Tracking Chirality Evolution in Tellurium Nanocrystals via Polarization-Resolved Second-Harmonic Scattering

Chirality pervades living systems and increasingly guides the design of functional nanomaterials. Yet weak or residual chirality can be difficult to detect, particularly in liquid-phase nanocrystal syntheses requiring noninvasive probes. Here we track chirality evolution in colloidal tellurium nanocrystals spanning strong, alloy-tuned, and reduced shape chirality. As morphological chirality decreases, linear circular dichroism drops by roughly an order of magnitude. In contrast, polarization-resolved second-harmonic scattering retains clear handedness-dependent responses. Across six independent observables─the nonlinear g-factor (gNL) and dual-circular polarization metrics (DCP1 and DCP2) measured in forward and right-angled geometries─the signal reverses sign between enantiomorphs and remains well-resolved. The geometry dependence of these responses is consistent with interference between mirror symmetry-even and mirror symmetry-odd nonlinear tensor contributions. These results establish chiroptical second-harmonic scattering as a sensitive probe of weak structural asymmetry in nanocrystals exhibiting coupled shape and crystal chirality.