Twins of Minimalistic Carbon Dots: Uniform Emitting‐Units and Molecular Level Repeatable Photoluminescence

Abstract Understanding the photoluminescence mechanism of carbon dots (C‐dots) is both of fundamental and technical significance. However, it has remained an extreme challenge due to C‐dots’ indeterminate constitution and complicated composition/structure. Herein, a combined processing system, namely extraction and subsequent preparative thin layer chromatography for C‐dots separation is presented. Benefiting from its powerful separation performances, two minimalistic C‐dots with almost identical structure and optical properties (named as “twin” C‐dots) are well separated. Then, by contrastive analysis, a photophysical picture for the C‐dots’ photoluminescence is presented: The C‐dots’ photoluminescence comes from uniform surface polycyclic aromatic hydrocarbon units instead of the whole particles, which is both size‐ and oxygen‐independent. The products not only are highly bright and stable against photobleaching, but possess repeatable photoluminescence with molecular level accuracy. So, the C‐dots favorably integrate the advantages from small molecule dyes to photoluminescent nanomaterials, which is unprecedented and desirable for property exploration and application expansion.