Lattice induced crystallization of nanodroplets: the role of finite-size effects and substrate properties in controlling polymorphism.

@article{Lam2018LatticeIC,
  title={Lattice induced crystallization of nanodroplets: the role of finite-size effects and substrate properties in controlling polymorphism.},
  author={Julien Lam and James F. Lutsko},
  journal={Nanoscale},
  year={2018},
  volume={10 10},
  pages={
          4921-4926
        }
}
Targeting specific technological applications requires the control of nanoparticle properties, especially the crystalline polymorph. Freezing a nanodroplet deposited on a solid substrate leads to the formation of crystalline structures. We study the inherent mechanisms underlying this general phenomenon by means of molecular dynamics simulations. Our work shows that different crystal structures can be selected by finely tuning the solid substrate lattice parameter. Indeed, while for our system… 
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References

SHOWING 1-10 OF 57 REFERENCES
Shape-anisotropy driven symmetry transformations in nanocrystal superlattice polymorphs.
TLDR
This work demonstrates solvent vapor-mediated NCSL symmetry transformations that are driven by the orientational ordering of NCs within the lattice that can be controlled by manipulating molecular interactions between ligands bound to the NC surface and the surrounding solvent.
Entropy-driven crystal formation on highly strained substrates
TLDR
This entropic component of lattice mismatched crystal growth could be used to develop unique methods for heterogeneous nucleation and growth of single crystals for applications ranging from protein crystallization to controlling the assembly of nanoparticles into ordered, functional superstructures.
Heterogeneous nucleation and shape transformation of multicomponent metallic nanostructures.
TLDR
In the heterogeneous nucleation and growth of Au on Pt or Pt-alloy seeds the heteroepitaxial growth of the Au shell exerts high stress on the seed by forming a core/shell structure in the early stage of the reaction.
Nucleation of colloidal crystals on configurable seed structures
Nucleation is an important stage in the growth of crystals. During this stage, the structure and orientation of a crystal are determined. However, short time- and length-scales make nucleation poorly
Atomic Scale Imaging of Nucleation and Growth Trajectories of an Interfacial Bismuth Nanodroplet.
TLDR
Atomic scale imaging allows this study to visualize the critical steps in the nucleation process of an interfacial nanodroplet, which suggests a revision of the perspective of CNT.
Real-Time Dynamical Observation of Lattice Induced Nucleation and Growth in Interfacial Solid–Solid Phase Transitions
Uncovering dynamical processes of lattice induced epitaxial growth of nanocrystal on the support is critical to understanding crystallization, solid-phase epitaxial growth, Oswald ripening process,
On the influence of a patterned substrate on crystallization in suspensions of hard spheres.
TLDR
A computer simulation study on crystal nucleation and growth in supersaturated suspensions of mono-disperse hard spheres induced by a triangular lattice substrate finds that compressed substrates are wet by the crystalline phase, while for stretched substrates the authors observe heterogeneous nucleation.
Controlling polymorphism during the crystallization of an atomic fluid.
TLDR
The results reveal that polymorph selection may take place, and be controlled, during the growth step, and that the predominantly fcc crystallites contain a notable amount of the hexagonal close packed form, due to the cross nucleation of the hcp form on the fcc form.
Nonequilibrium Synthesis of TiO2 Nanoparticle "Building Blocks" for Crystal Growth by Sequential Attachment in Pulsed Laser Deposition.
TLDR
This work demonstrates that nonequilibrium crystallization by particle attachment of metastable ultrasmall nanoscale "building blocks" provides a versatile approach for exploring and controlling the growth of nanoarchitectures with desirable crystalline phases and morphologies.
Polymorphic crystals selected in the nucleation stage
Molecular dynamics simulations are used to explore the atomic mechanism of formation of polymorphic crystals. Cooling the Lennard-Jones systems, we observe that the system almost always evolves into
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