One- and two-exciton states of pair centers of Kramers Nd3+ions in Nd-doped CaF2 and SrF2 crystals, and their possible use as qubits

Using two-color excitation with narrow laser lines of 0.2 cm−1 and time-resolved site-selective fluorescence spectroscopy, we measured the fluorescence excitation spectra of the one-exciton 4G5/2(1) x 4I9/2(1) state monitored in the near IR, and the two-exciton 4G5/2(1) x 4G5/2(1) state monitored in the near UV of the pair M centers in the Nd3+ doped CaF2 and SrF2 crystals at 6.5 K. We observed the splitting of the one-exciton state of the order of 2–3 cm−1 depending on the type of crystal matrix. A significant inhomogeneous splitting ∼1.5 cm−1 of the spectral lines of the one-exciton state of the pair M centers in the Nd3+: SrF2 crystals was found. The measured single spectral line of the two-exciton state of the pair M centers in these crystals has in one-photon scale the linewidth of ∼0.8 cm−1, which is mainly determined by inhomogeneous broadening.