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Chiral lattice modes are hybrid states arising from the chiral plasmonic particles assembled in ordered arrays with opportune periodicity. These resonances exhibit dependence on excitation handedness, and their observation in plasmonic lattices is strictly related to the chiroptical features of the fundamental plasmonic unit. Here, the emergence of chiral surface lattice resonances (c‐SLRs) is shown in properly engineered arrays of nanohelices (NHs), fully three dimensional (3D) chiral nano‐objects fabricated by focused ion beam processing. By tuning the relative weight of plasmonic and photonic components in the hybrid mode, the physical mechanism of strong diffractive coupling leading to the emergence of the lattice modes is analyzed, opening the way to the engineering of chiral plasmonic systems for sensing applications. In particular, a coupling regime is identified where the combination of a large intrinsic circular dichroism (CD) of the plasmonic resonance with a well‐defined balance between the photonic quality factor (Q factor) and the plasmonic field enhancement (M) maximizes the capability of the system to discriminate refractive index (RI) changes in the surrounding medium. The results lay the foundation for exploiting CD in plasmonic lattices to high performance refractometric sensing. [ABSTRACT FROM AUTHOR]

Fine control of the chiral light–matter interaction at the nanoscale, by exploiting designed metamaterial architecture, represents a cutting‐edge craft in the field of biosensing, quantum, and classic nanophotonics. Recently, artificially engineered 3D nanohelices demonstrate programmable wide chiroptical properties by tuning materials and architecture, but fundamental diffractive aspects that are at the origin of chiral resonances still remain elusive. Here, a novel concept of a 3D chiral metacrystal, where the chiroptical properties are finely tuned by in‐plane and out‐of‐plane diffractive coupling, is proposed. Different chiral dipolar modes can be excited along the helix arms, generating far field optical resonances and radiation pattern with in‐plane side lobes, and suggesting that a combination of efficient dipole excitation and diffractive coupling matching controls the collective oscillations among the neighbor helices. The proposed concept of compact chiral metacrystal can be suitable for integration with quantum emitters and open perspectives in novel schemes of enantiomeric detection. [ABSTRACT FROM AUTHOR]