Colossal negative thermal expansion induced by magnetic phase competition on frustrated lattices in Laves phase compound (Hf,Ta)Fe

Li, B.; Luo, X. H.*; Wang, H.*; Ren, W. J.*; Yano, S.*; Wang, C.-W.*; Gardner, J. S.*; Liss, K.-D.*; Miao, P.*; Lee, S.-H.*; Kamiyama, Takashi*; Wu, R. Q.*; Kawakita, Yukinobu  ; Zhang, Z. D.*

Competition between ferromagnetic and antiferromagnetic phases on frustrated lattices in hexagonal Laves phase compound HfTaFe is investigated by using neutron diffraction as a function of temperature and magnetic fields and density-functional-theory calculations. At 325 K, the compound orders into the 120 frustrated antiferromagnetic state with well-reduced magnetic moment and an in-plane lattice contraction simultaneously sets in. With further cooling down, however, the accumulated distortion in turn destabilizes this susceptible frustrated structure. The frustration is completely relieved at 255 K when the first-order transition to the ferromagnetic state takes place, where a colossal negative volumetric thermal expansion, /K, is obtained. Meanwhile, the antiferromagnetic state can be suppressed by few Tesla magnetic fields, which results in a colossal positive magnetostriction. Such delicate competition is attributed to the giant magnetic fluctuation inherent in the frustrated antiferromagnetic state. Therefore, the magnetoelastic instability is approached even under a small perturbation.