Determination of Handedness in a Single Chiral Nanocrystal via Circularly Polarized Luminescence

The occurrence of biological homochirality is attributed to symmetry-breaking mechanisms which are still debatable. Studies of symmetry breaking require tools for monitoring the population ratios of individual chiral nano-objects, such as molecules, polymers, or nanocrystals. Moreover, mapping their spatial distributions may elucidate on their symmetry-breaking mechanism. While luminescence is preferred for detecting single particle chirality due to its high signal-to-noise ratio, the typical low optical activity of chromophores limits its applicability. Here, we report on handedness determination of single chiral lanthanide-based luminescent nanocrystals with a total photon count of 2 × 10⁴. Due to the large emission dissymmetry, we could determine the handedness of individual particles using only a single circular polarization component of the emission spectrum, without polarization modulation. A machine learning algorithm, trained to several spectral line shape features, enabled us to determine and spatially map the handedness of individual nanocrystals with high accuracy and speed. This technique may become invaluable in studies of symmetry breaking in chiral materials.