Second-harmonic generation (SHG)
integrated with diverse nonlinear
optical activity characterization has high sensitivity to detect the
symmetry of materials at an interface, but the study is in its infancy.
Here, we employ SHG with linear dichroism (or SHG-LD) to study the
chiroptical origin of silver (Ag) chiral nanoparticles (CNPs) deposited
by glancing angle deposition (GLAD). It is found that Ag CNPs show
the chiroptical activity ascribed to not only the structural chirality
(i.e., atomically chiral lattices) but also one-fold anisotropy at
an interface due to the substrate rotation during GLAD. Therefore,
the SHG-LD shows great potential to provide valuable complementary
information to study the chiroptical properties of chiral metamaterials.