Exploring the Zone of Anisotropy and Broken Symmetries in DNA-Mediated Nanoparticle Crystallization*

Assembly mechanism of surface-functionalized nanocubes

“…We note that our model accounts only for weak vdW interactions and steric hindrance between ligands and is not suitable for nanocubes grafted with ligands exhibiting strong attractive interactions, such as hydrogen bonding, π-π stacking, or electrostatic interactions. Experiments 4,6,17 and simulations 18 on DNA-grafted NPs, where such interactions play a larger role, have shown that they exhibit novel assembly behavior including reconfigurable or chiral nanostructures that cannot be captured by our model. Following previous work, 15 the LJ size parameter σ cc for interactions between nanocubes was set equal to 0.4σ and the nanocube side length D = 10σ, where σ represents an arbitrary length scale.…”

“…16 These rough nanocubes were modeled by attaching an extra 24% surface beads at random positions on each face of the nanocubes. All beads in the system interact with each other via the Lennard Jones (LJ) potential 6 ], where ε ij , σ ij , and r ij represent the LJ energy and size parameters and the separation distance of the interacting beads i and j. The intramolecular interactions of the tethered chains were described by harmonic bond stretching and bending potentials…”

“…Self-assembly of faceted nanoparticles (NPs) offers an attractive approach for fabricating unique and complex nanostructures. [1][2][3][4][5][6][7] In cases where these NPs are made of noble metals, the NP assemblies can exhibit intriguing plasmonic, optical, and catalytic properties that are highly sensitive to the local arrangement of NPs within the structure. [1][2][3][8][9][10] Hence, controlling both the translational and rotational order of faceted NPs within their higher-order assemblies is crucial for creating the next generation of nanodevices and materials with desired properties.…”

Accelerated discovery of nanomaterials using computer simulation

“…Further examples of selfassembly studies that involve both experimental and computational efforts can be found in Refs. [54,58,[65][66][67].…”

Controlled Symmetry Breaking in Colloidal Crystal Engineering with DNA

“…13,24−29 With this approach, the particle core acts as a template to arrange the DNA into a conforming shell. 13,28 Anisotropic shapes can thus encode spatially discrete, collective DNA interactions localized along each facet or spatial region of the particle. The number, geometry, and relative strength (i.e., the number of DNA molecules within each collective interaction) of these "bonds" can be tuned to produce different symmetries.…”