Field-induced anomalous magnetic state beyond the magnetically ordered state in the slightly distorted triangular S=12 rare-earth antiferromagnet CeZn3P3

Abstract

Magnetic properties of ${\mathrm{CeZn}}_{3}{\mathrm{P}}_{3}$, which has been believed to have the same hexagonal ${\mathrm{ScAl}}_{3}{\mathrm{C}}_{3}$-type crystal structure as that of a spin dimer system of ${\mathrm{YbAl}}_{3}{\mathrm{C}}_{3}$ at room temperature, have been investigated by magnetization, magnetostriction, specific heat ($C$), and magnetocaloric effect measurements. In this research, we have found that ${\mathrm{CeZn}}_{3}{\mathrm{P}}_{3}$ certainly has a slightly deformed crystal structure from the hexagonal one even at room temperature, which is in contrast to the structural phase transition of ${\mathrm{YbAl}}_{3}{\mathrm{C}}_{3}$ occuring at around 80 K, although the very slight deformation along the $c$ plane, i.e., slightly deformed triangular lattice, and the formation of the multidomain structure are common to both compounds. ${\mathrm{CeZn}}_{3}{\mathrm{P}}_{3}$ is thought to maintain its deformed structure from a high-temperature region above room temperature to an extremely low-temperature region and shows a magnetic order below ${T}_{\mathrm{N}}=0.8$ K. The analysis of the temperature dependence of the magnetic susceptibility ($\ensuremath{\chi}$) and $C$ has revealed that a Kramers doublet ground state with an easy-plane type anisotropy on the $c$ plane is well isolated from the excited states by the crystal field splitting energy of more than 300 K. Above ${T}_{\mathrm{N}}, \ensuremath{\chi}$ makes a broad peak at around 2 K, which certainly originates from the dimer formation due to the slight deformation of the triangular lattice. On the other hand, below ${T}_{\mathrm{N}}$, a magnetic phase diagram reminiscent of a magnetic flower blooming on the $c$ plane was observed, which may have a close relation to a quantum effect of a quasi $S=\frac{1}{2}$ spin system and a contribution of the orbital component. With increasing magnetic field, we have found an anomalous magnetic state beyond the usual magnetically ordered state, where $C/T$ is anomalously enhanced. This anomalous magnetic state is similar to that observed in ${\mathrm{YbAl}}_{3}{\mathrm{C}}_{3}$ induced by the field, although the magnetic ground state in ${\mathrm{YbAl}}_{3}{\mathrm{C}}_{3}$ is a nonmagnetic dimer state different from the normal magnetically ordered state in ${\mathrm{CeZn}}_{3}{\mathrm{P}}_{3}$.