Spectroscopic study of cooperative states of Nd3+ pair centers in fluorite-type crystals: A competition of dipole-dipole and quadrupole-quadrupole energy exchange

Abstract

Pair centers of Nd3+ ions in the CdF2, CaF2, and SrF2 doped crystals at T=6.5K were studied under tunable narrow-linewidth laser excitation. It has been established that the exchange of electronic excitation leads to the splitting of the one-exciton cooperative 4G5/2(1) x 4I9/2(1) state by 2–3 cm−1 with a non-monotonic dependence on the distance between the ions in the pairs in these crystals. This dependence is explained by the competition of forced dipole-dipole and quadrupole-quadrupole interactions with spin flip. The high rate of such exchange mechanisms is due to strong spin–orbit interaction and small energy difference between the 4f levels of Nd3+ ions. It is shown that the pair centers in all one-exciton cooperative states, in contrast to the ground and two-exciton excited states, have nonzero static dipole moments. This makes it possible to use the latter states as ultrafast qubits, and one-exciton states as control qubit to implement a CNOT quantum gate.