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Heisenberg interactions are ubiquitous in magnetic materials and have beenprevailing in modeling and designing quantum magnets. Bond-directionalinteractions offer a novel alternative to Heisenberg exchange and provide thebuilding blocks of the Kitaev model, which has a quantum spin liquid (QSL) asits exact ground state. Honeycomb iridates, A2IrO3 (A=Na,Li), offer potentialrealizations of the Kitaev model, and their reported magnetic behaviors may beinterpreted within the Kitaev framework. However, the extent of their relevanceto the Kitaev model remains unclear, as evidence for bond-directionalinteractions remains indirect or conjectural. Here, we present direct evidencefor dominant bond-directional interactions in antiferromagnetic Na2IrO3 andshow that they lead to strong magnetic frustration. Diffuse magnetic x-rayscattering reveals broken spin-rotational symmetry even above Neel temperature,with the three spin components exhibiting nano-scale correlations alongdistinct crystallographic directions. This spin-space and real-spaceentanglement directly manifests the bond-directional interactions, provides themissing link to Kitaev physics in honeycomb iridates, and establishes a newdesign strategy toward frustrated magnetism.

Direct Evidence for Dominant Bond-directional Interactions in a Honeycomb Lattice Iridate Na2IrO3