Superconductivity in binary ruthenium pnictides occurs proximal to and upon suppression of a mysterious non-magnetic ground state, preceded by a pseudogap phase associated with Fermi surface instability, and its critical temperature, Tc, is maximized around the pseudogap quantum critical point. By analogy with isoelectronic iron based counterparts, antiferromagnetic fluctuations became "usual suspects" as putative mediators of superconducting pairing. Here we report on a high temperature local symmetry breaking in RuP, the parent of the maximum-Tc branch of these novel superconductors, revealed by combined nanostructure-sensitive powder and single crystal X-ray total scattering experiments. Large local Ru6 hexamer distortions associated with orbital-charge trimerization form above the two-stage electronic transition in RuP. While hexamer ordering enables the nonmagnetic ground state and presumed complex oligomerization, the relevance of pseudogap fluctuations for superconductivity emerges as a distinct prospect. As a transition metal system in which partial d-manifold filling combined with high crystal symmetry promotes electronic instabilities, this represents a further example of local electronic precursors underpinning the macroscopic collective behavior of quantum materials.
Interesting emergent behavior in quantum materials arises when the interaction of electrons with the lattice leads to localization and ordering. The triangular lattice of some transition metal dichalcogenides results in additional interplay of interactions involving spin, localized charge and lattice degrees of freedom. In the light of such complexity, the dominant mechanism that drives the formation of different orders is quite difficult to ascertain. Here we present a study of local symmetry breaking of the lattice structure in the prototype layered dichalcogenide material 1T-TaS2 to investigate the origin of the multiple charge and spin ordered phases. Remarkably, x-ray pair-distribution function measurements show symmetry-breaking polaronic distortions of the lattice structure around individual localized electrons at temperatures well above any of the known long-range ordered phases. The characteristic polaronic broken symmetry signatures remain present on cooling from 800 K to 15 K, through the purported quantum spin liquid (QSL) and charge ordered states, additionally revealing a new transition near 50 K to a state displaying partially restored symmetry and significant inter-layer dimerization. The appearance of locally broken symmetry and the associated order parameter at temperatures well above the appearance of long range order implies that charge ordering is driven by the Wigner crystallization of polarons, rather than Fermi surface nesting or conventional electron-phonon coupling. The local lattice distortions are consistent with a QSL state at intermediate temperatures where interlayer dimerization is incomplete. The breakup of the QSL state below 50 K is concurrent with the disappearance of domains in the charge order.
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