Symmetry and light coupling to phononic and collective magnetic excitations in SrCu_2(BO_3)_2

TL;DR

This study uses low temperature Raman scattering to explore symmetry, magnetic excitations, and spin-phonon interactions in SrCu_2(BO_3)_2, revealing insights into magnetic states, coupling mechanisms, and the effects of external magnetic fields.

Contribution

It introduces a minimal 4-spin cluster model to explain magnetic mode symmetries and anisotropic dispersions, and identifies two Raman coupling mechanisms including an intra-dimer Dzyaloshinskii-Moriya interaction.

Findings

Identification of symmetry and behavior of magnetic triplet states in magnetic fields

Discovery of two Raman coupling mechanisms affecting magnetic modes

Evidence of strong spin-phonon coupling and mode quasi-degeneracy

Abstract

We perform a low temperature Raman scattering study of phononic and collective spin excitations in the orthogonal dimers compound SrCu_2(BO_3)_2, focussing 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 intra-dimer 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 quasi-degeneracy of modes in the context of the present crystal structure determination.