  Heisenberg interactions are ubiquitous in magnetic materials and have been
prevailing in modeling and designing quantum magnets. Bond-directional
interactions offer a novel alternative to Heisenberg exchange and provide the
building blocks of the Kitaev model, which has a quantum spin liquid (QSL) as
its exact ground state. Honeycomb iridates, A2IrO3 (A=Na,Li), offer potential
realizations of the Kitaev model, and their reported magnetic behaviors may be
interpreted within the Kitaev framework. However, the extent of their relevance
to the Kitaev model remains unclear, as evidence for bond-directional
interactions remains indirect or conjectural. Here, we present direct evidence
for dominant bond-directional interactions in antiferromagnetic Na2IrO3 and
show that they lead to strong magnetic frustration. Diffuse magnetic x-ray
scattering reveals broken spin-rotational symmetry even above Neel temperature,
with the three spin components exhibiting nano-scale correlations along
distinct crystallographic directions. This spin-space and real-space
entanglement directly manifests the bond-directional interactions, provides the
missing link to Kitaev physics in honeycomb iridates, and establishes a new
design strategy toward frustrated magnetism.
