Crystallization of polarons through charge and spin ordering transitions in 1T-TaS(2)

1T-TaS(2)中极化子通过电荷和自旋有序转变的结晶

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Abstract

The interaction of electrons with the lattice in metals can lead to reduction of their kinetic energy to the point where they may form heavy, dressed quasiparticles-polarons. Unfortunately, polaronic lattice distortions are difficult to distinguish from more conventional charge- and spin-ordering phenomena at low temperatures. Here we present a study of local symmetry breaking of the lattice structure on the picosecond timescale in the prototype layered dichalcogenide Mott insulator 1T-TaS(2) using X-ray pair-distribution function measurements. We clearly identify symmetry-breaking polaronic lattice distortions at temperatures well above the ordered phases, and record the evolution of broken symmetry states from 915 K to 15 K. The data imply that charge ordering is driven by polaron crystallization into a Wigner crystal-like state, rather than Fermi surface nesting or conventional electron-phonon coupling. At intermediate temperatures the local lattice distortions are found to be consistent with a quantum spin liquid state.

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