Facile self-assembly of colloidal diamond from tetrahedral patchy particles via ring selection

Andreas Neophytou, Dwaipayan Chakrabarti, Francesco Sciortino

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Diamond-structured crystals, particularly those with cubic symmetry, have long been attractive targets for the programmed self-assembly of colloidal particles, due to their applications as photonic crystals that can control the flow of visible light. While spherical particles decorated with four patches in a tetrahedral arrangement-tetrahedral patchy particles-should be an ideal building block for this endeavor, their self-assembly into colloidal diamond has proved elusive. The kinetics of self-assembly pose a major challenge, with competition from an amorphous glassy phase, as well as clathrate crystals, leaving a narrow widow of patch widths where tetrahedral patchy particles can self-assemble into diamond crystals. Here we demonstrate that a two-component system of tetrahedral patchy particles, where bonding is allowed only between particles of different types to select even-member rings, undergoes crystallization into diamond crystals over a significantly wider range of patch widths conducive for experimental fabrication. We show that the crystallization in the two-component system is both thermodynamically and kinetically enhanced, as compared to the one-component system. Although our bottom-up route does not lead to the selection of the cubic polytype exclusively, we find that the cubicity of the self-assembled crystals increases with increasing patch width. Our designer system not only promises a scalable bottom-up route for colloidal diamond but also offers fundamental insight into crystallization into open lattices.

Original languageEnglish
Article numbere2109776118
Number of pages7
JournalProceedings of the National Academy of Sciences of the United States of America
Issue number48
Early online date24 Nov 2021
Publication statusPublished - 30 Nov 2021

Bibliographical note

Copyright © 2021 the Author(s). Published by PNAS.


  • colloidal self-assembly
  • tetrahedral networks
  • tetrahedral patchy particles
  • diamond lattice
  • polytype selection


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