Pressure-induced ferromagnetism in the topological semimetal EuCd$_2$As$_2$

Abstract: The antiferromagnet and semimetal EuCd$2$As$_2$ has recently attracted a lot of attention due to a wealth of topological phases arising from the interplay of topology and magnetism. In particular, the presence of a single pair of Weyl points is predicted for a ferromagnetic configuration of Eu spins along the $c$-axis in EuCd$_2$As$_2$. In the search for such phases, we investigate here the effects of hydrostatic pressure in EuCd$_2$As$_2$. For that, we present specific heat, transport and $\mu$SR measurements under hydrostatic pressure up to $\sim\,2.5\,$GPa, combined with {\it ab initio} density functional theory (DFT) calculations. Experimentally, we establish that the ground state of EuCd$_2$As$_2$ changes from in-plane antiferromagnetic (AFM${ab}$) to ferromagnetic at a critical pressure of $\,\approx\,$2\,GPa, which is likely characterized by the moments dominantly lying within the $ab$ plane (FM${ab}$). The AFM${ab}$-FM$_{ab}$ transition at such a relatively low pressure is supported by our DFT calculations. Furthermore, our experimental and theoretical results indicate that EuCd$_2$As$_2$ moves closer to the sought-for FM$_c$ state (moments $\parallel$ $c$) with increasing pressure further. We predict that a pressure of $\approx$\,23\,GPa will stabilize the FM$_c$ state, if Eu remains in a 2+ valence state. Thus, our work establishes hydrostatic pressure as a key tuning parameter that (i) allows for a continuous tuning between magnetic ground states in a single sample of EuCd$_2$As$_2$ and (ii) enables the exploration of the interplay between magnetism and topology and thereby motivates a series of future experiments on this magnetic Weyl semimetal.