title: Single-particle mapping of nonequilibrium nanocrystal transformations.
abstract: 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.
authors.affiliation: Department of Chemistry, University of California, Berkeley, Berkeley, CA 94720, USA.
authors.forename: Xingchen
authors.initials: X
authors.lastname: Ye
authors.affiliation: Department of Chemistry, University of California, Berkeley, Berkeley, CA 94720, USA.
authors.forename: Matthew R
authors.initials: MR
authors.lastname: Jones
authors.affiliation: Department of Chemistry, University of California, Berkeley, Berkeley, CA 94720, USA.
authors.forename: Layne B
authors.initials: LB
authors.lastname: Frechette
authors.affiliation: Department of Chemistry, University of California, Berkeley, Berkeley, CA 94720, USA.|Miller Institute for Basic Research in Science, University of California, Berkeley, Berkeley, CA 94720, USA.
authors.forename: Qian
authors.initials: Q
authors.lastname: Chen
authors.affiliation: Department of Chemistry, University of California, Berkeley, Berkeley, CA 94720, USA.
authors.forename: Alexander S
authors.initials: AS
authors.lastname: Powers
authors.affiliation: Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
authors.forename: Peter
authors.initials: P
authors.lastname: Ercius
authors.affiliation: Department of Physics, University of California, Berkeley, Berkeley, CA 94720, USA.
authors.forename: Gabriel
authors.initials: G
authors.lastname: Dunn
authors.affiliation: Biophysics Graduate Group, University of California, Berkeley, Berkeley, CA 94720, USA.
authors.forename: Grant M
authors.initials: GM
authors.lastname: Rotskoff
authors.affiliation: Department of Chemistry, University of California, Berkeley, Berkeley, CA 94720, USA.
authors.forename: Son C
authors.initials: SC
authors.lastname: Nguyen
authors.affiliation: Department of Physics, University of California, Berkeley, Berkeley, CA 94720, USA.
authors.forename: Vivekananda P
authors.initials: VP
authors.lastname: Adiga
authors.affiliation: Department of Physics, University of California, Berkeley, Berkeley, CA 94720, USA.|Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.|Kavli Energy NanoScience Institute, University of California, Berkeley, and Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
authors.forename: Alex
authors.initials: A
authors.lastname: Zettl
authors.affiliation: Department of Chemistry, University of California, Berkeley, Berkeley, CA 94720, USA.|Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.|Raymond and Beverly Sackler Center for Computational Molecular and Materials Science, Tel Aviv University, Tel Aviv 69978, Israel.
authors.forename: Eran
authors.initials: E
authors.lastname: Rabani
authors.affiliation: Department of Chemistry, University of California, Berkeley, Berkeley, CA 94720, USA.
authors.forename: Phillip L
authors.initials: PL
authors.lastname: Geissler
authors.affiliation: Department of Chemistry, University of California, Berkeley, Berkeley, CA 94720, USA. alivis@berkeley.edu.|Department of Materials Science and Engineering, University of California, Berkeley, Berkeley CA, 94720, USA.|Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.|Kavli Energy NanoScience Institute, University of California, Berkeley, and Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
authors.forename: A Paul
authors.initials: AP
authors.lastname: Alivisatos