Colloidal 2D Layered SiC Quantum Dots from a Liquid Precursor: Surface Passivation, Bright Photoluminescence, and Planar Self-Assembly

• Published in: ACS nano 2024-10, Vol.18 (39), p.26848-26857
• Main Authors: Thomas, Salim A., Alharthi, Naif S., Petersen, Reed J., Aldrees, Ahmed, Tani, Sakurako, Anderson, Kenneth J., Granlie, Joseph, Pringle, Todd A., Payne, Scott A., Choi, Yongki, Kilin, Dmitri S., Hobbie, Erik K.
• Format: Article
• Language: English
• ISSN: 1936-0851; 1936-086X; 1936-086X
• DOI: 10.1021/acsnano.4c08052

We report the bottom-up synthesis of colloidal two-dimensional (2D) layered silicon carbide (SiC) quantum dots with a cubic structure, lateral size of 5–10 nm, ⟨110⟩ exfoliation to few atomic layers, and surface passivation with 1-dodecene. Samples shielded from oxygen and plasma-annealed for purity exhibit narrow blue photoluminescence (PL) with quantum yields (QYs) over 60% in exceptional cases, while unshielded nanocrystals (NCs) exhibit broad blue/green/white PL with 10–15% QY. The latter scenario is attributed to excess surface carbon and oxygen accrued during synthesis and processing, with size separation through ultracentrifugation revealing size-dependent impurity emission. In contrast, the shape of the bright narrow blue PL shows little variation with NC size, while in both scenarios, the maximum QY occurs near four atomic layers. When dried under heat, the disk-like NC suspensions are observed to aggregate into microscale domains, with further self-assembly into planar superlattice domains with common crystalline orientation. The results are compared with photophysical simulations and bring clarity to the broad emission commonly reported for top-down approaches, while inspiring bottom-up schemes directed at improved material quality.