Journal
NANO LETTERS
Volume 13, Issue 10, Pages 4980-4988Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nl403149u
Keywords
Nanoparticles; Monte Carlo simulation; binary nanocrystal superlattice; electron microscopy; lamellar phase; demixing
Categories
Funding
- Office of Naval Research Multidisciplinary University Research Initiative [N00014-10-1-0942]
- U.S. Department of Defense [N00244-09-1-0062]
- Materials Research Science and Engineering Center program of the National Science Foundation (NSF) [DMR-1120901]
- Richard Perry University Professorship
- U.S. Department of Energy Office of Basic Energy Sciences, Division of Materials Science and Engineering [DE-SC0002158]
- IBM Ph.D. Fellowship Award
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Mixtures of anisotropic nanocrystals promise a great diversity of superlattices and phase behaviors beyond those of single-component systems. However, obtaining a colloidal shape alloy in which two different shapes are thermodynamically coassembled into a crystalline superlattice has remained a challenge. Here we present a joint experimental computational investigation of two geometrically ubiquitous nanocrystalline building blocks-nanorods and nanospheres-that overcome their natural entropic tendency toward macroscopic phase separation and coassemble into three intriguing pluses over centimeter scales, including an AB(2)-type binary superlattice. Monte Carlo simulations reveal that, although this shape alloy is entropically stable at high packing fraction, demixing is favored at experimental densities. Simulations with short-ranged attractive interactions demonstrate that the alloy is stabilized by interactions induced by ligand stabilizers and/or depletion effects. An asymmetry in the relative interaction strength between rods and spheres improves the robustness of the self-assembly process.
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