Second order Zeeman interaction and ferroquadrupolar order in TmVO$_4$

Abstract

TmVO$_{4}$ exhibits ferroquadrupolar order of the Tm 4f electronic orbitals at low temperatures, and is a model system for Ising nematicity that can be tuned continuously to a quantum phase transition via magnetic fields along the $c$-axis. Here we present $^{51}$V nuclear magnetic resonance data in magnetic fields perpendicular to the $c$-axis in a single crystal that has been carefully cut by a plasma focused ion beam to an ellipsoidal shape to minimize the inhomogeneity of the internal demagnetization field. The resulting dramatic increase in spectral resolution enabled us to resolve the anisotropy of the electric field gradient and to measure the magnetic and quadrupolar relaxation channels separately. Perpendicular magnetic fields nominally do not couple to the low energy degrees of freedom, but we find a significant nonlinear contribution for sufficiently large fields that give rise to a rich phase diagram. The in-plane magnetic field can act either as an effective transverse or longitudinal field to the Ising nematic order, depending on the orientation relative to the principle axes of the quadrupole order, and leads to a marked in-plane anisotropy in both relaxation channels. We find that the small in-plane transverse fields initially enhance the ferroquadrupolar ordering temperature but eventually suppress the long-range order. We tentatively ascribe this behavior to the competing effects of field-induced mixing of higher energy crystal field states and the destabilizing effects of field-induced quantum fluctuations.