Synergistic doping and stabilization of magnetically tunable LnTi${}_3$(Sb,Sn)${}_4$ (Ln:Ce--Gd) kagome metals

Abstract

Here we present our synthesis and characterization of the LnTi${}_3$(Sb,Sn)${}_4$ (Ln: Ce, Pr, Nd, Sm, Gd) family of cleavable kagome metals. While these materials are isostructural to the LnTi${}_3$Bi${}_4$ family, they only form as (Sb,Sn) solid-solutions with no corresponding LnTi${}_3$Sb${}_4$ or LnTi${}_3$Sn${}_4$ phases. We use a combination of first-principles density functional theory (DFT) and Crystal Orbital Hamilton Population (COHP) calculations to show that (Sb,Sn) alloying has a stabilizing effect on the structure by adjusting the Fermi level, filling bonding states, depopulating antibonding states, and adjusting the density-of-states (DOS) towards local minima, an effect we call ``synergistic doping.'' The tunable Fermi level also has a profound effect on the magnetism, which we demonstrate through a detailed characterization of the SmTi${}_3$(Sb,Sn)${}_4$ series. The series hosts multiple magnetic ground states resulting from competing magnetic interactions that are tunable by the (Sb,Sn) ratio. While the focus of this work is on SmTi${}_3$(Sb,Sn)${}_4$, we briefly comment on the (Sb,Sn) solubility range and the conferred magnetic tunability in the other rare-earths compounds (Ln: Ce, Pr, Nd, Gd) as well. Our work demonstrates how the (Sb,Sn) synergistic pair can be used to stabilize the LnTi${}_3$(Sb,Sn)${}_4$ structure while simultaneously providing a means to tune the magnetism, ultimately providing a potential route to develop new intermetallics with chemical, magnetic, and electronic tunability.

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