Design, synthesis, and physical properties of the intergrowth compound Eu$_2$CuZn$_2$As$_3$

Abstract

The rational combination of existing magnetic topological compounds presents a promising route for designing new topological materials. We report the synthesis and comprehensive characterization of the layered quaternary intergrowth compound Eu$_2$CuZn$_2$As$_3$, which combines structural units of two known magnetic topological materials, EuCuAs and EuZn$_2$As$_2$. Eu$_2$CuZn$_2$As$_3$ exhibits an antiferromagnetic ground state with successive magnetic transitions: quasi-two-dimensional ordering at $T_\mathrm{M} = 29.3$\,K, long-range antiferromagnetic ordering at $T_\mathrm{N} = 19$\,K, and spin-reorientation at $T_\mathrm{SR} = 16.3$\,K. The stepwise magnetic transitions manifest as plateau-like anomalies in the heat capacity. These transitions originate from multiple superexchange pathways and periodic variation of interplane Eu-Eu distances in the intergrowth structure. Charge transport shows a pronounced resistivity increase above $T_\mathrm{N}$ followed by minimal change below the ordering temperature. Magnetic fields rapidly suppress this resistivity rise, yielding significant negative magnetoresistance. Remarkably, Eu$_2$CuZn$_2$As$_3$ inherits the nonlinear anomalous Hall effect characteristic of its parent compounds. Energy evaluations of collinear spin configurations reveal a lowest-energy state with ferromagnetic coupling between Eu planes in EuCuAs units while maintaining antiferromagnetic coupling within EuZn$_2$As$_2$ units. The corresponding electronic structure displays potentially topologically nontrivial features. Our work demonstrates the efficacy of structural hybridization for discovering novel magnetic topological materials and establishes a general strategy for materials discovery.