Far-infrared spectroscopy of spin excitations and Dzyaloshinskii-Moriya interactions in a Shastry-Sutherland compound SrCu${}_2$(BO${}_3$)$_2

Abstract

We have studied spin excitation spectra in the Shastry-Sutherland model compound SrCu${}_2$(BO${}_3$)${}_2$ in magnetic fields using far-infrared Fourier spectroscopy. The transitions from the ground singlet state to the triplet state at 24 cm${}^{-1}$ and to several bound triplet states are induced by the electric field component of the far-infrared light. To explain the light absorption in the spin system we invoke a dynamic Dzyaloshinskii-Moriya (DM) mechanism where light couples to a phonon mode, allowing the DM interaction. Two optical phonons couple light to the singlet to triplet transition in SrCu${}_2$(BO${}_3$)${}_2$. One is $a$-polarized and creates an intra-dimer dynamic DM along the c axis. The other is $c$-polarized and creates an intra-dimer dynamic DM interaction, it is in the $(ab)$ plane and perpendicular to the dimer axis. Singlet levels at 21.5 and 28.6 cm${}^{-1}$ anti-cross with the first triplet as is seen in far-infrared spectra. We used a cluster of two dimers with a periodic boundary condition to perform a model calculation with scaled intra- and inter-dimer exchange interactions. Two static DM interactions are sufficient to describe the observed triplet state spectra. The static inter-dimer DM in the c-direction $d_1=0.7$ cm${}^{-1}$ splits the triplet state sub-levels in zero field [Cépas et al., Phys. Rev. Lett. \textbf{87}, 167205 (2001)]. The static intra-dimer DM in the $(ab)$ plane (perpendicular to the dimer axis) $d_2=1.8$ cm${}^{-1}$, allowed by the buckling of CuBO${}_3$ planes, couples the triplet state to the 28.6 cm${}^{-1}$ singlet as is seen from the avoided crossing.

12 pages with 7 figures, some references corrected