Abstract
We report high-resolution x-ray Raman scattering studies of high-order multipole spectra of rare earth excitations (the absorption edge) in nanoparticles of the phosphates LaPO4, CePO4, PrPO4, and NdPO4. We also present corresponding data for La excitations (the edge) in LaPO4. The results are compared with those from calculations by atomic multiplet theory and for the dipole contribution to the La transition from a calculation using time-dependent density functional theory (TDLDA). Agreement with the atomic multiplet calculations for the high-order multiplet spectra is remarkable in the case of the spectra. In contrast, we find that the shallow semicore excitations in LaPO4 manifest a relatively broad band and an apparent quenching of spin-orbit splitting. The more sophisticated TDLDA, which has earlier been found to explain dipolar spectra well in Ba compounds, is less satisfactory here in the case of La.
Highlights
Electronic properties of materials are of fundamental interest, as it is well known that understanding electronic properties gives the possibility to tailor the physical, chemical, and biological properties of matter
Interesting phenomena are still being found in atomic spectra, and for example recently it was reported [1] that electron correlation in lanthanide systems coupled to the different radiative and non-radiative decay channels causes a deformation of the inner-shell spectral profiles from a pure Lorentzian in x-ray absorption spectroscopy (XAS) measurements
A peculiar aspect found in rare earth atomic spectra is the giant dipole resonance (GDR) [2] that prevails in the XAS spectra of, e.g., 4d → 4f excitations
Summary
We report high-resolution x-ray Raman scattering studies of high-order multipole spectra of rare author(s) and the title of the work, journal citation earth 4d → 4f excitations (the N4,5 absorption edge) in nanoparticles of the phosphates LaPO4, and DOI. We present corresponding data for La 5p → 5d excitations (the O2,3 edge) in LaPO4. Agreement with the atomic multiplet calculations for the highorder multiplet spectra is remarkable in the case of the N4,5 spectra. We find that the shallow O2,3 semicore excitations in LaPO4 manifest a relatively broad band and an apparent quenching of 5p spin-orbit splitting. The more sophisticated TDLDA, which has earlier been found to explain dipolar spectra well in Ba compounds, is less satisfactory here in the case of La
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