Crystallization of heavy fermions via epitaxial strain in spinel LiV₂O₄ thin film.

Abstract

The mixed-valent spinel LiV₂O₄ is known as the first oxide heavy-fermion system. There is a general consensus that a subtle interplay of charge, spin, and orbital degrees of freedom of correlated electrons plays a crucial role in the enhancement of quasi-particle mass, but the specific mechanism has remained yet elusive. A charge-ordering (CO) instability of V³⁺ and V⁴⁺ ions that is geometrically frustrated by the V pyrochlore sublattice from forming a long-range CO down to <i>T</i> = 0 K has been proposed as a prime candidate for the mechanism. Here, we uncover the hidden CO instability by applying epitaxial strain on single-crystalline LiV₂O₄ thin films. We find a crystallization of heavy fermions in a LiV₂O₄ film on MgO, where a charge-ordered insulator comprising of a stack of V³⁺ and V⁴⁺ layers along [001], the historical Verwey-type ordering, is stabilized by the in-plane tensile and out-of-plane compressive strains from the substrate. Our discovery of the [001] Verwey-type CO, together with previous realizations of a distinct [111] CO, evidence the close proximity of the heavy-fermion state to degenerate CO states mirroring the geometrical frustration of the V pyrochlore lattice, which supports the CO instability scenario for the mechanism behind the heavy-fermion formation.