Asymmetric bimetallic Janus nanocrystals with a side-by-side
interface
have unique properties and important applications. However, understanding
their fundamental issues, including their formation mechanism, interfacial
linkage, and related properties, remains challenging, as does the
preparation of enantiopure samples. Atomically precise Janus bimetal
nanoclusters would unequivocally resolve these issues, yet they have
not been realized. Here, based on Au and transition metals (Cu/Cd),
and employing an S/P biligand strategy, we prepare and structurally
resolve four Janus nanoclusters, including racemate 6e Au8/Cu4, 6e R-/S-Au8/Cu4 enantiomers, and 2e racemateAu3/Cd. Their interfacial linkage is unambiguously
resolved at the atomic level, superatomic orbital splitting emerges,
and unique molecule-like electronic transitions and chiroptical properties
are present; more importantly, the dipolar distribution of bicomponents
leads to a maximum dipole moment of up to 45 D, which drives the formation
of 1D nanowires through self-assembly. This work provides a fundamental
knowledge of intermetallic nanomaterials and an avenue for the synthesis
of Janus nanoclusters.