Single-particle mapping of nonequilibrium nanocrystal transformations

• Published in: Science (American Association for the Advancement of Science) Vol. 354; no. 6314; pp. 874 - 877
• Main Authors: Ye, Xingchen, Jones, Matthew R., Frechette, Layne B., Chen, Qian, Powers, Alexander S., Ercius, Peter, Dunn, Gabriel, Rotskoff, Grant M., Nguyen, Son C., Adiga, Vivekananda P., Zettl, Alex, Rabani, Eran, Geissler, Phillip L., Alivisatos, A. Paul
• Format: Journal Article
• Language: English
• Published: United States American Association for the Advancement of Science 18.11.2016; The American Association for the Advancement of Science; AAAS
• Subjects: Atoms & subatomic particles; Computer simulation; Dissolution; Equilibrium; Gold; Graphene; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Liquids; Nanocrystals; NANOSCIENCE AND NANOTECHNOLOGY; Nanostructure; Tracking
• ISSN: 0036-8075; 1095-9203
• DOI: 10.1126/science.aah4434

Chemists have developed mechanistic insight into numerous chemical reactions by thoroughly characterizing nonequilibrium species. Although methods to probe these processes are well established for molecules, analogous techniques for understanding intermediate structures in nanomaterials have been lacking. We monitor the shape evolution of individual anisotropic gold nanostructures as they are oxidatively etched in a graphene liquid cell with a controlled redox environment. Short-lived, nonequilibrium nanocrystals are observed, structurally analyzed, and rationalized through Monte Carlo simulations. Understanding these reaction trajectories provides important fundamental insight connecting high-energy nanocrystal morphologies to the development of kinetically stabilized surface features and demonstrates the importance of developing tools capable of probing short-lived nanoscale species at the single-particle level.