ABSTRACT
Layered α-RuCl3 is a promising material to potentially realize the long-sought Kitaev quantum spin liquid with fractionalized excitations. While evidence of this state has been reported under a modest in-plane magnetic field, such behaviour is largely inconsistent with theoretical expectations of spin liquid phases emerging only in out-of-plane fields. These predicted field-induced states have been largely out of reach due to the strong easy-plane anisotropy of bulk crystals, however. We use a combination of tunnelling spectroscopy, magnetotransport, electron diffraction and ab initio calculations to study the layer-dependent magnons, magnetic anisotropy, structure and exchange coupling in atomically thin samples. Due to picoscale distortions, the sign of the average off-diagonal exchange changes in monolayer α-RuCl3, leading to a reversal of spin anisotropy to easy-axis anisotropy, while the Kitaev interaction is concomitantly enhanced. Our work opens the door to the possible exploration of Kitaev physics in the true two-dimensional limit.
Subject(s)
Electrons , Magnetic Fields , AnisotropyABSTRACT
Recent studies have brought α-RuCl_{3} to the forefront of experimental searches for materials realizing Kitaev spin-liquid physics. This material exhibits strongly anisotropic exchange interactions afforded by the spin-orbit coupling of the 4d Ru centers. We investigate the dynamical response at finite temperature and magnetic field for a realistic model of the magnetic interactions in α-RuCl_{3}. These regimes are thought to host unconventional paramagnetic states that emerge from the suppression of magnetic order. Using exact diagonalization calculations of the quantum model complemented by semiclassical analysis, we find a very rich evolution of the spin dynamics as the applied field suppresses the zigzag order and stabilizes a quantum paramagnetic state that is adiabatically connected to the fully polarized state at high fields. At finite temperature, we observe large redistributions of spectral weight that can be attributed to the anisotropic frustration of the model. These results are compared to recent experiments and provide a road map for further studies of these regimes.