Design of self-assembling mesoscopic Goldberg polyhedra
Palladium ions complexed with nonlinear bidentate ligands have been shown to form hollow, spherical shells with high symmetries. We show that such structures can be reproduced using model anisotropic mesoscale building blocks featuring excluded volume and long-range ionic interactions. A linear buil...
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| Published in | Nanoscale advances Vol. 4; no. 2; pp. 4272 - 4278 |
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| Main Authors | , , |
| Format | Journal Article |
| Language | English |
| Published |
RSC
11.10.2022
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| Subjects | |
| Online Access | Get full text |
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| Summary: | Palladium ions complexed with nonlinear bidentate ligands have been shown to form hollow, spherical shells with high symmetries. We show that such structures can be reproduced using model anisotropic mesoscale building blocks featuring excluded volume and long-range ionic interactions. A linear building block with a central charged particle, in combination with a bent 'ligand' particle with opposite charges at the ends is sufficient to drive the system towards planar coordination, and the charge ratio determines the coordination number. Similar to the molecular systems, the bend in the 'ligand' particle determines the curvature of the shells that these building blocks prefer. Besides reproducing exotic structures such as M
30
L
60
and M
48
L
96
tetravalent Goldberg polyhedra, we identify highly cooperative single transition state rearrangements between low-energy competing structures as well, corresponding to rotatory motions of a planar subunit within the spherical shell.
Simple coulombic and excluded volume interactions can give rise to highly symmetric shells, including tetravalent Goldberg polyhedra, in a model inspired by the shape and interactions of palladium ions complexed with nonlinear bidentate ligands. |
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| Bibliography: | Electronic supplementary information (ESI) available: Alternative parameterisation of the potential that gives rise to hollow shells of the same symmetry than those presented in the paper, MD simulation snapshots and trajectory analyses. Supplementary Movie 1: Change of the potential energy surface shown in Fig. 1 as the 'ligand' particle is rotated in-plane around a vertical axis centered on site D. Supplementary Movie 2: Highly cooperative low-energy single transition state rearrangement between a pseudorhombicuboctahedral structure and the rhombicuboctahedral global minimum (right panel of Fig. 3). Supplementary Movie 3: Lowest energy pathway for interconversion between the tetravalent Goldberg global minimum and the icosahedral structure shown in Fig. 2b. Supplementary Movie 4: Smoothed molecular dynamics trajectory for M 60 https://doi.org/10.1039/d2na00447j L 30 showing the final steps of assembly into an icosahedral structure. trajectories.zip: an archived folder containing the input files and MD trajectories. See ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
| ISSN: | 2516-0230 2516-0230 |
| DOI: | 10.1039/d2na00447j |