title: Shape-dependent ordering of gold nanocrystals into large-scale superlattices.
abstract: Self-assembly of individual building blocks into highly ordered structures, analogous to spontaneous growth of crystals from atoms, is a promising approach to realize the collective properties of nanocrystals. Yet the ability to reliably produce macroscopic assemblies is unavailable and key factors determining assembly quality/yield are not understood. Here we report the formation of highly ordered superlattice films, with single crystalline domains of up to half a millimetre in two dimensions and thickness of up to several microns from nanocrystals with tens of nanometres in diameter. Combining experimental and computational results for gold nanocrystals in the shapes of spheres, cubes, octahedra and rhombic dodecahedra, we investigate the entire self-assembly process from disordered suspensions to large-scale ordered superlattices induced by nanocrystal sedimentation and eventual solvent evaporation. Our findings reveal that the ultimate coherence length of superlattices strongly depends on nanocrystal shape. Factors inhibiting the formation of high-quality large-scale superlattices are explored in detail.
authors.affiliation: Chinese Academy of Science (CAS) Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, China.
authors.forename: Jianxiao
authors.initials: J
authors.lastname: Gong
authors.affiliation: Department of Chemical Engineering, University of Michigan, Ann Arbor, Michigan 48109, USA.|Biointerfaces Institute, University of Michigan, Ann Arbor, Michigan 48109, USA.
authors.forename: Richmond S
authors.initials: RS
authors.lastname: Newman
authors.affiliation: Department of Chemical Engineering, University of Michigan, Ann Arbor, Michigan 48109, USA.|Biointerfaces Institute, University of Michigan, Ann Arbor, Michigan 48109, USA.
authors.forename: Michael
authors.initials: M
authors.lastname: Engel
authors.affiliation: Chinese Academy of Science (CAS) Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, China.
authors.forename: Man
authors.initials: M
authors.lastname: Zhao
authors.affiliation: Shanghai Synchrotron Radiation Facility, Shanghai Institutes of Applied Physics, No. 239, Zhangheng Road, Shanghai, 201204, China.
authors.forename: Fenggang
authors.initials: F
authors.lastname: Bian
authors.affiliation: Department of Chemical Engineering, University of Michigan, Ann Arbor, Michigan 48109, USA.|Biointerfaces Institute, University of Michigan, Ann Arbor, Michigan 48109, USA.|Department of Materials Science &Engineering, University of Michigan, Ann Arbor, Michigan 48109, USA.
authors.forename: Sharon C
authors.initials: SC
authors.lastname: Glotzer
authors.affiliation: Chinese Academy of Science (CAS) Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, China.
authors.forename: Zhiyong
authors.initials: Z
authors.lastname: Tang