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Single-Determinant Ground State in Ce4+ Imidophosphorane Complexes.

Haruko Tateyama1, Can Liao2, Grant R Wilkinson1

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|December 11, 2025
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Analyzing high-valent lanthanides with X-ray spectroscopy is crucial. For cerium (Ce4+) complexes, the complex L3-edge features arise from excited-state behavior, not ground-state ligand field effects.

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Area of Science:

  • Materials Science
  • Quantum Chemistry
  • Spectroscopy

Background:

  • X-ray spectroscopy is vital for understanding high-valent lanthanide electronic structures.
  • Interpreting multipeaked features at the lanthanide L3-edge is challenging across material classes.
  • Ligand field perturbations are often considered for ground-state electronic structure.

Purpose of the Study:

  • To investigate the origin of multipeaked features at the Ce L3-edge in tetravalent cerium complexes.
  • To determine if ligand field perturbation influences the ground state electronic structure.
  • To elucidate the electronic behavior responsible for observed spectral features.

Main Methods:

  • Synthesis of structurally related Ce4+ imidophosphorane complexes.
  • UV-vis spectroscopy and electrochemistry to tune and verify electronic properties.
  • High-energy resolution fluorescence-detected X-ray absorption near-edge structure (HERFD-XANES) spectroscopy.
  • Resonant inelastic X-ray scattering (RIXS) to visualize spectral features.
  • Large complete active space configuration interaction singles and doubles (CASCISD) calculations.

Main Results:

  • Ligand derivatization successfully tuned electronic properties, confirmed by spectroscopy and electrochemistry.
  • Ce L3-edge HERFD-XANES spectra showed consistent features across all complexes, irrespective of ligand variation.
  • RIXS confirmed the visualization of observed features in HERFD-XANES spectra.
  • CASCISD calculations indicated that the ground state of all complexes is well-described by a single determinant wave function.

Conclusions:

  • The multipeaked feature at the Ce L3-edge is attributed to excited-state multiconfigurational behavior.
  • This behavior is independent of ligand variation in these Ce4+ imidophosphorane complexes.
  • The findings clarify the interpretation of L3-edge XANES spectra for high-valent lanthanides, distinguishing excited-state from ground-state effects.