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Orthogonal excitation polarization dictated by site symmetry in upconversion luminescence of microrods
Phys. Rev. B 114, 165403 – Published 2 September, 2026
DOI: https://doi.org/10.1103/l7qg-hm2p
Abstract
Elucidating the site symmetry of lanthanide dopants in micro/nanocrystals is essential for a comprehensive understanding of upconversion luminescence (UCL). Here, we report an excitation-wavelength-dependent polarization response in individual -doped microrods, where the degree of excitation polarization is tunable from 0 to 1 and the polarization orientation can be rotated by π/2. Further investigations reveal that subsequent excited-state absorption inherits the polarization orientation established by the initial ground-state absorption, with the degree of excitation polarization increasing as more excited-state absorption steps are involved in the upconversion process. Based on the Stark emission peaks of the multiplet, polarization-verified crystal field calculations indicate that occupies spectroscopic sites with approximately symmetry in the host. By assigning irreducible representations to all Stark levels, we establish a correlation between the macroscopic polarized UCL properties of and its local symmetry in a lattice via point-group selection rules. Our work provides valuable insights into the polarization origins of UCL, offering an approach to optimize upconversion and realize diverse applications in polarized photonics.