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Enriching the library of chiral plasmonic structures is of significant importance in advancing their applicability across diverse domains such as biosensing, nanophotonics, and catalysis. Here, employing triangle nanoplates as growth seeds, we synthesized a novel class of chiral-shaped plasmonic nanostructures through a wet chemical strategy with dipeptide as chiral inducers, including chiral tri-blade boomerangs, concave rhombic dodecahedrons, and nanoflowers. The structural diversity in chiral plasmonic nanostructures was elucidated through their continuous morphological evolution from two-dimensional to three-dimensional architectures. The fine-tuning of chiroptical properties was achieved by precisely manipulating crucial synthetic parameters such as the amount of chiral molecules, seeds, and gold precursor that significantly influenced chiral structure formation. The findings provide a promising avenue for enriching chiral materials with highly sophisticated structures, facilitating a fundamental understanding of the relationship between structural nuances and chiroptical properties.

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