Building the cooperativity in artificial
self-assembling systems
will synergistically reshape their properties and expand their application
spectrum. Here, we show how the cooperativity between achiral CdSe/CdS
nanorods (NRs) and chiral perylene diimide (PDI)-based molecules is
built upon their coassembly. We demonstrate that chirality transfer
from chiral molecular assemblies to CdSe/CdS NRs is enabled by the
encapsulation of NRs into PDI suprascrolls through chain–chain
van der Waals interactions, which in turn gives rise to markedly enhanced
circularly polarized luminescence of the nanocomposites. Additionally,
the circularly polarized emissive bands of the nanocomposites could
be finely tuned by engineering the emissive bands of NRs. More importantly,
these nanocomposites are able to invert their chirality when NRs are
self-assembled into chiral superlattices under a larger amount of
NRs. Detailed mechanistic studies unveil that these jammed NRs assemblies
hamper the folding of two-dimensional (2D) chiral nanosheets, which
consequently suppress the interlayer excitonic coupling and implement
the nanocomposites with inverted chirality. Our finding exemplifies
a way to invert the chirality switching from folding to unfolding
of 2D supramolecular nanosheets, akin to the chirality inversion in
the helix-to-superhelix transition in conventional one-dimensional
(1D) supramolecular systems. We also show that the strong van der
Waals interactions from aliphatic chains are crucial in achieving
such chirality transfer and inversion. Overall, we demonstrate that
these achiral CdS/CdSe NRs could serve as artificial molecular chaperones
to aid the unfolding of supramolecular nanosheets with controlled
chirality.