Selective laser spectroscopy of Mn4+-Mn4+ pair centers in SrTiO3 crystal

Zero-phonon lines of a pair center of Mn⁴⁺ ions are observed in the luminescence and luminescence-excitation spectra of SrTiO₃:Mn crystal. Based on the experimental data, the energy-level structure of the ground state ∣⁴ A _2g ,⁴ A _2g 〉 and excited state ∣⁴ A _2g ,² E _g 〉 of the Mn⁴⁺-Mn⁴⁺ pair center is constructed. It is shown that the exchange interaction in the ground state of the Mn⁴⁺-Mn⁴⁺ pair is antiferromagnetic. Energies of the levels are calculated assuming that the pair is formed by Mn⁴⁺ ions occupying neighboring octahedral positions of Ti⁴⁺ ions along the 110] axis. Experimental values of the exchange integral in the ground state ∣⁴ A _2g ,⁴ A _2g 〉 and energies of spin multiplets in the excited state ∣⁴ A _2g ,² E _g 〉 agree well with calculation of the exchange interaction carried out within the framework of the channel model with the parameters J _ξη = 32 cm^4-1 and J _ζζ = ?45.5 cm^4-1. Experimental data and calculations unambiguously demonstrate that zero-phonon lines in the luminescence and luminescence-excitation spectra have magnetic-dipole nature.