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Robust atomic-to-meso-scale chirality is now observed in the one-dimensional form of tellurium. This enables a large and counter-intuitive circular-polarization dependent second harmonic generation response above 0.2 which is not present in two-dimensional tellurium. Orientation variations in 1D tellurium nanowires obtained by four-dimensional scanning transmission electron microscopy (4D-STEM) and their correlation with unconventional non-linear optical properties by second harmonic generation circular dichroism (SHG-CD) uncovers an unexpected circular-polarization dependent SHG response from 1D nanowire bundles – an order-of-magnitude higher than in single-crystal two-dimensional tellurium structures – suggesting the atomic- and meso-scale crystalline structure of the 1D material possesses an inherent chirality not present in its 2D form; and which is strong enough to manifest even in the aggregate non-linear optical (NLO) properties of aggregates. 

The ability to reconfigure spin structure and spin‐photon interactions by an external electric field is a prerequisite for seamless integration of opto‐spintronics into modern electronics. In this study, the use of electric field on the tuning of circular photo galvanic effect in a quasi‐2D oxyhalide perovskite Bi₄NbO₈Cl is reported. The electrical transport measurements are applied to study the switching characteristics of the microsheet devices. The electric field is used to tune the nanoscale devices and an optical orientation approach is applied to understand the field‐tuned spin‐polarized band structures. It is found that the circular photogalvanic current can be erased and re‐created by poling, indicating the electric‐field‐based control over spin structure. The study enriches the basic understanding of the symmetry‐regulated optoelectronic response in ferroelectrics with spin‐orbit coupling.