Novel Strongly Spin-Orbit Coupled Quantum Dimer Magnet: Yb${}_2$Si${}_2$O${}_7$

Abstract

The quantum dimer magnet (QDM) is the canonical example of quantum magnetism. The QDM state consists of entangled nearest-neighbor spin dimers and often exhibits a field-induced triplon Bose-Einstein condensate (BEC) phase. We report on a new QDM in the strongly spin-orbit coupled, distorted honeycomb-lattice material Yb${}_2$Si${}_2$O${}_7$. Our single crystal neutron scattering, specific heat, and ultrasound velocity measurements reveal a gapped singlet ground state at zero field with sharp, dispersive excitations. We find a field-induced magnetically ordered phase reminiscent of a BEC phase, with exceptionally low critical fields of $H_{c1}\sim 0.4$ T and $H_{c2}\sim 1.4$ T. Using inelastic neutron scattering in an applied magnetic field we observe a Goldstone mode (gapless to within $\delta E$ = 0.037 meV) that persists throughout the entire field-induced magnetically ordered phase, suggestive of the spontaneous breaking of U(1) symmetry expected for a triplon BEC. However, in contrast to other well-known cases of this phase, the high-field ($\mu$${}_0$$H\ge 1.2$T) part of the phase diagram in Yb${}_2$Si${}_2$O${}_7$ is interrupted by an unusual regime signaled by a change in the field dependence of the ultrasound velocity and magnetization, as well as the disappearance of a sharp anomaly in the specific heat. These measurements raise the question of how anisotropy in strongly spin-orbit coupled materials modifies the field induced phases of QDMs.

6 pages, 4 figures, 12 pages of Supplemental Information, 15 Supplemental figures. Updated to published version