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The mixed-valent spinel LiV$_{2}$O$_{4}$ is known as the first oxideheavy-fermion system. There is a general consensus that a subtle interplay ofcharge, spin, and orbital degrees of freedom of correlated electrons plays acrucial role in the enhancement of quasi-particle mass, but the specificmechanism has remained yet elusive. A charge-ordering (CO) instability ofV$^{3+}$ and V$^{4+}$ ions that is geometrically frustrated by the V pyrochloresublattice from forming a long-range CO down to $T$ = 0 K has been proposed asa prime candidate for the mechanism. To uncover the hidden CO instability, weapplied epitaxial strain from a substrate on single-crystalline thin films ofLiV$_{2}$O$_{4}$. Here we show a strain-induced crystallization of heavyfermions in a LiV$_{2}$O$_{4}$ film on MgO, where a charge-ordered insulatorcomprising of a stack of V$^{3+}$ and V$^{4+}$ layers along [001], thehistorical Verwey-type ordering, is stabilized by the in-plane tensile andout-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 statesmirroring the geometrical frustration of the pyrochlore lattice, which supportsthe CO instability scenario for the mechanism behind the heavy-fermionformation.

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