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Quantum confinement in heterojunction architectures enable tunable electronic properties and efficient interfacial charge separation, forming a strong basis for next-generation optoelectronics. However, the nuanced interplay between an underlying structural asymmetry, Raman optical activity (ROA), and the nonlinear optical (NLO) signatures─especially under deliberate solvent modulation─remains largely unexplored. Inspired by the recently synthesized honeycomb monolayer of SiC ( Phys. Rev. Lett. 2023, 130, 076203), we report the very first extensive analysis of modal Raman optical activity and solvent-driven chirality-driven hyper-Rayleigh scattering (HRS) in 18 distinct quantum dots of SiC, GeC, and isostructural SiC–GeC─spanning 1–3 nm. Focusing on various point group symmetries within this material family, we identify a uniquely chiral SiC–GeC configuration and perform a full ROA study across all relevant scattering geometries and viable experimental conditions. The observation of a low-frequency chiral phonon mode, circular intensity difference signatures, and optical tensor-based handedness descriptors firmly establishes the vibrational origin of a chiral response. Leveraging nonlinear optical effects in such tailored nanostructures is pivotal for next-generation photonic platforms─from quantum information processing to integrated light control. Beyond dynamic higher-order hyperpolarizability profiling, we explore the second harmonic generation through the framework of HRS, revealing strongly polarized symmetry-governed signals characterized by a high depolarization ratio and multipolarity factor. Notably, when these engineered enantiomers are embedded in chiral environments, we observe a markedly enhanced chiral-specific HRS response, pointing to their potential in advancing chiral photonics.
Roy et al. (Mon,) studied this question.