Second order Zeeman interaction and ferroquadrupolar order in TmVO4

Abstract

TmVO₄ exhibits ferroquadrupolar order of the Tm 4f electronic orbitals at low temperatures, and is a model system for Ising nematicity. A magnetic field oriented along the c-axis constitutes a transverse effective field for the quadrupolar order parameter, continuously tuning the system to a quantum phase transition as the field is increased from zero. In contrast, in-plane magnetic fields couple to the order parameter only at second order, such that orienting along the primary axes of the quadrupole order results in an effective longitudinal field, whereas orienting at 45 degrees results in a second effective transverse field. Not only do in-plane fields engender a marked in-plane anisotropy of the critical magnetic and quadrupole fluctuations above the ferroquadrupolar ordering temperature, but in-plane transverse fields initially enhance the ferroquadrupolar order, before eventually suppressing it, an effect that we attribute to admixing of the higher crystalline electric field levels.