Crystallization of heavy fermions via epitaxial strain in spinel LiV$_{2}$O$_{4}$ thin film

TL;DR

This study demonstrates that epitaxial strain can induce a Verwey-type charge order in LiV$_{2}$O$_{4}$ thin films, revealing a link between charge ordering and heavy fermion behavior in a geometrically frustrated system.

Contribution

It provides experimental evidence that strain stabilizes charge-ordered insulating states in LiV$_{2}$O$_{4}$, elucidating the mechanism behind heavy fermion formation in this oxide.

Findings

Strain induces a Verwey-type charge order in LiV$_{2}$O$_{4}$ thin films.

Charge order states are stabilized by substrate-induced strain.

Heavy fermion behavior is linked to charge ordering near geometrical frustration.

Abstract

The mixed-valent spinel LiV$_{2}$O$_{4}$ 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 V$^{3+}$ and V$^{4+}$ ions that is geometrically frustrated by the V pyrochlore sublattice from forming a long-range CO down to $T$ = 0 K has been proposed as a prime candidate for the mechanism. To uncover the hidden CO instability, we applied epitaxial strain from a substrate on single-crystalline thin films of LiV$_{2}$O$_{4}$. Here we show a strain-induced crystallization of heavy fermions in a LiV$_{2}$O$_{4}$ film on MgO, where a charge-ordered insulator comprising of a stack of V$^{3+}$ and V$^{4+}$ 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 pyrochlore lattice, which supports the CO instability scenario for the mechanism behind the heavy-fermion formation.