Growth Synchronization and Size Control in Magic-Sized Semiconductor Nanocrystals

• Published in: ACS nano Vol. 17; no. 14; pp. 13232 - 13240
• Main Authors: Mazzotti, Sergio, Mule, Aniket S., Pun, Andrew B., Held, Jacob T., Norris, David J.
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 25.07.2023
• Subjects: atomically precise nanochemistry; magic-sized clusters; nanoparticles; semiconductors; classical nucleation theory
• ISSN: 1936-0851; 1936-086X
• DOI: 10.1021/acsnano.3c00585

“Magic-sized” nanocrystals (MSNCs) grow in discrete jumps between a series of specific sizes. Consequently, MSNCs have been explored as an alternative route to uniform semiconductor particles, potentially with atomic precision. However, because the growth mechanism has been poorly understood, the best strategies to control MSNC syntheses and obtain desired sizes are unknown. Experiments have found that common parameters, such as growth time and temperature, have limited utility. Here, we theoretically and experimentally investigate reactant supersaturation as a tool to control MSNC growth. We compare direct synthesis of CdSe MSNCs with ripening of isolated MSNCs or their mixtures. Surprisingly, we find that MSNCs readily synchronize to the same growth trajectory, even starting from distinct initial conditions, explaining the robustness of MSNC growth. Further, by understanding the synchronization mechanism, we demonstrate methods to control the final MSNC size. These results deepen our knowledge of MSNCs and indicate strategies to tailor their growth.