Ferromagnetic Order of Reduced Magnetic Moments in a Frustrated Sawtooth Chain of the Magnetic Semiconductor ZnYb$_2$S$_4$

Abstract

In a sawtooth spin chain, competing nearest- and next-nearest-neighbor interactions suppress long-range order, yielding novel quantum states such as a spin-dimer singlet, 1/2 magnetization plateau, and spin contraction. Here, we investigate the magnetic properties of the orthorhombic semiconductor ZnYb$_2$S$_4$, in which Yb$^{3+}$ ions with an effective spin-1/2 form a sawtooth chain along the $b$-axis. The specific heat exhibits a sharp peak at ${T}_{\rm m}$ $=$ 1.4 K, at which the magnetic entropy $S_{\rm m}$ reaches only 27% of $R$ln2. This reduced $S_{\rm m}$ at $T_{\rm m}$ indicates the entropy release of the ground state doublet of Yb$^{3+}$ even for $T$ $>$ $T_{\rm m}$. The isothermal magnetization $M(B)$ at 0.28 K exhibits hysteresis for $\left|B\right| \leq 0.2$ T and increases monotonically for $B > 0.2$ T. The spontaneous magnetization is only 0.1 ${\it μ}_{\rm B}$$/$Yb, an order of magnitude smaller than that expected for the ground state doublet of Yb$^{3+}$. Moreover, in powder neutron diffraction measurements, no superlattice reflections due to antiferromagnetic order are observed for $T$ $<$ $T_{\rm m}$. Therefore, in the ground state, the Yb moments are ferromagnetically aligned, but their amplitude is reduced by magnetic frustration in the sawtooth Yb chain.