer (ILCT) character and reduces the singlet-triplet energy gap.
  • Lutetium complex shows low fluorescence (0.15%), while gadolinium complex exhibits high phosphorescence (9.6%).
  • The terbium complex displays environmentally sensitive f-f emission due to ILCT state equilibration.

Conclusions:

  • Substituent engineering on terpyridine ligands offers a route to tune lanthanide complex photophysics.
  • The Tb(pyrr-T)(NO3)3 complex demonstrates a novel system with environment- and oxygen-sensitive f-f emission.
  • This sensitivity opens possibilities for new sensor applications.