Optical Spectrum ofCr3+Pairs in LaAlO3

Abstract
The optical spectrum and exchange splittings of the nearest-neighbor Cr3+ pairs in LaAlO3 have been studied. The absorption and emission spectra of the A24A24E2A24 pair transitions from 7200 to 7600 Å yield the ground-state exchange Jab(Sa·Sb)+j(Sa·Sb)2 with Jab=66.6 cm1 and j=0.76 cm1. The emission lines were studied as a function of uniaxial stress applied along the trigonal axis. The stress dependences of the pair lines are not very different from the single-ion shifts. The energy levels of the E2A24 and E2E2 pair states have also been determined. The latter corresponds to exciting both ions to the E2 state, and the absorption is in the ultraviolet at about twice the E2 single-ion energy. The excited-state splittings are compared with the values calculated from Hex=ΣJijSi·sj, where the sums are over the electronic spins Si and Sj of the Cr3+t2g orbitals and the Jij are empirical parameters. For the E2A24 levels we find that J11=531.1 cm1 and 12(J12+J21)=55.4 cm1 are the dominant exchange parameters. The signs and relative magnitudes agree with Anderson's theory. The pair lines have electric dipole polarization, and the strongest transitions obey the selection rule ΔS=0, ΔMs=0. The polarization agrees with the calculated selection rules of the exchange-induced spin-dependent dipole moment P=ΣPijSi·Sj.