Hierarchical self-assembly pathways to colloidal open crystals


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Shaw, James (2020). Hierarchical self-assembly pathways to colloidal open crystals. University of Birmingham. Ph.D.

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The self-assembly of colloidal particles provides promising bottom-up routes to three-dimensional structures from simple building blocks. Colloidal open crystals are periodic ordered structures composed of low-coordinated colloidal particles, thus having a maximum density less than what is achieved at close packing. The study of colloidal open crystals has drawn much interest in recent years because of their attractive photonic, phononic and mechanical properties, giving rise to a variety of potential applications.

This thesis extensively uses Brownian dynamics simulations of triblock patchy particles, complemented by a global optimisation method for structure prediction, to establish the versatility of a hierarchical self-assembly scheme encoded in triblock patchy particles to realise a variety of colloidal open crystals via colloidal molecules. The scheme employs a hierarchy of patch-patch interactions programmed into designer triblock
patchy particles and tunes the range of these interactions along with the patch sizes. The key to the success of this bottom-up route to yield colloidal crystals is the self-limiting growth of small colloidal clusters, known as colloidal molecules, in the first stage of assembly.

The thesis presents a detailed analysis of crystallisation pathways into a variety of colloidal open crystals, namely body-centred cubic, simple cubic and tetrastack crystals and explores any bias towards the cubic or hexagonal polymorph in the case of the tetrastack crystal. In the light of the synthetic realisability of triblock patchy particles and the versatility of the hierarchical self-assembly pathways established here, it is envisaged that the present body of work will underpin novel routes to colloidal open crystals.

Type of Work: Thesis (Doctorates > Ph.D.)
Award Type: Doctorates > Ph.D.
Licence: All rights reserved
College/Faculty: Colleges (2008 onwards) > College of Engineering & Physical Sciences
School or Department: School of Chemistry
Funders: Engineering and Physical Sciences Research Council
Subjects: Q Science > QD Chemistry
URI: http://etheses.bham.ac.uk/id/eprint/10947


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