Thermodynamics of the dipole-octupole pyrochlore magnet Ce$_2$Hf$_2$O$_{7}$ in applied magnetic fields

Abstract: The recently discovered dipole-octupole pyrochlore magnet Ce$_2$Hf$_2$O$_7$ is a promising three-dimensional quantum spin liquid candidate which shows no signs of ordering at low temperature. The low energy effective pseudospin-1/2 description in a magnetic field is characterized by the XYZ Hamiltonian and a Zeeman term where the dipolar local $z$-component of the pseudospin couples to the local $z$-component of the applied magnetic field, while the local $x$- and $y$-components of the pseudospin remain decoupled as a consequence of their octupolar character. Using effective Hamiltonian parameters determined in V. Poree et al., arXiv:2305.08261 (2023), remarkable experimental features can be reproduced, as for instance the specific heat and magnetization data as well as the continuum of states seen in neutron scattering. Here we investigate the thermodynamic response to magnetic fields applied along the global [110] direction using specific heat measurements and fits using numerical methods, and solve the corresponding magnetic structure using neutron diffraction. Specific heat data in moderate fields are reproduced well, however, at high fields the agreement is not satisfactory. We especially observe a two-step release of entropy, a finding that demands a review of both theory and experiment. We address it within the framework of three possible scenarios, including an analysis of the crystal field Hamiltonian not restricted to the two-dimensional single-ion doublet subspace. We conclusively rule out two of these scenarios and find qualitative agreement with a simple model of field misalignment with respect to the crystalline direction. We discuss the implications of our findings for [111] applied fields and for future experiments on Ce$_2$Hf$_2$O$_7$ and its sister compounds.