Magneto-Photoluminescence Based on Two-Photon Excitation in Lanthanide-Doped Up-Conversion Crystal Particles

Experimental studies on magneto-photoluminescence based on two-photon excitation in up-conversion Y₂ O₂ S:Er, Yb crystal particles are reported. It is found that the up-conversion photoluminescence generated by two-photon excitation exhibits magnetic field effects at room temperature, leading to a two-photon excitation-induced magneto-photoluminescence, when the two-photon excitation exceeds the critical intensity. By considering the spin selection rule in electronic transitions, it is proposed that spin-antiparallel and spin-parallel transition dipoles with spin mixing are accountable for the observed magneto-photoluminescence. Specifically, the two-photon excitation generates spin-antiparallel electric dipoles between ⁴ S_3/2 -⁴ I_15/2 in Er³⁺ ions. The antiparallel spins are conserved by exchange interaction within dipoles. When the photoexcitation exceeds the critical intensity, the Coulomb screening can decrease the exchange interaction. Consequently, the spin-orbital coupling can partially convert the antiparallel dipoles into parallel dipoles, generating a spin mixing. Eventually, the populations between antiparallel and parallel dipoles reach an equilibrium established by the competition between exchange interaction and spin-orbital coupling. Applying a magnetic field can break the equilibrium by disturbing spin mixing through introducing spin precessions, changing the spin populations on antiparallel and parallel dipoles and leading to the magneto-photoluminescence. Therefore, spin-dependent transition dipoles present a convenient mechanism to realize magneto-photoluminescence in multiphoton up-conversion crystal particles.