Symmetry and light coupling to phononic and collective magnetic excitations in SrCu2„BO3...2

We perform a low temperature Raman scattering study of phononic and collective spin excitations in the orthogonal dimers compound SrCu2!BO3"2, focusing on the symmetry and the effects of external fields on the magnetic modes. The zero field symmetry and the behavior in magnetic fields of the elementary and bound magnetic triplet states are experimentally determined. We find that a minimal 4-spin cluster forming the unit cell is able to describe the symmetry as well as the anisotropic dispersions in external fields of the spin gap multiplet branches around 24 cm−1. We identify two Raman coupling mechanisms responsible for the distinct resonance behavior of these magnetic modes and we show that one of these can be ascribed to an effective intradimer Dzyaloshinskii-Moriya spin interaction. Our data also suggest a possible explanation for the existence of a strongly bound two-triplet state in the singlet sector which has an energy below the spin gap. The low temperature phononic spectra suggest strong spin-phonon coupling and show intriguing quasidegeneracy of modes in the context of the present crystal structure determination.