In low-dimensional metallic systems, lattice distortion is usually coupled to a density-wave-like electronic instability due to Fermi surface nesting (FSN) and strong electron-phonon coupling. However, the ordering of other electronic degrees of freedom can also occur simultaneously with the lattice distortion thus challenges the aforementioned prevailing scenario. Recently, a hidden electronic reconstruction beyond FSN was revealed in a layered metallic compound BaTi2As2O below the structural transition temperature Ts ~ 200 K. The nature of this hidden electronic instability is under strong debate. Here, by measuring the local orbital polarization through 75As nuclear magnetic resonance experiment, we observe a p-d bond order between Ti and As atoms in BaTi2As2O single crystal. Below Ts, the bond order breaks both rotational and translational symmetry of the lattice. Meanwhile, the spin-lattice relaxation measurement indicates a substantial loss of density of states and an enhanced spin fluctuation in the bond-order state. Further first-principles calculations suggest that the mechanism of the bond order is due to the coupling of lattice and nematic instabilities. Our results strongly support a bond-order driven electronic reconstruction in BaTi2As2O and shed light on the mechanism of superconductivity in this family.
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