Interplay between spherical confinement and particle shape on the self-assembly of rounded cubes

Wang, Da; Hermes, Michiel; Kotni, Ramakrishna; Wu, Yao‐Ting; Tasios, Nikos; Liu, Y.; Nijs, Bart de; Wee, Ernest B. van der; Murray, Christopher B.; Dijkstra, Marjolein; Blaaderen, Alfons van

doi:10.1038/s41467-018-04644-4

Cited by 102 publications

(119 citation statements)

References 66 publications

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“…Similar design principles may be applied to hierarchical structures of bimetallic nanoparticles 53 , molecular self-assembly 71 , and plasmonic nanocluster formation 72 . It remains to be investigated if MCCs can undertake structural transition towards other symmetries as observed in atomic clusters 73 , and if magic number effect exists in other finite soft matter systems when the shape 38 , 74 , length scale 75 , or rigidity of confinement 76 is varied.…”

Section: Discussionmentioning

confidence: 99%

Magic number colloidal clusters as minimum free energy structures

et al. 2018

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Clusters in systems as diverse as metal atoms, virus proteins, noble gases, and nucleons have properties that depend sensitively on the number of constituent particles. Certain numbers are termed ‘magic’ because they grant the system with closed shells and exceptional stability. To this point, magic number clusters have been exclusively found with attractive interactions as present between atoms. Here we show that magic number clusters exist in a confined soft matter system with negligible interactions. Colloidal particles in an emulsion droplet spontaneously organize into a series of clusters with precisely defined shell structures. Crucially, free energy calculations demonstrate that colloidal clusters with magic numbers possess higher thermodynamic stability than those off magic numbers. A complex kinetic pathway is responsible for the efficiency of this system in finding its minimum free energy configuration. Targeting similar magic number states is a strategy towards unique configurations in finite self-organizing systems across the scales.

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Section: Discussionmentioning

confidence: 99%

Magic number colloidal clusters as minimum free energy structures

et al. 2018

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“…Next, heating of the grid is performed inside a vacuum chamber, with pressure below 5 × 10 −6 mbar and with temperature rate of +2.6 °C, until room temperature. These conditions enabled the phase transition of the vitreous ice layer from solid state to gaseous state without going through liquid state, minimizing the artifacts related with the drying process …”

Section: Methodsmentioning

confidence: 99%

Encapsulation of Noble Metal Nanoparticles through Seeded Emulsion Polymerization as Highly Stable Plasmonic Systems

Scarabelli

Aberasturi

et al. 2019

Adv Funct Materials

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The implementation of plasmonic nanoparticles in vivo remains hindered by important limitations such as biocompatibility, solubility in biological fluids, and physiological stability. A general and versatile protocol is presented, based on seeded emulsion polymerization, for the controlled encapsulation of gold and silver nanoparticles. This procedure enables the encapsulation of single nanoparticles as well as nanoparticle clusters inside a protecting polymer shell. Specifically, the efficient coating of nanoparticles of both metals is demonstrated, with final dimensions ranging between 50 and 200 nm, i.e., sizes of interest for bio-applications. Such hybrid nanocomposites display extraordinary stability in high ionic strength and oxidizing environments, along with high cellular uptake, and low cytotoxicity. Overall, the prepared nanostructures are promising candidates for plasmonic applications under biologically relevant conditions.

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“…The NC self-assembly can be induced, for example, by solvent evaporation (i.e., by increasing the NC density). In this case, a close-packed NC superstructure is obtained, whose geometry is dictated mainly by entropic factors, i.e., the shape and size of the NCs [67][68][69][70][71]. NC-NC attractive interactions can be activated (e.g., by ligand-exchange [72] or facet-specific ligand-detachment [73] reactions), inducing NC self-assembly in different types of superstructures.…”

Section: Introductionmentioning

confidence: 99%

Understanding the Formation of PbSe Honeycomb Superstructures by Dynamics Simulations

Soligno

Vanmaekelbergh

2019

Phys. Rev. X

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Using a coarse-grained molecular dynamics model, we simulate the self-assembly of PbSe nanocrystals (NCs) adsorbed at a flat fluid-fluid interface. The model includes all key forces involved: NC-NC shortrange facet-specific attractive and repulsive interactions, entropic effects, and forces due to the NC adsorption at fluid-fluid interfaces. Realistic values are used for the input parameters regulating the various forces. The interface-adsorption parameters are estimated using a recently introduced sharpinterface numerical method which includes capillary deformation effects. We find that the final structure in which the NCs self-assemble is drastically affected by the input values of the parameters of our coarsegrained model. In particular, by slightly tuning just a few parameters of the model, we can induce NC selfassembly into either silicene-honeycomb superstructures, where all NCs have a f111g facet parallel to the fluid-fluid interface plane, or square superstructures, where all NCs have a f100g facet parallel to the interface plane. Both of these nanostructures have been observed experimentally. However, it is still not clear their formation mechanism, and, in particular, which are the factors directing the NC self-assembly into one or another structure. In this work, we identify and quantify such factors, showing illustrative assembled-phase diagrams obtained from our simulations. In addition, with our model, we can study the self-assembly dynamics, simulating how the NCs' structures evolve from few-NCs aggregates to gradually larger domains. For example, we observe linear chains, where all NCs have a f110g facet parallel to the interface plane as typical precursors of the square superstructure, and zigzag aggregates, where all NCs have a f111g facet parallel to the interface plane as typical precursors of the silicene-honeycomb superstructure. Both of these aggregates have also been observed experimentally. Finally, we show indications that our method can be applied to study defects of the obtained superstructures.

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Interplay between spherical confinement and particle shape on the self-assembly of rounded cubes

Cited by 102 publications

References 66 publications

Magic number colloidal clusters as minimum free energy structures

Magic number colloidal clusters as minimum free energy structures

Encapsulation of Noble Metal Nanoparticles through Seeded Emulsion Polymerization as Highly Stable Plasmonic Systems

Understanding the Formation of PbSe Honeycomb Superstructures by Dynamics Simulations

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