Abstract
By exploiting the exquisite selectivity of DNA hybridization, DNA-coated colloids (DNACCs) can be made to self-assemble in a wide variety of structures. The beauty of this system stems largely from its exceptional versatility and from the fact that a proper choice of the grafted DNA sequences yields fine control over the colloidal interactions. Theory and simulations have an important role to play in the optimal design of self assembling DNACCs. At present, the powerful model-based design tools are not widely used, because the theoretical literature is fragmented and the connection between different theories is often not evident. In this Perspective, we aim to discuss the similarities and differences between the different models that have been described in the literature, their underlying assumptions, their strengths and their weaknesses. Using the tools described in the present Review, it should be possible to move towards a more rational design of novel self-assembling structures of DNACCs and, more generally, of systems where ligand-receptor are used to control interactions.
Highlights
Colloidal suspensions are well described by the same statistical mechanical equations as systems of atoms or small molecules
We believe that the present perspective is timely, as the rational design of novel DNACCbased materials will require a complete integration of theory and experiment
It is appealing that a simple theory that needs not invoke specific, system-dependent cooperative effects can provide a unified explanation of DNA-coated colloids (DNACCs) melting for a wide range of systems
Summary
Colloidal suspensions are well described by the same statistical mechanical equations as systems of atoms or small molecules. It is not our aim to provide a comprehensive overview of all simulation and modelling results in the field, but rather, to present a critical assessment of the various theoretical and computational approaches that have been proposed to describe DNACCs. Daan Frenkel: received his PhD in Physical Chemistry from the University of Amsterdam (NL). We aim to highlight the connections between different theoretical models, and explain the differences between various coarse-graining strategies used to describe DNACCs. We believe that the present perspective is timely, as the rational design of novel DNACCbased materials will require a complete integration of theory and experiment. We aim to establish a ‘hierarchy of accuracy’ in terms of the effects included These analytical models contain input parameters that depend on the molecular structure of the system, e.g. the specific DNA-sequence grafted on the colloids, or details of the spacer used for grafting. In the Concluding section (Section IV), we will identify possible new directions where the existing theoretical and computational framework could be profitably integrated with experiments to yield a more rational design of DNACC-based systems
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